Field of the Invention
[0001] The present invention relates to processes and process plants for the conversion
of feedstock comprising a carbon-containing solid fuel such as biomass and/or carbon-containing
solid waste material.
Background
[0002] Waste materials such as municipal solid waste (MSW), agricultural and industrial
waste etc. are mainly landfilled and/or incinerated. Currently, waste recycling is
gaining more and more attention, since it allows reuse of a large portion of the already
used materials, such as paper, some plastics, glass, metals etc. However, other non-recyclable
materials are still either dumped into landfills or incinerated in order to recover
some of the chemical energy stored in these materials by converting it into electricity
and heat. This energy, however, cannot be stored.
[0003] There is therefore a need for methods and process plants, which are able to better
process these other non-recyclable materials.
[0004] Gasification of biomass and non-recyclable carbon-containing solid waste materials
converts waste materials into synthesis gas thus providing the possibility to convert
waste into more valuable products, such as chemicals or synthetic fuels. In other
words, gasification of waste helps to recycle the waste materials differently to conventional
recycling methods by converting the carbon in the waste materials into more useful
molecules (i.e., synthesis gas) which can then be synthesised into valuable final
products. Overall, gasifying biomass and waste materials can bring the following advantages
to communities: (1) the utilization of carbon containing solid waste materials in
an environmentally-friendly process, without emissions of toxic substances into the
atmosphere (2) providing the most efficient way for converting the chemical energy
stored in municipal solid waste (MSW) into electricity and (3) providing the most
efficient way for converting the carbon content of MSW, resp. refuse derived fuel
(RDF), into a highly valuable product, such as chemicals or synfuels.
[0005] Synthesis gas is typically a fuel gas mixture consisting primarily of hydrogen, carbon
monoxide, and very often some carbon dioxide. It is commonly used as an intermediate
in creating synthetic natural gas and for producing ammonia or methanol. Synthesis
gas (syngas) may be produced by thermochemical conversion of carbon containing sourced
materials, such as forest residues, agricultural residues, industrial and urban waste,
etc. In general, the gasification of such carbon containing sourced materials provide
raw synthesis gas which may include several impurities such as sulfur compounds (mainly
hydrogen sulfide, H
2S and carbonyl sulfide, COS), ammonia, chlorine compounds (mainly HCI), volatile matters,
lower and high molecular weight tars and fines (mainly in the form of micron and sub-micron
fly-ash containing metal salts), and char particles (carbon contained particulates
typically above 500 microns). It is desirable to be able to convert, in an efficient
process and apparatus, biomass and other carbon-containing solid waste materials into
more useful synthesis gas products which can then be used to produce high valuable
materials, such as methanol, synthetic natural gas and/or Fischer-Tropsch synthesis
fuels. For this reason, the gasification agent used in the process should not contain
high values of nitrogen, which is an inert gas in the process and cannot be separated
from the syngas. This means that air cannot be used as gasification agent, when the
final purpose is to synthesise bio-fuels. By replacing air with O
2/water steam/CO
2 mixture, the cold gas efficiency (CGE) of the process significantly increases and
the raw syngas obtained has much higher calorific value and lower volume flow rate.
[0006] The use of O
2/steam/CO
2, however, requires additional investments in production of these agents. Usually
an air separation unit and steam boiler are used for industrial scale production of
O
2 and steam, respectively. The CO
2 can be supplied in two ways: (i) by importing it from external supplier, means from
an external combustion unit, or (ii) by separating it from the syngas in the downstream
units and further recycle back to the gasification process.
[0007] Various approaches have been devised for producing, purifying, and modifying raw
synthesis gas from carbon-containing solid fuel materials. These existing approaches
are briefly discussed below.
[0008] US Patent No. 6063355 discloses a method for treating waste through two successive fluidized bed and combustion
reactors. The solidified and/or slurry waste is introduced to the fluidized bed with
revolving flow pattern at a temperature ranging from 450 °C to 650 °C, thereby producing
gaseous and carbonaceous materials. These products are directly fed to a swirling
flow combustion reactor, which is separate from the fluidized bed reactor, and increasing
the temperature to at least 1300 °C to produce synthesis gas. The crude syngas produced
in the second reactor is then quenched to separate the slag and the quenched crude
syngas is passed through a cyclone and scrubber for further cleaning. This method
involves the use of two successive fluidized beds which results in higher capital
and operational costs.
[0009] DE 4317319 A1 discloses a gasification-based technology to produce crude synthesis gas, which is
further conditioned and used as a feed for alternative end products such as methanol,
cleaned synthesis gas and hydrogen. The shredded wastes are fed to two parallel-connected
fixed bed gasifiers wherein the feed is reacted with oxygen, steam and raw carbon
dioxide at temperatures up to 1200 °C. The produced crude synthesis gas is partly
sent to an entrained-flow gasifier at a temperature of 1400 °C and pressure of 26
bar (2600 kPa) and partly to a gasification unit consisting of washing, heat recovery
and cooling stages, followed by a two-stage gas scrubbing unit, COS hydrolysis and
lastly used for power generation. The produced crude synthesis gas from the entrained-flow
gasifier is further processed in a soot wash unit, followed by CO conversion, gas
cooling and scrubbing units and finally used for producing methanol. Again, the use
of two parallel fixed bed gasifiers and one entrained flow gasifier results in higher
capital and operational costs.
[0010] EP 2376607 B1 discloses a method for producing and treating crude syngas from biomass through a
three-step gasification and reforming process at pressure lower than 10 atm (1013
kPa). The solid biomass is fed to the bottom section, described as a gasification
zone, of a fluidized bed reactor in the presence of oxygen and steam, wherein the
temperature lies within the range of 500 °C to 750 °C (in the first step). The portion
of said oxidized biomass produced in the first step is directly treated in a freeboard
region with a residence time lower than 8s in the presence of oxygen and steam at
temperatures ranging from 800 °C to 850 °C (in the second step). The portion of said
oxidized biomass produced in the second step is then treated in a separate thermal
reformer with oxidizing gas comprising oxygen and steam at a temperature of at least
900 °C and not exceeding a maximum of 1000 °C to produce crude syngas (in the third
step). The crude syngas produced in the thermal reformer is then passed through a
cyclone, followed by a heat recovery unit and finally scrubbers for further cleaning.
This method has a number of disadvantages, such as:
- the third step takes place in a separated thermal reformer apparatus which means that
an additional reactor is required, leading to higher capital and operational costs;
- the method is restricted to the operating pressure of the gasifier, which is below
10 atm (1013 kPa). This results in larger gasifier unit sizes being required when
processing larger quantities of feedstock;
- due to shorter residence times in the post-gasification zone, heavier hydrocarbons
are not completely decomposed and therefore a subsequent separate thermal reforming
unit is required (as mentioned above); and
- the reliance on using external catalysts and bed material for gasification increases
the operational costs of the system.
[0011] WO 2014/131700 A1 discloses a method for the recycle of by-products arising from gasification to improve
the yield of the gasification plant in question which is achieved by separation of
the components not reacted at temperatures of 900°C to 1200°C such as C
6H6 or C
10H
8 (by-products) and hydrogen-based products such as NH
3 which are contained in the synthesis gas and returning them to the gasification process.
The return of liquid by-products into the gasifier through various embodiments covered
in the patent may improve the yield of the plant but the consumption of gasification
agents are still high, compared to when at least a portion of the produced synthesis
gas is recycled to the gasifier.
[0012] All these processes have the disadvantage that considerable amounts of carbon dioxide
are needed at various process stages, e.g. as fluidization agent or as cooling agent,
therefore creating an increased carbon footprint, as the necessary CO
2 often needs to be obtained from external combustion units. In addition, due to the
use of carbon dioxide, high amounts of oxygen as gasification agents are needed.
[0013] Therefore, there exists a need for processes and plants providing a reduced carbon
footprint and an increased cold gas efficiency.
Summary
[0014] The problem is solved by the present invention as set forth in the independent claims.
[0015] In a first aspect, the present invention is directed to a process for converting
feedstock comprising a carbon-containing solid fuel, such as biomass and/or carbon-containing
solid waste material, to synthesis gas and downstream processing of the synthesis
gas, the process comprising the following steps :
- (a) converting the feedstock in a gasifier, the gasifier comprising a fluidized bed
zone and a post-gasification zone to produce synthesis gas;
- (b) obtaining the synthesis gas produced in step (a) downstream of the gasifier, in
particular including refining said synthesis gas in order to produce clean synthesis
gas;
- (c) recycling a portion of the synthesis gas of step (b) into at least one upstream
process unit, such as the gasifier, the upstream process unit being arranged upstream
of a position in the process from which said portion is recycled.
[0016] In a second aspect, the present invention is directed to a process plant for converting
feedstock comprising a carbon-containing solid fuel, such as biomass and/or carbon-containing
solid waste material, to synthesis gas and downstream processing of the synthesis
gas, the plant comprising:
a gasifier, the gasifier comprising a fluidized bed zone and a post-gasification zone
and being configured to produce synthesis gas;
a downstream arrangement connected to said gasifier, the downstream arrangement being
configured to obtain the synthesis gas produced in said gasifier, in particular the
downstream arrangement being configured to refine the synthesis gas;
a recycling arrangement arranged downstream of the gasifier and being configured to
recycle at least a portion of the synthesis gas obtained in the downstream arrangement
into at least one upstream process unit, such as the gasifier, the upstream process
unit being arranged upstream of a position in the process from which said portion
is recycled.
[0017] The features, technical advantages, effects, and explanations with respect to the
first aspect of the present application discussed herein equally apply to the second
aspect of the present invention.
[0018] Due to the process and the process plant according to the first and second aspects
of the present invention, in particular due step (c) of recycling of a portion of
the synthesis gas to at least one upstream process unit, a significant amount of carbon
dioxide which would otherwise be used in these upstream process units within a process/process
plant for converting said feedstock to synthesis gas, can be substituted by synthesis
gas and, therefore, the use of carbon dioxide can be significantly reduced. This leads
to a reduced carbon footprint, as less carbon dioxide is needed in the process or
process plant. Besides, usually the carbon dioxide used in various process units/process
steps, i.e. at least one upstream process units, needs to be prepared by external
combustion units. In other words, due to the present invention, synthesis gas produced
in the process can be recycled, introduced, and used as a process gas in various upstream
process stages/upstream process units preceding the position from which it is recycled,
wherein carbon dioxide is at least partially substituted by said recycled syngas portion.
For example, the recycling of a synthesis gas portion can substitute significant amounts
of carbon dioxide as a fluidization agent in the gasifier and/or as a cooling agent.
In addition, it has been surprisingly found that the use of the recycled syngas portion
in the gasifier as fluidization agent leads to an increased carbon conversion efficiency
and to a reduced need for gasification agents such as steam and/or oxygen. Furthermore,
the recycled synthesis gas can substitute carbon dioxide as a dust removal agent in
a filter within the process. Finally, the use of recycled synthesis gas also leads
to an increased cold gas efficiency. Further technical advantages resulting from the
present invention will be set forth herein below.
Brief Description of the Drawings
[0019] Certain embodiments of the present invention are shown in the accompanying drawing
and hereinafter described in detail.
[0020] Figure 1 shows an example process and production plant arrangement for converting
feedstock comprising a carbon-containing solid fuel, such as biomass and/or carbon-containing
solid waste material to synthesis gas, according to an embodiment of the invention.
Definitions
[0021] As used herein, "upstream" is a relative term describing an earlier stage or a preceding
position in the process or process plant, e.g. of a process unit, relative to the
direction of the stream of the process components, i.e. feedstock and synthesis gas,
through the process and plant, and, therefore, takes the usual meaning in the field.
As a non-limiting example, within a classical gasification process, a gasifier is
arranged upstream of a product raw gas cooler.
[0022] As used herein, "downstream" is a relative term describing a later stage or a subsequent
position within the process or process plant, e.g. of a process unit, relative to
the direction of the stream of the process components, i.e. feedstock and synthesis
gas, through the process and plant, and, therefore, takes the usual meaning in the
field. As a non-limiting example, within a classical gasification process, such as
a High Temperature Winkler (HTW) process, a cyclone separator is arranged downstream
of the gasifier.
[0023] As used herein, the term "recovering" is understood in a broad sense. During a step
of recovering or recovery of the synthesis gas, the synthesis gas, having a corresponding
composition depending on the process stage, can be treated and/or processed in accordance
with any suitable treatment/processes known in the art to refine raw syngas in order
to produce clean synthesis gas. These treatments typically involve removing impurities
and undesired material from the synthesis gas.
[0024] As used herein, the term "average temperature" takes it usual meaning within the
art and refers to the average temperature of each step and/or subzone and it will
be understood that within each step and/or subzone there higher/lower temperatures
than the average will likely be present. The "average temperature" can be determined
in accordance with methods known to the skilled person. In particular, an average
temperature can be determined by placing multiple thermocouples at different locations
within a subzone in the gasifier for measuring the individual temperatures at said
locations. In this measurement setup, the average temperature is the mean temperature
of the individual temperatures (usually the instant gas temperatures) measured by
said thermocouples (by their thermoelements) at said different locations in said subzone
of the gasifier over a certain time period. In particular, if the average temperature
remains constant the process conditions are considered stable.
[0025] As used herein, the term "ash softening temperature" takes its usual meaning in the
art, namely the temperature at which particles of ash obtained from the feedstock
will begin to deform (i.e., soften) or fuse. Ash softening temperature when referred
to herein is measured experimentally using the standard method CEN/TS 15370-1.
[0026] As used herein, the term "with respect to the earth's surface" is used as a positional
reference within the inventive process and process plant and the various zones in
the gasifier are counted beginning from the closest distance from the earth's surface
ending at the farthest distance from the earth's surface under the consideration of
a set-up where the gasifier is used in an upright position with an upwards flow, i.e.
away from the earth's surface, of the process components, i.e. feedstock and synthesis
gas. For example, the fluidized bed zone of the gasifier is arranged at a lower position
than the post-gasification zone with respect to the earth's surface. As further used
herein, if a second zone is arranged "on top" of a first zone it means that the second
zone directly follows the first zone, i.e. without a space in between, and the second
zone being arranged at a higher position than the first zone with respect to an earth's
surface.
[0027] The terms "converting a carbon-containing solid fuel to synthesis gas" and "gasification/gasifying"
are used interchangeably herein.
[0028] As used herein, the term "synthesis gas" or "syngas" describes a fuel gas mixture
consisting primarily of hydrogen and carbon monoxide, which can, however, depending
on the process stage, include impurities, such as dust, fly ash, sulfur components
and a minor amount of carbon dioxide. Therefore, in order to denote the state of the
synthesis gas, i.e. to which extend it contains impurities, the process stages/process
steps of gasification are additionally mentioned and/or further denotations, such
as "clean" synthesis gas are additionally used. Therefore, the skilled person in the
field of gasification is aware at any stage which composition the synthesis gas has.
[0029] As used herein, the term "obtaining" is to be understood broadly and mainly refers
to a process step of keeping the effluent discharged from the gasifier in the process.
Obtaining can also include process steps carried out downstream of the gasifier, such
as recovery of synthesis gas, e.g. by separation of solids from the synthesis gas
discharged from the gasifier.
[0030] As used herein, the term "pressure-loaded gasifier" means that the operating pressure
within the gasifier, e.g. the fluidized bed zone and the post-gasification zone, is
above atmospheric pressure. Preferably, the gasifier of the present invention, i.e.
the fluidized bed and post-gasification zones are operated in a pressure-loaded mode.
In other words, the gasifier of the first and second aspect of the present invention
is preferably a pressure-loaded gasifier. Such pressure used to operate the pressure-loaded
gasifier or a pressure-loaded gasifying process can comprise pressure ranges of between
about 200 kPa and about 3000 kPa or between about 200 kPa and about 4000 kPa, more
optionally between about 1000 kPa and about 3000 kPa or between about 200 kPa and
about 4000 kPa.
[0031] As used herein "High Temperature Winker" gasification or abbreviated "HTW" gasification
can be described as a pressure-loaded bubbling fluidized bed gasification process.
The reactor for carrying out HTW gasification is called "HTW" gasifier. A HTW gasifier
is the preferred gasifier for carrying out the inventive process and to be used in
the inventive process plant. A HTW gasifier is a refractory-lined reactor, typically
comprising a fluidized bed zone and a post-gasification zone, such as a freeboard
zone, wherein the reactor is equipped with a cyclone separator and recirculation line.
A HTW gasifier is typically operated under elevated pressures disclosed herein, such
as about 200 kPa to about 3000 kPa or 200 kPa to about 4000 kPa, and temperatures
disclosed herein with respect to the present invention. A HTW gasifier is well known
in the art and for example described by
S. De et al., Coal and Biomass Gasification - Recent Advances and Further Challenges,
Springer Nature Singapore Pte Ltd, published 2018 which is incorporated herein in its entirety.
[0032] As used herein, the term "carbon-containing solid fuel" is any solid fuel principally
which releases heat by the oxidation of carbon and which is suitable for gasification
to produce synthesis gas.
[0033] As used herein, the term "recycling" is to be understood broadly and includes the
process step of returning a portion of the synthesis gas obtained downstream of the
reactor to at least one upstream process unit, arranged upstream from the position
from where a recycling takes place, in particular for introducing said portion into
the process unit and/or using the portion as a fluidization agent or a heating agent
for gasification. In other words, said portion is divided from the synthesis gas product
stream obtained in step (b). Said recycling can take place using conduits, valves,
mass flow controllers, nozzles and/or other process equipment known to the skilled
person. The recycled portion can also be used as a cooling agent. In that case, the
skilled person understands that the synthesis gas obtained in step (b) from the converting
step (a) is cooled to a certain extend in order to recycle a portion of it for the
purpose of cooling.
[0034] The term "a portion" as used herein may refer to, unless otherwise explicitly stated,
at least 1 Ma.-% (mass percent), optionally at least 5 Ma.-%, optionally at most 10
Ma.-%, optionally at most 20 Ma.-%, optionally at most 30 Ma.-%, optionally at most
40 Ma.-%, optionally at most 50 Ma.-%, optionally at most 60 Ma.-%, optionally at
most 70 Ma.-%, optionally at most 80 Ma.-%, optionally at most 90 Ma.-%, optionally
at most 95 Ma.-%, optionally at most 99 Ma.-%. Furthermore, a portion can comprise
about 1 to about 50 Ma.-%, preferably about 2 to about 30 Ma.-% or about 5 to about
15 Ma.-%. The portion of recycled synthesis gas of step (c) according to the present
invention represented in Ma.-% refers to the total mass of the synthesis gas recovered
in step (b). Furthermore, as used herein, a "part" is a relative subunit of said portion
which is represented in Ma.-% related to the total mass of the portion. The ranges
defined above for the "portion" equally apply to the "part".
[0035] As used herein, the term "carbon conversion efficiency (CCE) represents the percentage
of total carbon in the gasifier feedstock which is successfully converted to product
gases, which contain carbon (such as CO, CO
2, CH
4, C2H2, C
2H
4,C
2H
6, C6H6 and C
10H
8).
[0036] As used herein, the term "about" referring to numerical values can cover the respective
value in a range of ±10 %; ±5 %, ±2 %; or ±1%.
[0037] As used herein, the term "Cold Gas Efficiency (CGE)" represents the ratio of chemical
energy stored in the raw syngas over the chemical energy stored in the solid feedstock.
Detailed Description
[0038] Processes and process plants for the conversion of feedstock comprising carbon-containing
solid fuel, such as biomass and/or carbon-containing solid waste material, to synthesis
gas are provided herein and in accordance with the present claimed invention to resolve
the foregoing problems in prior art processes and process plants.
The Process
[0039] In a first aspect, the present invention is directed to a process for converting
feedstock comprising a carbon-containing solid fuel, such as biomass and/or carbon-containing
solid waste material, to synthesis gas and downstream processing of the synthesis
gas, the process comprising the following steps :
- (a) converting the feedstock in a gasifier, the gasifier comprising a fluidized bed
zone and a post-gasification zone to produce synthesis gas;
- (b) obtaining the synthesis gas produced in step (a) downstream of the gasifier;
- (c) recycling a portion of the synthesis gas of step (b) into at least one upstream
process unit, such as the gasifier, the at least one upstream process unit being arranged
upstream of a position in the process from which said portion is recycled.
[0040] The position in the process from which said portion is recycled is typically a branching
unit. Said branching unit is configured to branch off a portion of the synthesis gas
product stream and lead said portion into a conduit for recycling into at least one
upstream process unit. Devices for realizing such branching unit are well known to
the skilled person.
[0041] The at least one upstream process is not limited by number. Thus, there can be more
than one upstream process units, such as at least two, at least three, at least four,
at least five, at least six or at least ten e.g. 1 to 4 upstream units, into which
the portion of the synthesis gas is recycled. Optionally, "at least one upstream unit"
can comprise one, two, three, four, five, six, seven, eight, or ten upstream units.
It is well understood that the portion is further divided into parts, if more than
one upstream process units are used. The number of the parts corresponds to the number
of process units to which the synthesis gas is recycled. For example, if two upstream
process units are used, there are two parts of the portion. The percentage of each
part is not limited, but usually, the portion is divided into equal parts (i.e. 50:50
in case of two process units) in case more than one upstream process unit is used.
In a particular embodiment, only one upstream process unit, for example the reactor,
is used.
[0042] In certain embodiments, combinable with each other embodiment disclosed herein, the
at least one upstream process unit comprises the gasifier. Further features of the
gasifier are described below in the section "The Gasifier". At least a part of the
portion of the synthesis gas of step (c), such as at least 25 Ma.-%, at least 50 Ma.-%
or at least 75 Ma.-%, or 100 Ma.-% of the portion, can be recycled into the gasifier.
Said recycling synthesis gas portion of step (c) is introduced into an inner volume
of the gasifier where the conversion according to step (a) takes place. The recycled
portion in step (c) can be ranging from about 2 to about 30 Ma.-%, preferably from
about 5 to about 15 Ma.-% with respect to the produced synthesis gas. Said introducing
can for example be carried out by a nozzle or other means known to the skilled person.
Preferably step (c) comprises at least one of the sub-steps:
(c1) recycling the portion of the synthesis gas of step (b) into the fluidized bed
zone; and/or
(c2) recycling the portion of the synthesis gas of step (b) into the post-gasification
zone.
[0043] In step (c1) the recycled synthesis portion can be directly introduced into the fluidized
bed zone over an inlet, such as a nozzle, in the gasifier wall encasing the fluidized
bed zone and/or by introducing the portion over a zone below (with respect to the
earth's surface) the fluidized bed zone and/or by introducing the portion over a recycle
line, which is explained in more detail below. The recycled portion in step (c1) can
be ranging from about 2 to about 30 Ma.-%, preferably from about 5 to about 15 Ma.-%,
e.g. about 10 Ma.-%, with respect to the produced synthesis gas. Said step (c1) automatically
includes fluidizing the fluidized bed by the recycling portion of the synthesis gas.
The fluidization velocity provided by the contribution of the recycling according
to step (c1) can range from about 0.5 to about 1.6 m/s being the typical fluidization
velocity for a fluidized bed. Due to recycling in step (c1) a significant portion
of carbon dioxide, which is usually employed as a fluidization agent, can be substituted
by the recycled synthesis gas portion, therefore, significantly reducing the carbon
footprint of the process, even independently of the composition of the feedstock.
In other words, the carbon dioxide consumption for fluidization can be significantly
reduced.
[0044] Surprisingly it was found that the recycling according to step (c1) has further unexpected
technical advantages. It was surprisingly found that the recycling of a portion of
synthesis gas considerably decreases the demand of gasification agent, in particular
oxygen and steam, and at the same time increases the conversion efficiency of the
feedstock. Such reduction of oxygen demand is in particular very advantageous in terms
of process costs, as the production of oxygen is very expensive. As a non-limiting
example, a recycling portion of about 10 Ma.-% of the synthesis gas obtained in step
(b) can reduce about 2 Ma.-% or more of overall oxygen consumption, depending on the
feedstock composition, for gasification compared to conventional processes operating
without recycling of synthesis gas. Such reduction of oxygen consumption can lead
to considerable cost savings in a process or process plant, as oxygen is expensive
to produce.
[0045] Without wishing to be bound by a particular theory, it is partly assumed that the
surprising and additional effects lie in the particular nature of synthesis gas. In
terms of the reduced consumption of oxygen and steam, synthesis gas has a lower molar
heat capacity compared to carbon dioxide. Because of the difference in molar heat
capacity, it is assumed that carbon dioxide acts as an energy sink within the gasification
zones compared to synthesis gas and, therefore, the use of carbon dioxide requires
a higher amount of oxygen in order to compensate for temperature drop. In terms of
the increased cold gas efficiency (CGE) and also in terms of the reduced need of gasification
agents, it is further assumed that, due to the increased higher heating value of synthesis
gas compared to that of the feedstock, the recycled synthesis gas portion acts as
an additional energy source and, therefore, favourable influences thermodynamics,
in particular the thermochemistry, in the fluidized bed zone. In particular, the effect
of the higher heating value of the recycled synthesis gas allows for the carbon content
in the feedstock to react exothermically resulting in the formation of CO, thereby
enhancing the carbon gasification efficiency of the process.
[0046] In step (c2) a recycling of the portion can take place into the post-gasification
zone, for example as a cooling agent, as described further below. In this case, the
portion obtained in step (b) has been at least subjected to a cooling according to
step (b2).
[0047] In certain embodiments, being combinable with any other embodiment disclosed herein,
step (b) comprises the sub-steps of:
(b1) cooling the synthesis gas produced in step (a) by a raw gas cooler downstream
of the gasifier to obtain a cooled synthesis gas;
(b2) filtering the cooled synthesis gas obtained in step (b1) by a filter unit, such
as a fly-char (dry basis) removal unit, to obtain a filtered synthesis gas;
(b3) cleaning the filtered synthesis gas obtained in step (b2) by a washing unit,
such as a quench and scrubbing unit, to obtain a purified synthesis gas;
(b4) removing carbon dioxide from purified synthesis gas obtained in step (b3) using
a CO shift and CO hydrolysis unit to obtain clean synthesis gas; and optionally
(b5) removing further carbon dioxide and H2S in an acid gas removing unit to produce clean synthesis gas for further processing.
[0048] Preferably, the synthesis gas of which a portion is recycled in step (c) is selected
from the any of the synthesis gases obtained in any of steps (b1) to (b5) or a combination
thereof.
[0049] In other words, the composition of the synthesis gas of which a portion is recycled
to the gasifier is not critical.
[0050] Nevertheless, it is preferred that the portion of the synthesis gas of step (c) is
recycled is the clean synthesis gas from step (b5). The units in which steps (b1)
to (b5) are carried out are well known to the skilled person.
[0051] After recovering the clean synthesis gas from step (b5), the portion which is not
recycled to an upstream process unit of the synthesis gas can be further processed
into an appropriate feedstock for production of various useful products such as advanced/bio-fuels,
by processes known to those skilled in the art. Such processes can offer tar-free
syngas as an appropriate feedstock to produce high valuable materials, such as methanol,
synthetic natural gas and/or Fischer-Tropsch synthesis fuels.
[0052] In certain embodiments, being combinable with each other embodiment disclosed herein,
the synthesis gas portion in step (c) is ranging from about 1 Ma.-% to about 70 Ma.-%,
preferably about 2 Ma.-% to about 30 Ma.-% or to about 40 Ma.-%, more preferably about
5 Ma.-% to about 15 Ma.-%, even more preferably from about 5 Ma.-% to about 10 Ma.-%,
in relation to the total mass of synthesis gas obtained in step (b). Preferably, the
synthesis gas obtained in step (b) is the synthesis gas obtained in step (b5).
[0053] The further components of the process according to the present invention are described
in the following sections "The Gasifier", "The Feedstock" and "The Upstream Process
Unit".
The Gasifier
[0054] The gasifier comprises a fluidized bed zone and a post-gasification zone i.e., both
zones are present in a single reactor (i.e., gasifier). In certain embodiments, the
fluidized bed zone is below the post-gasification zone with respect to the earth's
surface. Preferably, the gasifier is a HTW gasifier. A fluidized bed zone takes its
usual meaning in the art and in HTW gasification, namely a bed of material in which
the properties during operation are such that the material therein behaves as a fluid.
In certain embodiments, the bubbling fluidized bed includes internally produced solid
remnants of gasified feedstock, termed here as bed material. In general, the bed materials
can have a particle size ranging from about 200 to about 1600 microns.
[0055] The post-gasification zone as used herein also takes its usual meaning in the art
and in HTW gasification. In preferred embodiments, the post-gasification zone is a
freeboard zone.
[0056] The gasifier is preferably pressure-loaded during operation. As already defined,
this means that the gasifier is preferably operated at pressures above atmospheric
pressure. In particular, the gasifier, i.e. the fluidized bed zone and the post-gasification
zone, is operated at a pressure of between about 200 kPa and about 3000 kPa or between
about 200 kPa and about 4000 kPa, optionally about 1000 kPa to about 3000 kPa or to
about 4000 kPa, optionally wherein the gasifier is a refractory lined reactor. The
advantages of the elevated operating pressures have already been explained herein.
[0057] In certain embodiments, combinable with all other embodiments disclosed herein, the
particulate matter has a residence time in the fluidized bed zone of at least about
8 minutes. Preferably, the residence time is about 8 minutes to about 90 minutes,
preferably about 15 minutes to about 75 minutes, preferably about 25 minutes to about
60 minutes, preferably about 35 minutes to about 45 minutes. As used herein, the term
"residence time of particulate matter in the fluidized bed zone" may be understood
as the time period from an entry of a solid material into the fluidized bed to the
time point said solid material leaves the fluidized bed from the bottom of the gasifier
as a bottom product. Said residence time can be measured by methods well known to
the skilled person.
[0058] In certain embodiments, combinable with all other embodiments disclosed herein, the
raw synthesis gas in has a residence time in the post-gasification zone of at least
about 7 or 8 seconds, preferably at least about 10 seconds, preferably at least about
12 seconds, preferably at least about 15 seconds. Preferably the residence time in
the post-gasification zone is no greater than about 20 seconds, preferably no greater
than about 15, preferably no greater than about 10 seconds. The higher residence times
in the post-gasification zone help to improve the thermal decomposition of the heavier
hydrocarbons, thus helping to reduce the amount of tar present in the syngas product.
In particular, the term "residence time of raw synthesis gas in the post gasification
zone" may be understood as the time period from the entry of a raw synthesis gas molecule,
produced in the fluidized bed, into the post gasification zone until the exit of the
raw synthesis gas molecule from the post-gasification zone. Said residence time can
be determined by common methods known to the skilled person. The higher residence
time of more than 8 seconds in the post gasification zone which can immensely improve
the thermal decomposition of the heavier hydrocarbons
[0059] The flexibility of operating conditions in the gasifier by operating at higher pressures,
up to 4000 kPa, which offers more compacted units for higher production capacity,
offering appropriate flowrate, and operating conditions for the bio-fuel production
processing which basically calls for higher pressure and flowrate of synthesis gas
stream. Furthermore, it is advantageous that the availability of pressurized synthesis
gas downstream of the process facilitates the possibility of recycling of synthesis
gas without additional need for pressurization.
[0060] In certain embodiments, combinable with all other embodiments disclosed herein, the
gasifier comprises a conical portion. In certain embodiments, combinable with all
other embodiments disclosed herein, the fluidized bed zone is located within the conical
portion and the post-gasification zone is located within the non-conical portion.
In certain embodiments, the conical portion is angled between 3 and 12 degrees. Having
the fluidized bed zone situated in the conical portion allows nearly constant gas
velocity and uniform oxygen supply across the height of fluidized bed with the advantage
of controlled process conditions leading to homogeneous bubble formation in the fluidized
bed zone which enhances thereby partial oxidation and thermal decomposition of the
feedstock.
[0061] In preferred embodiments, an external catalyst is not added into the system i.e.,
the gasifier is operated absent the addition of external (or fresh) catalyst. This
means that no external catalyst is specifically added into the gasifier during operation.
Instead, in the preferred embodiment, the ash material within the feedstock is essentially
used as the catalyst. In this respect, the bottom product of the present process typically
contains both ash and carbon and the ash contains a lot of different materials such
as aluminum, iron, nickel, etc. which act as the catalyst. As is explained herein,
it is particularly advantageous not to have to handle and add an external catalyst
into the process.
[0062] The operating temperatures of the gasifier are dependent on the ash softening temperature
of the feedstock to be gasified. Therefore, in preferred embodiments the ash softening
temperature of the feedstock to be gasified is measured prior to operating the gasifier.
[0063] In certain embodiments the fluidized bed zone comprises the following subzones, starting
from the lowest position of subzone A with respect to the earth's surface:
- Subzone A in which a process step (a1) of contacting the feedstock with a gasification
agent comprising steam and oxygen is carried out, at an average temperature in the
range of between about 350-400°C below the ash softening temperature of the feedstock,
to partially oxidize the feedstock; and
- Subzone B, being arranged on top of subzone A, in which a process step (a2) of contacting
the partially oxidized product produced in step (a1) with a gasification agent comprising
steam and oxygen is carried out, at a higher average temperature than in step (a1)
and at an average temperature in the range of between about 250-350°C below the ash
softening temperature of the feedstock;
and/or wherein the post-gasification zone comprises the following subzones starting
from the lowest position of subzone C with respect to the earth's surface:
- Subzone C, being arranged on top the fluidized bed zone, in which process step (a3)
of contacting at least a portion of the product produced in the fluidized bed zone,
in particular in process step (a2), with a gasification agent comprising steam and
oxygen is carried out, at a higher average temperature than in the fluidized bed zone,
in particular than in process step (a2), the average temperature being between about
200-300°C below the ash softening temperature of the feedstock; and
- Subzone D, being arranged on top of subzone C, in which process step (a4) of contacting
at least a portion of the product produced in process step (a3) with a gasification
agent comprising steam and oxygen is carried out at a higher average temperature than
in process step (a3), the average temperature being between about 100-250°C below
the ash softening temperature of the feedstock, to produce the synthesis gas.
[0064] In a preferred embodiment, at least a part of the portion of step (c) is recycled
and introduced into subzone A. Furthermore or alternatively, the post-gasification
zone further comprises:
- Subzone E, arranged on top of subzone D, in which process step (a5) of cooling at
least a portion of the product produced in process step (a4) to an average temperature
lower than in process step (a4) is carried out, the synthesis gas within this subzone
E being cooled by about 50°C to about 100°C; and
- wherein at least a part of the synthesis gas portion in step (c) is recycled into
subzone E for cooling.
[0065] The temperatures mentioned above for Subzones A to E are controlled by the supply
of the gasification agent.
[0066] The gasification agent comprises oxygen and steam. In certain embodiments, the gasification
agent further comprises any other suitable gasification agent. In certain embodiments,
the gasification agent further comprises air. In certain embodiments the gasification
agent further comprises CO
2. In certain embodiments, the gasification agent is oxygen and steam i.e., the gasification
agent does not comprise any other substantial gas (with the exception of impurities).
Preferably, the gasification agent is either oxygen and steam or oxygen, steam and
air, most preferably oxygen and steam. In possible alternative embodiments, the gasification
agent is air. The gasification agent is fed into the fluidized bed zone of the gasifier
using any suitable feeding means.
[0067] It is preferred that the gasification agent is introduced into the gasifier via a
controlled flowrate, optionally through a single or multilayered nozzle system, as
is described in more detail herein.
[0068] In some embodiments, the content of the gasification agent and the amount of gasification
agent introduced into the gasifier will depend on the identity quality of the feedstock
and its characteristics and properties. In some embodiments, this includes properties
of the feedstock such as the fixed carbon content, heating value, ash melting point,
and metal content and other impurity levels. In certain embodiments, the content and
amount provided should be sufficient to partially oxidize and thermochemically decompose
the feedstock to high quality, tar free syngas, as will be understood in the art.
Ultimately, in preferred embodiments the gasification agent is selected so as to be
sufficient to convert the feedstock to raw syngas.
[0069] In certain embodiments, subject to the specific feedstock that is used in the process,
the gasification agent is supplied to the gasifier so that the oxygen content in the
gasifier is in the controlled range of 0.28 - 0.52 Nm
3/kg (daf) of the feedstock, of which at least about 20% and not greater than about
80% is supplied to the fluidized bed zone. In further embodiments, the gasification
agent is supplied to the gasifier so that the oxygen content in the gasifier is in
the controlled range of 0.35 - 0.45 Nm
3/kg (daf) of the feedstock, of which at least about 35% and not greater than about
65% is supplied to the fluidized bed zone.
[0070] daf or DAF = Dry Ash Free content, the weight percentage from the dry and ash free
material, is calculated as follows:

where, TM = total moisture content of the feedstock, ash = ash content in the feedstock.
TM is calculated using ISO 18134-1 and ash content using ISO 18122 standard.
[0071] In certain embodiments, subject to the specific feedstock that is used in the process,
the gasification agent is supplied to the gasifier so that the amount of steam in
the gasifier is in the controlled range of 0.23 - 0.52 Nm
3/kg (daf) of the feedstock, of which at least about 40% and not greater than about
80% is supplied to the fluidized bed zone. In further embodiments, subject to the
specific feedstock that is used in the process, the gasification agent is supplied
to the gasifier so that the amount of steam in the gasifier is in the controlled range
of 0.30 - 0.45 Nm
3/kg (daf) of the feedstock, of which at least about 50% and not greater than about
70% is supplied to the fluidized bed zone.
[0072] The gasifier comprises a fluidized bed zone and a post-gasification zone i.e., both
zones are present in a single reactor (i.e., gasifier). In certain embodiments, the
fluidized bed zone is below the post-gasification zone. A fluidized bed zone takes
its usual meaning in the art and in HTW gasification, namely a bed of material in
which the properties during operation are such that the material therein behaves as
a fluid. In certain embodiments, the bubbling fluidized bed includes internally produced
solid remnants of gasified feedstock, termed here as bed material. In general, the
bed materials mayhave a particle size ranging from about 200 to about 1600 microns.
[0073] In certain embodiments the gasifier comprises a conical portion. In certain embodiments,
the fluidized bed zone is located within the conical portion and the post-gasification
zone is located within the non-conical portion. In certain embodiments, the conical
portion is angled between 3 and 12 degrees. Having the fluidized bed zone situated
in the conical portion allows nearly constant gas velocity and uniform oxygen supply
across the height of fluidized bed with the advantage of controlled process conditions
leading to homogeneous bubble formation in the fluidized bed zone which enhances thereby
partial oxidation and thermal decomposition of the feedstock.
[0074] The operating temperatures of the gasifier are dependent on the ash softening temperature
of the feedstock to be gasified. Therefore, in preferred embodiments the ash softening
temperature of the feedstock to be gasified is measured prior to operating the gasifier.
[0075] The ash softening temperature of some example feedstocks at reducing atmosphere condition
are provided below:
| Feedstock type |
Ash softening temperature (°C) |
| Mix of refuse derived fuels (RDF) and municipal solid waste (MSW) |
1178 |
| MSW |
1180 |
| RDF with plastic |
1130 |
| Untreated wood |
1372 |
| Hard wood |
1456 |
| Lignite |
1150 |
| Bituminous coal |
1270 |
[0076] The above values are taken from particular feedstocks which have been tested. In
general, RDF will have an ash softening temperature ranging from 1130 to 1230 °C and
typical untreated and hard-wood from 1150 to 1600 °C, although impurities therein
can result in ash softening temperatures falling outside of these ranges. The temperature
ranges are therefore merely provided as approximate ranges.
[0077] It has been identified that operating the gasifier at temperatures based on the ash
softening temperature of the feedstock results in a highly efficient conversion of
the feedstock to synthesis gas. Operating the process within these temperature ranges
has been found to advantageously avoid melting the ash in the gasifier and the particles
becoming sticky, which can lead to agglomerations that damage the fluidized bed.
[0078] The biomass and/or carbon-containing solid waste material feedstock (as discussed
in detail earlier) is supplied to the gasifier (by means discussed in detail earlier),
preferably in pelletized form. Preferably, the feedstock is supplied to the gasifier
in the fluidized bed zone i.e., via an entry point in the fluidized bed zone. In certain
embodiments the feedstock is supplied to the gasifier at up to 3 different entry points
within the fluidized bed zone. In certain embodiments, there are 3 entry points, in
other embodiments 2 entry points and in further embodiments only 1 entry point.
[0079] In certain embodiments, the gasification agents are supplied to the gasifier at multiple
locations along the gasifier. In certain embodiments, the gasification agent is supplied
to both the fluidized bed zone and the post-gasification zone of the gasifier. In
certain embodiments, the gasification agent is supplied to the gasifier at approximately
2 to 15 locations along the gasifier, preferably 4 to 10 locations, preferably 5 to
8 locations along with the gasifier.
[0080] In certain embodiments, the gasification agent is supplied to the gasifier via a
plurality of nozzles. In certain embodiments, each of the nozzles are multilayered.
In preferred embodiments, at least one of the nozzles is arranged at an acute angle
relative to a horizontal plane of the gasifier. In certain embodiments, the nozzles
are tuyeres.
[0081] In certain embodiments, being combinable with all other embodiments disclosed herein,
the gasifier further comprising a sedimentation subzone with at least one discharge
leg, the sedimentation zone being arranged below the fluidized bed zone with respect
to the earth's surface, wherein
- heavy solid residues migrating in a downwards direction within the gasifier and being
obtained in the fluidized bed zone are discharged from the at least discharge leg
of the sedimentation zone; and
- at least a part of the synthesis gas portion of step (c) is recycled to the sedimentation
zone, in particular into the at least one discharge leg. In other words, step (c1)
further comprises introducing the recycled synthesis gas portion as a fluidization
agent in over the at least one discharge leg of the gasifier. In this case, the technical
advantages as discussed above are even more pronounced, as the recycled portion, e.g.
of step (c1), enters the fluidized bed from below and comes into contact with the
entire fluidized bed. In particular, the sedimentation zone has two discharge legs
at the lowest position, with respect to the earth's surface, of the reactor. The average
temperature the sedimentation zone is lower than the average temperature in subzone
B and is between 400-500 °C below the ash softening temperature of the feedstock.
In the sedimentation subzone the bottom product, i.e. heavy solid residues, is treated
with a gasification agent comprising steam (and CO2).
[0082] In certain embodiments, a cyclone separator, in which entrained dust particles are
separated from the synthesis gas, is arranged downstream of the gasifier. In certain
embodiments, the cyclone removes a majority (greater than 50 Ma.-%) of entrained dust.
In certain embodiments, the cyclone removes a majority (greater than 50 Ma-%) of pyrolytic
fly-ash/char with a particle size greater than 10 microns. Any suitable cyclone apparatus
may be used that is suitable for use in a gasification process. In certain embodiments,
the cyclone comprises a return line to return/recycle the separated material (i.e.,
dust) directly back to the gasifier, optionally the fluidized bed zone of the gasifier.
This helps to improve the carbon conversion efficiency of the system and process.
In certain embodiments, the return line is positioned at the bottom of the cyclone.
In certain embodiments, the synthesis gas product is treated in the cyclone directly
after leaving the gasifier i.e., the cyclone is the first post-treatment step, situated
directly downstream of the gasifier.
[0083] Preferably, the solids are recycled into the gasifier by a return line which connects
said cyclone separator and the gasifier; and wherein the at least one upstream unit
comprises the return line at least a part of the synthesis gas portion of step (c)
is recycled and introduced into the return line. This helps the introduction of the
portion of step (c) as a fluidization agent for the fluidized bed and is connected
to the technical advantages described above.
[0084] Furthermore or alternatively, an intermediate cooling unit is arranged downstream
and outside of the gasifier and upstream of the cyclone separator, wherein the at
least one upstream unit comprises the intermediate cooling unit and at least another
part of the synthesis gas portion of step (c) is recycled and introduced into the
intermediate cooling unit; and wherein the cyclone separator is a cyclone candle filter
unit. A cyclone candle filter unit is a cyclone separators as commonly used in the
field HTW gasification but also including a candle filter, as also known to the skilled
person, at the synthesis gas effluent in order to filter fine particles, i.e. particles
having sizes below 5 µm, out of the synthesis gas stream. Compared to conventional
cyclone separator, having a separation efficiency for such fine particles of at most
95%, a cyclone candle filter unit has a separation efficiency of 99.99%. Such cyclone
candle filter unit is for example known from
CN 201684496 U, which is incorporated by reference herein in its entirety. However, if the temperature
of the gas is too high, the dust particles irreversibly clog the filter. Therefore
an intermediate cooling unit is needed. The recycled portion of step (c) can also
be used as a coolant in the intermediate cooling unit. However, in this particular
embodiment, the recycled synthesis gas is primarily used to clean the filter. The
dust adsorbed on the candle filter surface is usually removed by carbon dioxide as
a cleaning gas, e.g. by applying pulses. Recycling a portion of synthesis gas to the
candle filter unit to replace carbon dioxide as the cleaning gas can lead to considerable
reduction in carbon dioxide consumption of the process. In other words, the recycled
synthesis gas is using as pulsing gas in order to remove dust adsorbed on the candle
filter surface. In certain embodiments, being combinable with each of the embodiments
disclosed herein, an intermediate cooling unit is the intermedia cooling unit disclosed
in
WO 2018/228946 A1, which is incorporated by reference herein in its entirety.
[0085] In certain embodiments, the process further comprises the step of densifying, in
particular pelletising, the feedstock prior to an introduction into the gasifier.
Using carbon-containing solid fuel feedstocks in the form of pellets which is favourable
for feedstock to be used at elevated pressure conditions, thus offering higher energy
density than shredded or non-pelletized materials. It has been found that densifying
and pressurizing the feedstock prior to it entering the gasifier allows the gasifier
to operate at elevated pressures and also provides a feedstock with higher carbon
density than shredded or non-pelletized material. The densified feedstock may be in
the form of pellets. Optionally, such pellets may be cylindrical and may have a diameter
substantially ranging from about 4 mm to 30 mm, in particular from about 4 mm to about
15 mm, more particularly being of a size of about 6 mm, about 8 mm or about 12 mm;
and a length substantially ranging from about 8 mm to about 80 mm. Operating the gasifier
at elevated pressures is beneficial since it produces a synthesis gas product at elevated
pressures. This is useful because the conversion of the synthesis gas into a synthetic
product also requires elevated pressures. Compared with a system operating at lower
pressures, the present invention represents a considerably energy saving. This is
because the pressure required to densify and pressurize the feedstock is considerably
less than the additional pressure requirements for compression of synthesis gas produced
at a lower gasifier pressure to levels required for conversion into a synthetic product.
Thus, the net energy consumption is lower than in the prior art systems not utilizing
a densified and pressurized feedstock, which makes the present invention more environmentally
friendly.
[0086] The feedstock can also comprise coal, such as bituminous coal, sub-bituminous coal,
lignite, peat and/or combinations thereof. In addition, mixtures between coal and
the above-mentioned feedstock are possible.
The Feedstock
[0087] The feedstock is a carbon-containing solid fuel and can be any material which is
suitable as a carbon-containing fuel, can be oxidized and can be used for gasification
to yield synthesis gas.
[0088] The feedstock preferably comprises biomass and/or carbon-containing solid waste material
is fed into the fluidized bed zone of the gasifier. The feedstock may be fed to the
fluidized bed zone via a lock hopper system and feed screw conveyer at elevated pressures.
The feed system (not shown in detail in Figure 1) may include a series of lock hoppers,
star feeders and screw conveyers which are pressurized with CO
2. In certain embodiments, the CO
2 is separated from the raw syngas during downstream processing in methods known in
the art. In certain embodiments, the separated CO
2 is reused as a pressurizing agent in the feed system to enable the feeding system
to operate at the similar pressure as the gasifier.
[0089] Alternatively, any suitable apparatus for feeding the feedstock to the fluidized
bed zone of the gasifier can be used.
[0090] Any suitable feedstock comprising biomass and/or carbon-containing solid waste material
is suitable to be processed in the process of the present invention. In alternative
embodiments the feedstock comprises biomass. In an alternative embodiment the feedstock
comprises a carbon-containing solid waste material. In some embodiments, the feedstock
comprises only biomass, in other embodiments only carbon-containing solid waste material
and in further embodiments comprises a blend of biomass and carbon-containing solid
waste material.
[0091] The process of the present invention is able to process homogenous and heterogeneous
feedstocks. In certain embodiments the feedstock is a homogenous feedstock. In other
embodiments the feedstock is a heterogeneous feedstock. The term "homogenous feedstock"
refers to single-sourced material e.g., trees, agricultural residues, wood chips.
"Heterogeneous feedstock" refers to multi-sourced materials e.g., materials such as
wood residues from sawmills, textiles, paper, plastic, cardboard, hydrocarbon compounds
and contaminants compounds.
[0092] Biomass refers to materials typically classed as biomass i.e., organic matter. Examples
of biomass that may be used in the invention are wood and plants. Carbon-containing
solid waste material is defined as any form of solid waste which comprises material
that is carbon-containing. Examples of carbon-containing solid waste include wastes
such as wood waste, agricultural waste, municipal solid waste (MSW), refuse derived
fuels (RDF), dried sewage sludge and industrial waste. The above materials may be
processed in the invention alone or in combination with one another in a blend. Preferred
feedstocks include: RDF, MSW, waste wood (preferably untreated) and hard wood, all
of which may be processed alone or in combination with one another. In particular,
preferred feedstocks are selected from RDF alone, MSW alone, RDF and MSW blend, RDF
with plastic, untreated wood and hard wood. Particularly preferred is the use of an
RDF and MSW blend.
[0093] Various different feedstocks that comprise biomass and carbon-containing solid waste
material, and in various different forms, are suitable feedstocks in the present process.
Particularly preferred, however, is the use of a pelletized feedstock. Any suitable
pelletizing method known in the art may be used. The pelletized feedstock is preferably
pressurized in a pressurisation system prior to being supplied to the gasifier. The
use of a pelletized material is not only favourable for gasification processes at
elevated pressures but also provides a feedstock with higher bulk density than shredded
or non-pelletized material. The use of pelletized flow material facilitates operation
at high pressures achieving two main advantages, namely the higher feed density leads
to lower CO
2 consumption which is advantageous for the process and improving the flowability of
the feed material which can be important when using lock hopper gravity system for
pressurization. Furthermore, there is a possibility to mix the moderate-to-high carbon
content dust, removed from the process with pelletized feedstock, and thereby increasing
the overall carbon conversion efficiency of the system. There is a possibility to
premix minor amounts of additives including but not limited magnesium compounds to
neutralize impurities such as chorine, fluorine and sulphur which are inherently present
in pelletized carbon containing material.
The Plant
[0094] The features disclosed in the aforementioned sections "the gasifier", and "the feedstock",
"the upstream process unit", especially the features relating to the process, equally
apply to the plant according to the second aspect of the present invention and are
combinable with the embodiments disclosed as follows.
[0095] In a second aspect, the present invention is directed to a process plant for converting
feedstock comprising a carbon-containing solid fuel, such as biomass and/or carbon-containing
solid waste material, to synthesis gas and downstream processing of the synthesis
gas, the plant comprising:
a gasifier, the gasifier comprising a fluidized bed zone and a post-gasification zone
and being configured to produce synthesis gas;
a downstream arrangement connected to said gasifier, the downstream arrangement being
configured to obtain the synthesis gas produced in said gasifier;
a recycling arrangement arranged downstream of the gasifier and being configured to
recycle at least a portion of the synthesis gas obtained in the downstream arrangement
into at least one upstream process unit, such as the gasifier, the upstream process
unit being arranged upstream of a position in the process from which said portion
is recycled.
[0096] In certain embodiments, being combinable with all embodiments disclosed herein, a
downstream arrangements individual units discloses in steps (b1) to (b5) or combinations
thereof.
[0097] In certain embodiments, being combinable with all embodiments disclosed herein, a
recycling arrangement includes a branching unit in which a portion of the synthesis
gas for recycling is branched off. The branching unit is preferably arranged downstream
of the unit in process step (b5). Furthermore the recycling arrangements includes
pumps, conduits, mass flow controllers, valves, nozzles and/or further process components
known to the skilled person for carrying out a recycling of a gas into an upstream
process unit.
[0098] In certain embodiments, being combinable with all embodiments disclosed herein, the
plant according to the second aspect of the present invention is configured to carry
out the process according to the first aspect of the present invention.
Detailed Figure Description
[0099] A non-limiting embodiment of the process and the process plant of the present invention
is shown in Figure 1.
[0100] In Figure 1, a pelletized biomass and/or carbon-containing solid waste material feedstock,
produced in the pelletisation unit 202, is fed into the system via line 1, through
lock hopper system 101 and via a connecting line to feed screw conveyer 102 at elevated
pressures into a lower section of the fluidized bed zone, subzone A, of gasifier 103.
Gasifier 103 has a fluidized bed zone, comprising subzones A to B, and a post-gasification
zone comprising subzones C to E above (downstream from) the fluidized bed zone. The
pelletized feedstock is introduced into the gasifier at subzone A, the socalled solid
entry fluidized bed zone, in Figure 1.
[0101] Gasification agent comprising steam and oxygen is fed to gasifier 103 through lines
4 to 4d..
[0102] Although not shown in Figure 1, the gasification agent is introduced into the gasifier
103 via controlled flowrate through specialized multilayered nozzles. The form and
amount of gasification agent introduced into the gasifier 103 will depend on the properties
of the feedstock to be gasified. Typically the gasification agent is supplied to the
gasifier so that the oxygen content in the gasifier is in the controlled range of
0.28 - 0.52 Nm
3/kg (daf) of the feedstock, of which at least about 20% and not greater than about
80% is supplied to the fluidized bed zone. In further embodiments, the gasification
agent is supplied to the gasifier so that the oxygen content in the gasifier is in
the controlled range of 0.35 - 0.45 Nm
3/kg (daf) of the feedstock, of which at least about 35% and not greater than about
65% is supplied to the fluidized bed zone. The temperature of the subzones is dependent
on the ash softening temperature of the feedstock. The temperature of each subzone
is achieved through the content, properties and amount of gasification agent (comprising
at least oxygen and steam) added to the gasifier. An external heat source does not
need to be used and in preferred embodiments is not used.
[0103] The feedstock is treated through the fluidized bed zone comprising sub-zones A and
B and post-gasification zone comprising sub-zones C to E of the gasifier 103 by travelling
and being treated through subzones A, B, C, D, E (with the bottom product being treated
in sedimentation zone 201 and instead leaving via the bottom of the gasifier) for
carrying out steps (a1) to (a5) as discussed herein before leaving the gasifier as
a raw syngas product via line 8.
[0104] In subzone A, in which step (a1) is carried out, termed here as the solid entry fluidized
bed zone, the pelletized feedstock is partially oxidized by the gasification agent
comprising oxygen and steam. The gasification agent supply is controlled such that
the average temperature of subzone B, in which step (a2) is carried out is within
the range of 350-400°C below the ash softening temperature of the pelletized feedstock.
Priorto carrying out the process the ash softening temperature of the pelletized feedstock
is calculated and the supply of the gasification agent throughout the gasifier adjusted
accordingly.
[0105] In subzone B of the fluidized bed zone, some of the feedstock in contact with hot
fluid bed particles heats up and due to thermal expansion and physical abrasion decomposes
on small pieces that after contacting the gasification agents decompose thermally,
going through drying, pyrolysis and char-oxidation processes thereby producing heavy
moderate-to-high carbon content residue that accumulates in the sedimentation subzone.
The average temperature in the sedimentation zone is lower than the average temperature
in subzone A and is between 400-500°C below the ash softening temperature of the feedstock.
In the sedimentation subzone the bottoms product is treated with a gasification agent
comprising steam (and CO
2).
[0106] The sedimentation zone, heavy solid carbonaceous residue settles down and leaves
the gasifier via the bottom of the fluidized bed zone through discharge legs 5a and
5b. Over lines 303a and 303b, at least a part of the portion of synthesis gas, branched
off at a branching unit (not shown in the figure), being arranged downstream of the
acid gas removing unit 305, after the recovery is recycled into the process over discharge
legs 5a and 5b providing a fluidization velocity ranging from 0.5 to 1.6 m/s depending
on the bottom product physical properties. This arrangement is particularly advantageous
to achieve the inventive effects as discussed earlier. Another part of the recycling
portion can, at the same time be provided over lines 303e and 303d into subzone A,
wherein in the latter case, the part of the recycling synthesis gas portion is provided
over a return line 9 of a cyclone separator 104, the cyclone separator 104 being configured
to remove dust from the raw synthesis gas leaving the gasifier 103, over line 8. Due
to this recycling, a significant amount of carbon dioxide can be replaced, reducing
the carbon footprint of the process. Furthermore, surprisingly the consumption of
gasification agent oxygen entering the gasifier 103 through any of lines 4 to 4d can
be significantly reduced by for example 2 Ma.-%. In addition, the carbon conversion
efficiency and the cold gas efficiency are increased. Via lines connected to discharge
legs 5a and 5b, the heavy residue is processed through lock hoppers 105, and then
the via following lines to bottom product removal unit 106 before leaving via following
lines to be used in the cement industry.
[0107] A partially oxidized produced gas containing low and high molecular weight hydrocarbons
in the form of volatiles and heterocyclic compounds (e.g., phenol, cresol, quinoline,
pyridine), together with light aromatic compounds (e.g., toluene, xylems, ethyl benzene),
and light polyaromatic hydrocarbons (e.g., naphthalene, indene, biphenyl, anthracene),
along with unreacted parts of the gasification agent, rises from the sedimentation
zone to the upper most subzone of the fluidized bed zone, subzone B, termed here as
the highly fluidized bed subzone.
[0108] Again, the supply of gasification agent to subzone B, in which step (a2) is carried
out, is controlled by properties of the pelletized feedstock and the oxygen and steam
gasification agent is supplied such that the average temperature in subzone B is higher
than in subzone A and 250-350°C below the ash softening temperature of the feedstock.
This condition provides an optimum temperature gradient along the reactor in the highly
fluidized bed zone (subzone B) in which the produced gas from subzone B, in the form
of heavy fly char loaded gas bubbles, is further decomposed and transformed thermally
into a raw product gas with a higher fraction of lower molecular weight hydrocarbons.
[0109] In the fluidized bed zone, the pelletized carbon containing feedstock and the generated
carbon content residue is contacted with fluidization agent for a time period of at
least 8 minutes to ensure a high degree of completion for partial oxidation and homogenous
and heterogenous thermal decomposition reactions.
[0110] The pelletized carbon containing feedstock in the fluidized bed zone gets partially
oxidized and thermally decomposed to produce carbon monoxide and hydrogen, and volatiles
of majorly lower molecular weight hydrocarbons together with intermediate species
in the form of heterocyclic compounds, light aromatics, light polyaromatic hydrocarbons,
unreacted part of the gasification agent, and entrained fly ash/char particles and
then passes to the post-gasification zone, including subzones C to E, of the gasifier
103. The fly ash/char particles, still contain high carbon concentration have inorganic
materials, such as alkali chlorides, metal oxides, etc. in the form salts. Fly ash/char
particles are usually less than 200 microns in size, and therefore rise to the post-gasification
zone. In the post-gasification zone, the partially oxidized material is contacted
with gasification agent containing oxygen and steam (and sometimes CO
2) for a period of at least 7 s through three successive thermal subzones which are
elaborated hereafter.
[0111] The thermochemically transformed material from the fluidized bed zone enters the
post-gasification zone through subzone C, termed here as, heavily loaded solid fly
ash/char subzone, wherein the temperature is adjusted through a controlled supply
of gasification agent of steam and oxygen such that the average temperature is higher
than in subzone C and is 200-300°C below the ash softening temperature of the feedstock.
In subzone C, the carbon present in the fly char is further converted thermochemically
in the presence of steam and oxygen to produce carbon monoxide and hydrogen, where,
in parallel, the intermediate hydrocarbons produced in subzone C undergo cracking,
thereby achieving a high carbon conversion efficiency.
[0112] The reformed and oxidized raw gas then enters subzone D, in which step (a3) is carried
out, in the post-gasification zone, termed here as, low fly ash loaded subzone, where
the steam and oxygen gasification agent supply is controlled such that the average
temperature of subzone D is higher than in subzone C and 100-250°C below the ash softening
temperature of the feedstock. Subzone D is characterized by further conversion of
carbon present in the char particles and even further decomposition of intermediate
hydrocarbons and tars present in the form of heterocyclic compounds, light aromatics,
and light polyaromatic hydrocarbons. High temperatures in low fly ash loaded subzone
(subzone D) allows for even better carbon conversion efficiency due to enhanced gasification
reactions which improves the carbon conversion.
[0113] The raw syngas product from subzone D is passed through the topmost section of the
gasifier, subzone E, where step (a5) is carried out, termed here a quench subzone.
This subzone is still within the post-gasification zone of the gasifier 103. In subzone
E, the raw syngas being cooled by about 50°C to about 100°C. In this subzone, the
raw syngas is cooled using quench water or process condensate or a part of the recycled
portion of the synthesis gas, which is sufficient to lower the average temperature
below the ash softening point. The recycling of a portion of the recovered synthesis
gas from branching unit 305, starting at line 303 can also take place into sub-zone
E via line 303c. In this case, a cooling of sub-zone E takes place via the recycled
synthesis gas. In such case, a further cooling step between line 303 and 303c (not
shown in the figure) can be necessary.
[0114] This quenches the raw syngas thus freezing or quenching sticky particles formed in
the higher temperatures and helps to minimize agglomeration problems or deposition
of melted materials on the walls in the post-gasification zone and downstream units
such as the cyclone separator 104 and the raw gas cooler 108.
[0115] The cooled raw syngas is then withdrawn from the gasifier 103 through line 8 and
passed through a cyclone 104, in which approximately 95 % of the entrained dust is
separated and recycled back through line 9 to the fluidized bed zone 116 of the gasifier
103. In general, recycling such particles which comprise of inorganic compounds coated
with carbon can improve the overall carbon conversion efficiency by increasing the
residence time of the fly ash/char particles in the gasifier.
[0116] The tar free syngas is withdrawn from the top of cyclone 104 and passes through raw
gas cooler 108 to produce saturated steam. Part of the steam can be re-used in the
process by going via a connecting line to superheater 115 and the superheated steam
recycled to the gasifier 103 via line 12. The cooled syngas with a minimum temperature
of 250 °C is subjected to further processing, enhancement, and purification including
filtering in the fly-char dry based removal unit 109 through the connecting line,
wherein the dust with the particle size greater than 5 microns is filtered and as
a byproduct can be sent to either feedstock pelletizing unit 202 or the cement industry
(through line 15b) via lock hopper 110 and dust removal unit 111. As shown in Figure
1, a part of the recycled synthesis gas portion of step (c) can also be used to clean
the filter in the fly-char dry based removal unit 109, e.g. by pulsing. Through the
further line to quench and scrubbing unit 112 where (a) the tar free syngas is saturated
which is a favourable condition for downstream processing, e.g. CO shift and COS hydrolysis,
and (b) the impurities such as hydrogen chloride are absorbed in alkali solution,
while other impurities including H
2S, COS, NH
3, HCN, etc. are partially eliminated by adjusting the pH of the alkali solution. The
sour water from the quench and scrubbing unit 112 is sent to the waste-water treatment
unit 113 (through line 18b) for further stripping and treatment. The purified synthesis
gas product is then obtained from the quench and scrubbing unit 112 and the clean
synthesis gas is obtained in the CO shift and CO hydrolysis unit. Afterwards the clean
synthesis gas proceeds to an acid gas removing unit 305 where a chemical or physical
adsorption of CO
2 and H
2S and their removing from the syngas take place in order to provide clean synthesis
gas for further processing. After the acid gas removing unit, a portion of the clean
synthesis gas can be branched off for recycling to at least one upstream unit over
lines 303 to 303e. where portions of it are branched off, the branched off portions
either being led over line 303 as a recycling synthesis gas, to further processing
in order to produce biofuel, such as methanol, gasoline and jet fuel) or to a further
sulfur removal unit and CO2 polishing.
[0117] The gasification agent is introduced into the gasifier at various entry points throughout
the fluidized bed zone and the post-gasification zone. The optimized conditions throughout
the gasifier are aided through the use of specialized, multilayered nozzles (not shown
in Figure 1) that introduce the gasification agent into the gasifier at an acute angle
relative to a horizontal plane. The gasification agent is supplied in sufficient quantity
and content to partially oxidize and thermochemically decompose the pelletized feedstock
to high quality, tar free syngas. As will be understood by the person skilled in the
art, the conditions within the gasifier may also be further optimized based on thermochemical
properties of the pelletized feedstock, such as fixed carbon content, heating value,
metal content and other impurity levels etc.
[0118] The order of the steps of the processes described herein is exemplary (unless a certain
order is necessitated through the explicit wording of the steps), but the steps may
be carried out in any suitable order, or simultaneously where appropriate. Additionally,
steps may be added or substituted in, or individual steps may be deleted from any
of the processes without departing from the scope of the subject matter described
herein.
[0119] It will be understood that the description of preferred embodiments herein is given
by way of example only and that various modifications may be made by those skilled
in the art. What has been described above includes examples of one or more embodiments.
It is, of course, not possible to describe every conceivable modification and alteration
of the above process and apparatus for purposes of describing the aforementioned aspects,
but one of ordinary skill in the art can recognize that many further modifications
and permutations of various aspects are possible. Accordingly, the described aspects
are intended to embrace all such alterations, modifications, and variations that fall
within the scope of the appended claims.