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The production of synthetic natural gas (SNG):

A comparison of three wood gasification systems


for energy balance and overall efficiency.

C.M. van der Meijden

H.J. Veringa

L.P.L.M. Rabou

ECN-W--09-042 DECEMBER 2009


2 ECN-W--09-042
ARTICLE IN PRESS
biomass and bioenergy xxx (2009) 1–10

Available at www.sciencedirect.com

http://www.elsevier.com/locate/biombioe

The production of synthetic natural gas (SNG): A comparison


of three wood gasification systems for energy balance and
overall efficiency

Christiaan M. van der Meijden a,*, Hubert J. Veringa b, Luc P.L.M. Rabou a
a
Energy research Centre of the Netherlands (ECN), Biomass, Coal & Environmental Research, P.O. Box 1, 1755 ZG Petten, The Netherlands
b
Eindhoven University of Technology, P.O. Box 513, 5600 MB Eindhoven, The Netherlands

article info abstract

Article history: The production of Synthetic Natural Gas from biomass (Bio-SNG) by gasification and
Received 31 January 2008 upgrading of the gas is an attractive option to reduce CO2 emissions and replace declining
Received in revised form fossil natural gas reserves. Production of energy from biomass is approximately CO2
28 October 2009 neutral. Production of Bio-SNG can even be CO2 negative, since in the final upgrading step,
Accepted 6 November 2009 part of the biomass carbon is removed as CO2, which can be stored. The use of biomass for
Available online xxx CO2 reduction will increase the biomass demand and therefore will increase the price of
biomass. Consequently, a high overall efficiency is a prerequisite for any biomass
Keywords: conversion process. Various biomass gasification technologies are suitable to produce SNG.
Biomass The present article contains an analysis of the Bio-SNG process efficiency that can be
Allothermal obtained using three different gasification technologies and associated gas cleaning and
Gasification methanation equipment. These technologies are: 1) Entrained Flow, 2) Circulating Fluidized
Twin-bed Bed and 3) Allothermal or Indirect gasification. The aim of this work is to identify the
Indirect gasification gasification route with the highest process efficiency from biomass to SNG and to quantify
CFB the differences in overall efficiency. Aspen Plus was used as modeling tool. The heat and
Entrained flow mass balances are based on experimental data from literature and our own experience.
SNG Overall efficiency to SNG is highest for Allothermal gasification. The net overall effi-
Bio-SNG ciencies on LHV basis, including electricity consumption and pre-treatment but excluding
Bio-CNG transport of biomass are 54% for Entrained Flow, 58% for CFB and 67% for Allothermal
Natural gas gasification. Because of the significantly higher efficiency to SNG for the route via Allo-
Biogas thermal gasification, ECN is working on the further development of Allothermal gasifica-
Aspen plus tion. ECN has built and tested a 30 kWth lab scale gasifier connected to a gas cleaning test
CCS rig and methanation unit and presently is building a 0.8 MWth pilot plant, called Milena,
which will be connected to the existing pilot scale gas cleaning.
ª 2009 Elsevier Ltd. All rights reserved.

1. Introduction importance a transportation fuel (CNG). In the Netherlands


about 50% of the primary energy consumed is covered by
Natural gas is increasingly important as a primary energy natural gas. A sustainable alternative is required anyhow, as
source. It is used for electricity production, industrial and the natural gas reserves are finite and their use contributes to
domestic heating purposes, as chemical feedstock and gaining greenhouse gas emissions. Clearly, ambitious plans to derive

* Corresponding author. Tel.: þ31 224 564582; fax: þ31 224 568487.
E-mail address: vandermeijden@ecn.nl (C.M. van der Meijden).
0961-9534/$ – see front matter ª 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.biombioe.2009.11.001

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001
ARTICLE IN PRESS
2 biomass and bioenergy xxx (2009) 1–10

30% of the primary energy used from renewable sources cannot Both types of cleaned gasses can be converted into a gas
be realized, without a renewable alternative for natural gas. containing only CH4, CO2, H2O and a small amount of Ar and N2.
Renewable Synthetic Natural Gas (SNG) production via CO2 and H2O are easily removed from the gas, leaving an SNG
digestion has been developed and implemented on a small that can contain small amounts of N2 and Ar. The maximum
scale. The limited amount of suitable digestible feed stocks [1], allowable concentration of non-combustible gasses is site-
some 60 PJ per year in the Netherlands, demands for devel- specific.
opment of a production technology for SNG by gasification, In this study a model is made to calculate the overall effi-
because that route has a much larger potential as a wider ciencies to SNG for large scale systems of 1 GWth input on HHV
range of fuels (e.g. wood) can be used. World-wide the net basis, based on three different types of gasifiers. The relatively
available biomass is estimated to be 200–700 EJ per year [2]. large scale was selected because it matches the commercial
Fig. 1 shows a simplified scheme of a biomass to SNG scale of Entrained Flow coal gasifiers and the production
configuration. Biomass is gasified at high temperature, capacity of a small natural gas field. Oxygen blown Entrained
producing a syngas which is cooled before it enters the gas Flow gasification is compared to both Indirect (or Allothermal)
cleaning section. The cleaned gas is sent to the methanation gasification and oxygen-blown Circulating Fluidized Bed gasi-
unit where CO and H2 are converted into CH4 and CO2. After fication at the same scale. The comparison is solely based on
CO2 removal and drying, the gas is ready for injection into the energetic efficiency numbers. Economics and transport of
natural gas grid. biomass are not taken into account. The goal of this compar-
The methanation of gas produced by the gasification of ison is to quantify the differences in overall process efficiencies
coal was investigated intensely in the 1970s and 1980s. Most for the three different gasifiers. The results were used by ECN
demonstrations were not successful because of the low to select to most promising gasification technology for SNG
natural gas price. The Dakota Gasification Company SNG production.
installation survived and is now a commercial success. The Dry wood (moisture content ¼ 15 wt.%) was selected as the
installation built in the 1970s and 1980s uses lignite as a fuel. fuel for this study, as it can be readily used for all three different
As the price of lignite is low, high efficiency was less of an types of gasifiers. Wood mixed with coal was gasified in the
issue. Biomass is a more expensive feedstock. The price may Shell Entrained Flow gasifier in Buggenum in the Netherlands
even increase further because of increasing demand, fueled by and wood is gasified in several fluidized bed gasifiers.
the CO2 reduction objectives. Hence, the production of SNG The next paragraph describes the system layout for each
from biomass requires a process with high overall efficiency. gasification technology. Sub systems are described in detail in
As the overall efficiency is mainly determined by the type of separate paragraphs. The final paragraph presents results of
gasifier, the gas cleaning and the level of heat integration, the the analysis.
goal of the work described here is to calculate the difference in
efficiency for the various options.
The three gasifier types under consideration all deliver gas 2. Process configurations
suitable for upgrading to SNG, but the high temperature
Entrained Flow gasifier (z1300  C) produces a syngas con- In all cases the gas cleaning and gas upgrading steps are kept
taining mostly CO, H2, CO2 and H2O while the medium similar as much as possible to allow an honest comparison of
temperature Allothermal and CFB gasifiers (z850  C) give the overall efficiencies due to various types of gasifiers.
a producer gas which in addition to CO, H2, CO2 and H2O Operating pressures were selected on the basis of what is
contains CH4, unsaturated and aromatic hydrocarbons like thought to be commercially available in the near future. Fig. 3
C2H4 and C6H6 and tar. Pollutants like dust, sulphur and chlo- shows the process scheme for the Entrained Flow SNG system.
ride need to be removed from the gas in all cases. The medium Entrained flow gasification requires an energy intensive pre-
temperature gasifiers also require tar removal. Fig. 2 shows the treatment to produce fine powder. Torrefaction [3] is selected,
general process efficiencies for wood to SNG. A high amount of followed by milling, because of the relatively low energy
‘instant SNG’ gives the highest efficiency to SNG, because the requirement. Dried biomass is fed into the torrefaction reactor
loss caused by the exothermic synthesis of CO and H2 is (T in Fig. 3). The torrefied biomass is milled, pressurized with
minimized. CO2 and pneumatically fed into the Entrained Flow gasifier (EF
Syngas, as produced conventionally by oil or coal gasifiers, in Fig. 3) which operates at 3 MPa and 1300  C. Syngas leaving
is seen as a more common feedstock gas than producer gas the gasifier is first cooled by a gas quench down to 600  C and
because gas-cleaning processes for syngas applications are subsequently cooled in a heat exchanger producing steam. Fly
already commercially available. The gas cleaning processes ashes are removed from the cooled gas by a filter. Part of the
for producer gas are still under development. gas is recycled to act as quench gas. Sulphur and chloride are

Fuel pre- Gas Gas H2O & CO2


Gasifier Cleaning Methanation
treatment cooler removal
Biomass

Fig. 1 – Simplified scheme of Biomass to SNG configuration.

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001
ARTICLE IN PRESS
biomass and bioenergy xxx (2009) 1–10 3

instant SNG * SNG


wood gas 52 - 72%
gasifier H2, CO
70 - 80% CH4
CH4 synthesis
75%

* mainly CH4, but also olefins and aromatics

Fig. 2 – General process efficiencies for wood to SNG.

removed from the gas by adsorbents. The gas is moisturized (carbon containing ash) is removed from the producer gas by
and pre-heated prior to conversion into methane. The heat a cyclone. The remaining dust and tar are dissolved in oil in
produced in the methanation section is used for steam the Olga gas cleaning system (OC and OA in Fig. 5). Heavy tars
generation. Water and carbon dioxide are removed from the and a small amount of ash are recycled back to the combus-
gas prior to injection into the natural gas grid. tion section of the Allothermal gasifier. Light tars are removed
Fig. 4 shows the CFB configuration. Wood chips are pres- from the oil with air in a stripper (OS in Fig. 5). The air/light tar
surized by a lock hopper system and fed into the gasifier which mixture is pre-heated and used as fuel enriched combustion
operates at 1 MPa and 850  C. Producer gas leaving the gasifier is air in the combustion section (MC in Fig. 5) of the Allothermal
cooled down to 400  C. Most of the dust (carbon containing ash) gasifier. For the rest the SNG production steps are the same as
is removed from the producer gas by a cyclone. The remaining in the previous case. Air is added to the flue gas leaving the
dust and tar are dissolved in oil in the Olga gas cleaning system. fluidized bed combustor (MC in Fig. 5) in the freeboard or after
Heavy tars are removed in the collector (OC in Fig. 4) and light burner section (MA in Fig. 5) to reduce CO and CxHy emissions.
tars are removed in the absorber (OA in Fig. 4). Heavy tars and The flue gas is cooled and dedusted by a bag-house filter
a small amount of ash are recycled back to the gasifier. Light before it is sent to the stack. Heat is used for steam production.
tars are removed from the oil with steam in a stripper (OS in
Fig. 4). The steam/light tar mixture is pre-heated and sent back
to the gasifier. Prior to the sulphur and chloride removal by 2.1. Fuel pre-treatment
adsorbents the producer gas is pre-heated to 250  C. The
cleaned gas is then pre-heated, moisturized and converted into In case of Entrained Flow gasification a pre-treatment step is
methane in several methanation reactors. The heat produced is required to be able to feed the biomass into the gasifier. Tor-
used for steam generation. Water and carbon dioxide are refaction is seen as the most logical pre-treatment step for
removed from the gas before the SNG is compressed to 3 MPa Entrained Flow gasification [3]. The energy required for milling
and injected into the natural gas grid. the fuel is significantly reduced and the fuel contains less H2O,
Fig. 5 shows the system based on the Allothermal gasifier. which improves the cold gas efficiency of an Entrained Flow
Wood chips are fed into the gasifier (MG in Fig. 5) which gasifier. Torrefaction also reduces transportation and storage
operates at atmospheric pressure and 850  C. Producer gas costs for biomass [4]. For the fluidized bed gasifiers no such
leaving the gasifier is cooled down to 400  C. Most of the dust pre-treatment is required. Because the torrefaction process

3 MPa 1300°C
Biomass T EF
CO2 600°C 250°C

Fly ash
O2 Ash

210°C 280°C 160°C 250°C

Methanation Methanation Water


ZnS NaCl 150°C ZnS

SNG (+ H2)
Air MD steam
Syngas MD steam, superheated
H2O CO2 Ash Waste heat

Fig. 3 – Scheme of EF SNG system.

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001
ARTICLE IN PRESS
4 biomass and bioenergy xxx (2009) 1–10

850°C 1 MPa 400°C 150°C

Biomass CFB OC OA OS
CO2

O2

200°C 160°C 10 bara 250°C

Methanation Methanation Water


ZnS NaCl ZnS
150°C LD steam,180°C
3 MPa
SNG (+ H2) LD steam, 250°C
Producer gas LD steam, 480°C
CO2 Tar / Dust Waste heat
H2O

Fig. 4 – Scheme of CFB SNG system.

requires a relatively dry fuel to operate without additional treatment [5]. For this study a moisture content of 3.5% was
heat input wood with 15% moisture was selected as the input assumed. The torrefied biomass particles fed into the gasifier
fuel for all three systems in this comparison. Integrating have to be relatively small to be completely converted into
a dryer using low temperature waste heat will increase effi- syngas. An average particle size of 0.1 mm is assumed. The
ciencies (on LHV basis) for all systems, but drying is not required milling electricity is 17 kWe MWth1 input (LHV) [3].
considered in this study. Table 1 gives the composition of clean wood and torrefied
The energetic efficiency of the torrefaction process as wood used in this study. Data have been taken from the
estimated from data published by ECN for dry wood [3,5], was Phyllis biomass database (www.ecn.nl/phyllis/, accessed on
assumed to be 90% on HHV basis and 93% on LHV basis. The 23.11.2007). The ash content of wood is estimated to be 1%.
electricity consumption of the torrefaction process is assumed The composition of the torrefied wood is derived from ECN
to be 1% of the biomass input (on LHV basis). At the moment of measurements.
writing the ECN torrefaction pilot plant is under construction. It should be noted that the heating values of wood can vary
More reliable data for overall efficiency and electricity substantially [6] and have a strong effect on calculated cold gas
consumption of the process will be available in the future. The efficiencies of the gasifiers. The heating values and composi-
moisture content of torrefied biomass varies between 1 and tions for clean wood given in Table 1 are an average of
6% depending on the torrefaction conditions and the post- approximately 200 samples of different types of wood, so the

900°C 100 kPa 80°C


100°C 400°C
MA MC MG
OC OA OS

Ash

CO2 Biomass
E E

200°C 280°C° 160°C 250°C

7 bara
Methanation Methanation Water
ZnS NaCl ZnS
3 MPa
SNG (+ H2)
Air LD steam, 180°C
Producer gas LD steam, 480°C
H2O CO2
Tar / Dust MD steam, 275°C
Waste heat MD steam, 480°C

Fig. 5 – Scheme of Allothermal gasifier SNG system.

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001
ARTICLE IN PRESS
biomass and bioenergy xxx (2009) 1–10 5

bed gasifiers [10]. To reduce the risk of agglomeration the


Table 1 – Composition of wood used in analysis.
oxygen is diluted with steam. The selected steam to oxygen
Clean wood Torrified wood ratio is 1 (kg kg1). It should be noticed, however, that this
Moisture (wt% a.r.) 15.0 3.5 assumption has a major impact on overall efficiency. VTT in
Ash (wt% d.b.) 1.0 1.1 Finland has built a pressurized steam/oxygen blown CFB
C (wt% d.a.f.) 50.7 56.1 biomass gasifier, but at this moment no experimental results
H (wt% d.a.f.) 6.1 5.7 are available in the public domain. ECN has previously done
O (wt% d.a.f.) 42.8 37.9
some experiments with atmospheric steam/oxygen blown
N (wt% d.a.f.) 0.3 0.3
CFB gasification where the steam to oxygen ratio was taken
S (wt% d.a.f.) 0.06 0.06
Cl (wt% d.a.f.) 0.05 0.05 similarly to the ratio assumed in this study.
LHV (MJ kg1 d.a.f.) 18.8 20.8 A heat loss of 1% from the reactor was assumed as for the
LHV (MJ kg1 d.a.f.) 15.4 19.7 EF gasifier. For this study a carbon conversion of 90% was
HHV (MJ kg1 d.a.f.) 20.1 22.0 assumed. This assumption is based on published data [11] and
HHV (MJ kg1 d.a.f.) 16.9 21.0 practical experience from the ECN CFB gasifier BIVKIN [12].
The system for the Allothermal gasifier is based on the ECN
Milena technology [13,14]. The basic working principles of the
inaccuracy in the heating value is negligible. The number of Milena gasifier are similar to the Silvagas [15] Allothermal
representative samples for torrefied wood is still low, so the gasifier. Biomass is fed into a riser where a small amount of
heating value can be inaccurate. superheated steam is added (5 wt% of the biomass input). Hot
bed material (typically sand) enters the riser from the
combustor through a hole in the riser, which is located under
2.2. Gasifiers the biomass feeding point. The bed material heats the
biomass to typically 850  C. The heated fuel particles degasify
The Shell type high temperature slagging Entrained Flow and create a vertical linear velocity of approximately 6 ms1,
gasifier was selected because this is the only commercial high leading to a ‘‘turbulent fluidization’’ regime in the riser and
temperature gasifier where solid biomass has been gasified so a carry-over of the bed material together with the degasified
far (co-fired with coal) [7]. It uses oxygen as gasification agent, biomass particles (char). The vertical velocity of the gas is
containing only 1% of nitrogen to minimize the amount of reduced in the settling chamber, causing the larger solids (bed
nitrogen in the syngas. The inert gas (CO2) requirement for material and char) to separate from the gas and to fall down
pneumatic feeding was calculated to be 6 dm3 kg1 biomass. into the downcomer. The producer gas leaves the reactor from
This is based on a void fraction of 0.75 required for dense the top and is sent to the cooling and gas cleaning section. The
phase transport and a particle density of 500 kg m3. It is char is burnt in the bubbling fluidized bed, were it heats the
assumed that the amount of water present in the fuel is bed material to approximately 925  C. The heated bed material
sufficient to prevent the formation of soot in the gasifiers so leaves the bubbling fluidized bed from the bottom and is sent
no external steam has to be added to the gasifier. The slag to the riser again. Measurement in the lab-scale Allothermal
flowing down the reactor wall is kept liquid by controlling the gasifier, Milena, have shown that the nitrogen content in the
mineral composition [8]. To maintain the right composition producer gas can be as low as 1 vol% (in dry gas) by purging the
and the right amount of slag to cover the membrane wall of feeding system with CO2 and minimizing the flue gas leaking
the reactor a flux material is added. The amount of flux added from the combustor to the gasifier. A leakage of flue gas from
is assumed to be 8 wt.% of the biomass. The typical operating combustor to gasifier of 1% is calculated from the measured
temperature of an Entrained Flow gasifier is between 1300 and nitrogen concentration in the producer gas.
1500  C. At lower temperatures the fuel is not converted The carbon conversion (CC) in the Allothermal gasifier was
completely and the viscosity of the slag can become too high. calculated using the following relation:
Higher temperatures decrease the cold gas efficiency (CGE).
The temperature selected is a tradeoff between fuel conver- CC(%) ¼ 65 þ 0.15 * (T-760); T in  C
sion and cold gas efficiency. As the biomass is more reactive
then coal, a gasification temperature of 1300  C was selected This relation is an estimate based on experimental results
[8]. The assumed carbon conversion at this temperature is from the ECN Milena lab scale gasifier using wood particles
99.5%. Heat loss through the membrane wall of gasifier vessel between 0.3 and 3 mm and conversion data published for the
is assumed to be 2% of the thermal input (LHV basis) [9]. 1% of Battelle/Silvagas Allothermal gasifier [15]. Again a gasifier heat
the heat is used to produce medium pressure steam, the loss of 1% was assumed.
remaining 1% is seen as an overall heat loss. The gasifier exit gas compositions for all cases were
Conventional Circulating Fluidized Bed biomass gasifiers calculated using empirical relations and assuming an offset
use air as the gasification medium. This dilutes the producer temperature for water gas shift equilibrium. Table 2 shows the
gas with nitrogen, which will end up in the SNG and cannot be relations used for the two fluidized bed gasifiers and the
easily removed. To prevent this nitrogen dilution oxygen has Entrained Flow gasifier. Table 3 shows the calculated gas
to be used as gasification medium. Replacing air by oxygen compositions.
will increase the chance of local hot spots in the fluidized bed ER (equivalence ratio) is defined as the amount of oxygen
resulting in an increased risk of agglomeration of the fed into the gasifier divided by the amount of oxygen required
bed material which is a major problem in operating fluidized for stoichiometric combustion of the biomass. The relation

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001
ARTICLE IN PRESS
6 biomass and bioenergy xxx (2009) 1–10

above the dew point of the tar in the gas. The heat is used to
Table 2 – Relations used to calculate gasifier outlet gas
composition. pre-heat the air to the Allothermal gasifier and/or to superheat
steam. In the Allothermal gasifier the fly ashes removed by
Component Fluidized bed Entrained Flow
a cyclone from the producer gas are sent back to the
1
CH4 (kg kg fuel d.a.f.) 0.0873–0.082 $ ER 0 combustor, where the carbon on the ash is converted into flue
C2H2 (mol mol1 CH4) 0.02 $ CH4 0 gas. The completely converted ashes are blown out of the
C2H4 (mol mol1 CH4) 0.32 $ CH4 0
combustor and are collected in a bag-house filter. The carbon
C2H6 (mol mol1 CH4) 0.02 $ CH4 0
containing ashes from the CFB gasifier are disposed. Tar and
C6H6 (mol mol1 CH4) 0.08 $ CH4 0
C7H8 (mol mol1 CH4) 0.01 $ CH4 0 remaining dust are removed by the Olga gas cleaning tech-
NH3 (mol mol1 N) 0.5 $ N in fuel 0 nology [17]. The Olga gas cleaning system comprises of three
H2S (mol mol1 S) 0.9 $ S in fuel 0.9 $ S in fuel stages. In the first stage, the collector (OC in Figs. 4 and 5),
COS (mol mol1 S) 0.1 $ S in fuel 0.1 $ S in fuel heavy tars are condensed from the gas by contacting the gas
with cooled scrubbing oil. Most of the fine dust which passes
through the upstream cyclone is also removed with the
given in the table and used in the model for the yield of scrubbing liquid. Dust and heavy tar are separated from the oil
methane as function of ER was published by Maniatis [16]. and returned to the gasifier. In the Allothermal gasifier the
These relations correspond well with ECN measurements heavy tar is used as fuel for the combustor. In the second
from Bubbling Fluidized Bed, Circulating Fluidized Bed and stage, the absorber (OA in Figs. 4 and 5), light tar components
Allothermal gasification between 800 and 900  C at atmo- are dissolved in the oil. The absorber is operated above the
spheric pressure and wood as fuel. The relations for the higher water dew point to prevent condensation of water. Producer
hydrocarbons were determined from experiments in the ECN gas exiting the OLGA absorber is free of condensable tars. The
lab scale Milena gasifier [14]. The influence of pressure on the oil from the absorber is sent to the third stage of the Olga
formation of hydrocarbons in fluidized bed biomass gasifiers system, the stripper (OS in Figs. 4 and 5). The stripper is either
is not known yet, therefore the same relations as for atmo- operated with air at 180  C (Allothermal gasifier) or with steam
spheric operation were used. The tar concentration in the raw at 210  C (CFB gasifier). The air or steam leaving the stripper
producer gas is 30 g Nm3 dry for both fluidized bed gasifiers. contains some oil, which can be partly regained in
This figure is relatively high because no catalytic active bed a condenser if air is used to operate the stripper. The oil
material, like olivine, is used in the gasifier to reduce the tar consumption of the Olga system is 100 mg Nm3 for the
concentration and tar from the gas cleaning section is stripper operated on air (Allothermal gasifier) and 1 g Nm3 for
returned to the gasifier in the case of CFB gasification. The the stripper operated on steam (CFB). The oil consumption is
water gas shift equilibrium was set at 1200  C for the fluidized only a fraction of the thermal input of the plant and is
bed gasifiers and at operating temperature for the EF gasifier. therefore neglected in the overall heat balance. More infor-
Chloride (as HCl) and NH3 leaving the gasifiers have minor mation on the Olga can be found on the website www.
influence on the overall energy balance and were therefore Olgatechnology.com.
neglected.

2.4. Cl and sulphur removal


2.3. Gas cooling and gas cleaning
Clean biomass like wood contains low amounts of sulphur
Syngas from the Entrained Flow gasifier is cooled down to
and chloride. A 1 GWth gasifier fed with clean wood produces
600  C by quenching with its own cooled gas of 250  C. A gas
2.5 Mg day1 of sulphur. Typically 90% of the sulphur converts
quench was chosen to prevent salt condensation and depo-
into H2S and 10% into COS. Other organic sulphur compounds
sition on the downstream heat exchangers. The gas is cooled
are neglected in this study. Measured HCl concentrations in
further by a conventional heat exchanger. The heat is used to
raw producer gas are low (<5 ppm). The Cl concentration in
produce steam.
wood is low already and most of the chloride is removed from
Producer gas leaving the CFB or Allothermal gasifier is
the gas together with the ash. The maximum allowable
cooled down to 400  C. This temperature is selected to stay
sulphur inlet concentration for the different methanation
catalysts is not known yet. An acceptable inlet concentration
of 100 ppb was assumed for this study. A ZnO sorbent was
selected for the bulk sulphur removal. This sorbent can
Table 3 – Required steam to dry gas ratios to prevent soot remove H2S and COS. Non-regenerative processes are
formation. commercially available and regenerative processes are under
Gasifier Operating Final Steam to dry development. The removal principal is based on the following
pressure methanation gas ratio equilibrium:
methanation temperature ( C) (mol mol1)
unit (MPa)
ZnO þ H2S 4 ZnS þ H2O
EF 3 280 1.4
CFB O2/Steam 1 280 1.4
In this case the majority of H2S is removed at 250  C. A
Allothermal 0.7 280 1.5
guard bed removes the remaining H2S at a slightly lower

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001
ARTICLE IN PRESS
biomass and bioenergy xxx (2009) 1–10 7

temperature (160  C). The same guard bed reactor is used to


remove HCl. In the case of Fluidized Bed gasification other 2.7. Steam system
organic sulphur compounds are present in the producer gas as
well. It is assumed that these components are converted to All enthalpy streams from the process with a temperature
H2S and removed by the ZnO sorbent. ECN is testing different greater than 200  C are used within the system to generate
sorbents/catalysts for this goal. Ammonia removal is not steam or pre-heat combustion air. The remaining low
included in the analysis. temperature heat is sufficient for heating up all feed water to
150  C. Most of the heat is used to produce low pressure
(1 MPa) and medium pressure (60 MPa) steam of which
2.5. Methanation a significant part is mixed into the producer gas before the
methanation unit to prevent soot formation. The remaining
CO and H2 in the cleaned gas are converted into methane by steam is sent to medium and low pressure steam turbines. An
the following strongly exothermic reactions: isentropic efficiency of 80% and a mechanical efficiency of 98%
were assumed for the steam turbines.
1
CO þ 3H2 4CH4 þ H2 O DHr ¼ 217 kJ mol
1
CO2 þ 4H2 4CH4 þ 2H2 O DHr ¼ 178 kJ mol
2.8. Electricity consumption
The generated heat is used to produce steam. In the case of
An overall electricity consumption of 1.5% of biomass input to
Fluidized Bed gasification a major problem is the formation of
the gasifier (HHV basis) was assumed. Major electricity
soot in the methanation reactors which deactivates the cata-
consumers like the air separation unit and the different gas
lyst and blocks the system. The presence of higher hydro-
compressors, are not included in this figure and calculated
carbons in the producer gas seems to enhance the formation
separately. An isentropic efficiency of 80% and a mechanical
of soot on the methanation catalysts [18]. The required
efficiency of 98% were assumed for the gas compressors. The
boundary conditions to prevent the formation of soot on the
cryogenic air separation unit consumes 0.4 kWhe Nm3
methanation catalyst are not well known yet, but in theory it
oxygen [21].
can be suppressed by adding steam prior to the methanation.
Table 3 shows the resulting steam to dry gas ratios for the
three different configurations on the basis of Aspen Plus
calculations. 3. Results and discussions
The steam gas mixture is pre-heated to 350  C before it
enters the first methanation reactor. The performance of a gasifier is given by its Cold Gas Efficiency
(CGE), which is defined here by the heating value of the dry,
cold producer gas after gas cleaning divided by the heating
value of the biomass or torrefied biomass to the gasifier. The
2.6. SNG upgrading CGE on HHV basis is defined as the higher heating value of the
dry and cleaned gas divided by the higher heating value of the
The SNG upgrading step is similar for the different systems; biomass. The CGE on LHV (lower heating value) basis is
therefore this step is not modeled in detail. Gas leaving the defined as the lower heating value of the dry and cleaned gas
last methanation reactor is cooled and water is condensed out (thus excluding condensation heat of water in the gas
of the gas which is then compressed to 3 MPa (if required). produced when the gas is combusted) divided by the lower
Different CO2 removal technologies are commercially heating value of the biomass. Fig. 6 shows the calculated cold
available; PSA (Pressure Swing Adsorption), Physical absorp- gas efficiencies for the different gasifiers.
tion (e.g. Selexol process) or membrane gas separation (UOP
Separex membrane). In this study CO2 is assumed to be
removed for 98%. The energy consumption for CO2 removal is 85
calculated from the required pumping energy for the solvent LHV
HHV
in a Selexol unit [19]. The methane loss is assumed to be 1%.
Cold gas efficiency (CGE) [%]

The CO2 rich gas is sequestrated in empty gas fields, which 81.1
80.0
means that the overall process becomes CO2 negative. The 80
required compression energy is not included in the calculated
77.4
overall efficiency.
The Swiss national standard for unlimited gas injection 75.9
74.9
limits the hydrogen concentration in SNG to 5 vol% [20]. This 75
73.7
value was used in this study as the maximum allowable
hydrogen concentration in the final SNG. The hydrogen
concentration can be kept below this concentration by
70
choosing the appropriate operating conditions (temperature
EF Torrefied wood 3 MPa CFB oxygen 1 MPa Allothermal 100 kPa
and pressure) of the last methanation reactor. Although
additional hydrogen removal is not required, selective oxida- Fig. 6 – Cold Gas Efficiencies for the three different biomass
tion could be applied if necessary. gasifiers.

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001
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8 biomass and bioenergy xxx (2009) 1–10

40
Latent heat combustor Pre heating air / oxygen / steam
35 Latent heat producer gas / syngas Heat from reactor vessel
Carbon loss

Loss in Cold Gas Efficiency [LHV%]


30

25

20

15

10

-5

-10
EF Torrefaction 3 MPa CFB oxygen 1 MPa Allothermal 100 kPa

Fig. 7 – Visualization of losses in Cold Gas efficiency (CGE).

It should be noted that the cold gas efficiency presented for net electricity production in the EF based system is the signifi-
Entrained Flow gasification (EF) does not include the efficiency cantly higher production of steam in both the syngas cooler and
from wood to torrefied wood. Torrefaction gives a loss of the methanation unit. The overall efficiencies are higher on
approximately 10% on HHV basis and 7% on LHV basis. The HHV basis than on LHV basis. It is caused by the conversion of
torrefaction process is still under development. The efficiencies CO into CH4 in the methanation reactors. The lower and higher
assumed for torrefaction are based on preliminary data. Fig. 7 heating values of CO are equal, while the higher heating value of
visualizes the different losses on Cold Gas Efficiency for the CH4 is higher than the lower heating value.
three gasifiers. The main loss in cold gas efficiency for the Gross and net overall efficiencies on LHV and HHV basis are
Entrained Flow gasifier is due to the latent heat in the syngas. highest for the Allothermal atmospheric gasifier. These high
The gasifier exit temperature of the Entrained Flow gasifier is values are due to the low losses, both heat and unconverted
z450  C higher than the exit temperatures of the two fluidized carbon, and the fact that the gas from the gasifier already
bed gasifiers. The main losses for the CFB gasifier are due to the contains a significant amount of hydrocarbons. These hydro-
unconverted carbon in the ash and the latent heat in the carbons, as indicated in Table 3, amount to a 55% contribution
producer gas. The Allothermal gasifier has the highest cold gas to the calorific value of the producer gas. Hydrocarbons are
efficiency, because the losses are reduced to a minimum. The converted into methane with a relatively high efficiency
combined latent heat in flue gas and producer gas is the high- compared to conversion of syngas into methane. The gas after
est, but is compensated by pre-heating the combustion air. the methanation reactors in all three systems contains
Table 4 gives the gas compositions for the three gasifiers approximately 60 mol% of water. All the condensation heat of
after tar removal. The concentration of methane and other
hydrocarbons in the gas from the Allothermal gasifier is higher
than the concentration in the gas from the CFB gasifier, because
the water concentration is lower and no methane is burnt. As Table 4 – Gasifier wet gas compositions (after tar removal,
can be seen in Table 2 the yield of hydrocarbons is a function of if applicable).
the air to fuel ratio (ER). A typical ER for an oxygen – steam EF Torrefied CFB Allothermal
blown CFB is 0.25. The air to fuel ratio in an Allothermal gasifier wood 3 MPa oxygen 1 MPa 100 kPa
is near zero, giving the maximum yield in hydrocarbons. A high CO (mol%) 49.8 18.7 25.9
initial concentration of methane and other hydrocarbons has H2 (mol%) 18.6 14.4 21.3
a positive influence on overall efficiency to SNG. CO2 (mol%) 14.7 19.8 12.0
The overall efficiencies to SNG are calculated on a net and O2 (mol%) 0.0 0.0 0.0
gross basis. Gross efficiency does not take into account the H2O (mol%) 16.5 39.2 24.8
CH4 (mol%) 0.0 5.1 10.3
electricity production or consumption of the system. To calcu-
N2 þ Ar (mol%) 0.3 0.4 0.9
late the net efficiency the electricity consumed (or produced) is C2H2 (mol%) 0.0 0.1 0.3
assumed to be produced by converting SNG into electricity C2H4 (mol%) 0.0 1.7 3.4
assuming an efficiency of 60% for electricity generation. Fig. 8 C2H6 (mol%) 0.0 0.1 0.2
shows the calculated overall efficiencies of biomass to SNG at C6H6 (mol%) 0.0 0.3 0.6
3 MPa. As can be seen from the figure the gross efficiencies to C7H8 (mol%) 0.0 0.0 0.1
H2S (ppm) 195 200 314
SNG are relatively low for Entrained Flow gasification. The net
COS (ppm) 22 22 35
efficiency is higher, because the system produces electricity.
NH3 (ppm) 0 1471 2308
The other two systems consume electricity. The reason for the

Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
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ARTICLE IN PRESS
biomass and bioenergy xxx (2009) 1–10 9

75
LHV (gross)
HHV (gross) 70.9
LHV (net) 70.3
70
HHV (net)
67.8
66.8

Efficiency to SNG [%]


65 64.1
63.5

60 59.2
58.1

55 54.3 54.7
52.7 53.2

50
EF Torrefaction 3 MPa CFB oxygen 1 MPa Allothermal 100 kPa

Fig. 8 – Gross efficiency to SNG and net efficiency to SNG and electricity.

this water (approximately 20% of the thermal input) is not used in the natural gas grid are not yet clear and may vary per
in the defined systems. If a biomass dryer is integrated in the country.
system this low temperature heat can be used to dry the Because of the significant differences in overall efficiencies
biomass. Integrating the drying step will increase overall effi- to SNG for the different gasifiers, ECN has decided to select the
ciency for all defined systems. Another possible improvement Allothermal gasification as the preferred technology for the
of the systems efficiency is reduction of the amount of steam production of SNG. ECN works on the development of its own
required in the different methanation steps to prevent forma- Allothermal gasification concept (Milena). Other Allothermal
tion of soot. The amount of steam required currently is based gasification concepts under development or demonstration
on thermodynamic and not kinetic considerations. are the Silvagas [22] and the FICFB process [23]. A particularly
The methane yield is possibly increased by pressure. This attractive aspect of the Milena design is integration of the
will have a positive effect on overall efficiency to SNG. The different processes in one reactor vessel. This makes
Allothermal gasifier is operated at atmospheric pressure, construction of small scale pilot and demo installations rela-
because pressurized operation of an Allothermal gasifier is not tively cheap and pressurization of the process relatively easy.
yet demonstrated. In principle it is possible to operate an A lab-scale version (30 kWth input) has been in operation
Allothermal gasifier at elevated pressures which will further since 2004 and is being optimized for the production of SNG by
increase the overall efficiency. maximizing methane yield. The new 0.8 MWth pilot plant,
Table 5 shows the calculated concentrations of the major coupled to the existing Olga gas cleaning system, will be put
components in the produced SNG after water and CO2 into operation at the beginning of 2008. A 10 MWth demon-
removal. All volumes are defined at 273.15 K and 101.325 kPa. stration is foreseen for the near future.
As can be seen the calculated heating values are similar. The
amount of hydrogen is lower in the case of EF gasification,
because the methanation pressure is higher. The concentra-
Acknowledgements
tion of CO is below 0.1 mol% in all cases. The gas composition
can be influenced by changing the level of CO2 removal.
Financial support from SenterNovem is acknowledged.
From a technical point of view the gas should be suitable to
replace fossil natural gas, but exact specification for injection
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doi:10.1016/j.biombioe.2009.11.001
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Please cite this article in press as: Christiaan M. van der Meijden et al., The production of synthetic natural gas (SNG): A
comparison of three wood gasification systems for energy balance and overall efficiency, Biomass and Bioenergy (2009),
doi:10.1016/j.biombioe.2009.11.001

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