i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 7 6 1 6 e7 6 2 2

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Life cycle assessment of hydrogen production

from biomass gasification. Evaluation of
different Spanish feedstocks

J. Moreno a, J. Dufour b,c,*

a
Department of Chemical and Environmental Technology, ESCET, Universidad Rey Juan Carlos, c/ Tulipán s/n,
28933 Móstoles, Madrid, Spain
b
Department of Chemical and Energy Technology, ESCET, Universidad Rey Juan Carlos, c/ Tulipán s/n,
28933 Móstoles, Madrid, Spain
c
IMDEA Energı́a, c/ Tulipán s/n, 28933 Móstoles, Madrid, Spain

article info abstract

Article history: Gasification of biomass can be used for obtaining hydrogen reducing the total greenhouse gases
Received 13 April 2012 emissions due the fixation of CO2 during photosynthetic processes. The kind of raw materials is
Received in revised form an important variable since has a great influence on the energy balance and environmental
8 November 2012 impacts. Wastes from forestry are considered as the most appropriate raw materials since they
Accepted 16 November 2012 do not compete for land. The aim of this work is to determine the environmental feasibility of
Available online 21 December 2012 four Spanish lignocellulosic wastes (vine and almond pruning and forest waste coming from
pine and eucalyptus plantation) for the production of hydrogen through gasification. LCA
Keywords: methodology was applied using global warming potential, acidification, eutrophication and the
Life cycle assessment gross energy necessary for the production of 1 Nm3 of hydrogen as impact categories. As ex-
Biomass pected, the use of biomass instead of natural gas leads to the reduction of CO2 emissions.
Gasification Regarding to the different feedstocks, biomass coming from forestry is more environmental-
Hydrogen friendly since does not need cropping procedures. Finally, the distribution of environmental
charges between pruning wastes and fruits (grape and almond) and the use of obtained by-
products have a great influence, reducing the environmental impacts.
Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
reserved.

1. Introduction reductions of greenhouse gases (GHG) emissions, since CO2 is

Hydrogen can be considered as the most appropriate alterna-
tive for a future de-carbonized energy scenario. It can be
produced from a wide variety of primary energy sources and
production technologies [1]. Nowadays, thermo-catalytic and
gasification processes starting from fossil fuels (natural gas,
heavy oils and coal) are the most usual systems but, as known,
they contribute to the greenhouse effect. Biomass can be
used for hydrogen production through gasification, leading to
fixed during plant growth due to photosynthetic processes.
Therefore, it has received increasing attention in the last years
[1e3]. There is a wide variety of biomass resources that can be
converted into energy products (including hydrogen) [4]: many
kinds of crops, agricultural/forestry wastes and industrial/
municipal wastes. In inland regions of Spain, some of the most
usual biomass sources for energy are forestry waste coming
from pine (5 M ha. of cultivated land) and eucalyptus (0.5 M ha.
of cultivated land) and pruning waste from grapevine (5 M ha.

* Corresponding author. Department of Chemical and Energy Technology, ESCET, Universidad Rey Juan Carlos, c/ Tulipán s/n, 28933
Móstoles, Madrid, Spain. Tel.: þ34 914888138; fax: þ34 914887068.
E-mail address: javier.dufour@urjc.es (J. Dufour).
0360-3199/$ e see front matter Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijhydene.2012.11.076
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 7 6 1 6 e7 6 2 2
List of symbols
GHG greenhouse gases
LCA life cycle assessment
NER net energy ratio (calculated as: MJ contained in
1 Nm3 H2/total energy input)
NG natural gas
of cultivated land) and almond (0.5 M ha. of cultivated land)
[5e10]. Besides biomass coming directly from trees (by
pruning), other parts of the plant can be also used such as fruits
shell, fruits peel and waste produced during fruit manufacture,
i.e., cake from olive oil extraction. However, the production of
hydrogen from biomass has still some drawbacks such as the
low yield obtained (related to the low hydrogen content of
biomass: approximately 6% versus 25% existing in methane [2])
and the limited energy content of biomass (composition can
reach 40% oxygen), an inherent limitation of the process which
increases energy requirements and, thus, GHG emissions.
Therefore, the kind of raw materials used is an important
variable since it has a great influence on the energy balance
and environmental impacts. Likewise, the type of used
gasifiers (fixed or fluidized bed reactor) affects the products
distribution, operation conditions and type of necessary
treatments for raw materials and final products [3]. Fixed bed
gasifiers have been the traditional technology used for gasifi-
cation with operation temperatures around 1000  C. Depend-
ing of the air flow direction, these gasifiers are classified as
downdraft, updraft and cross-flow. Downdraft systems
require a well-defined fuel being difficult to change it (low
adaptability) whereas updraft fixed bed gasifiers are more
adaptable but give a gas with significant tar concentration,
increasing gas-cleaning problems. Fluidized bed gasifiers
ensure a very uniform temperature distribution and are rela-
tively flexible for changing fuel and/or biomass characteristics.
However, they present some operational problems such as the
formation of melt and agglomerates which disturb fluidiza-
tion. For this study we have supposed a fixed bed reactor for the
gasification of biomass produced in Spain because of the
higher number of works published [5e8,11].
Life cycle assessment (LCA) is a very useful tool for the
evaluation of whole processes (from extraction of raw
Fig. 1 e Overall system and boundaries for hydrogen production.
7617
PAH polycyclic aromatic hydrocarbons
PSA pressure swing adsorption
SR steam reforming
VOC’s volatile organic compounds
WGS wateregas shift
materials to wastes treatment: cradle-to-grave) in order to
know the main environmental impacts [12,13]. As known, LCA
methodology has some advantages in comparison with other
method for evaluation of environmental impacts such as:
systematic estimation of the environmental changes related
to the examined product or process, quantification of
consumptions and emissions and their effects on human
health and eco-systems and allocation of impacts in one or
more items of environmental interest. In this work, we eval-
uate the environmental feasibility, using LCA methodology, of
the production of hydrogen by gasification of several biomass
feedstocks typical in Spain (vine and almond pruning and
forest waste coming from pine and eucalyptus plantation) in
a fixed bed gasifier. GHG emissions, total energy require-
ments, acidification and eutrophication effects have been
determined for the different raw materials.
2. Methodology
2.1. Systems descriptions and LCA assumptions
The functional unit selected for the assessment was the
production of 1 Nm3 of hydrogen (purity ¼ 99.99%) from
several biomass sources (vine, almond, pine and eucalyptus)
through gasification and reforming of the obtained gas (so-
called syngas). After that, wateregas shift reaction (WGS) is
used to increase concentration of H2, and pressure swing
adsorption (PSA) is used to purify the product. Fig. 1 shows the
system boundaries and factors considered for life cycle
assessment which is focused on the raw material, energy
acquisition and manufacturing stages. It is important to
remark that the biomass transportation is not included in thus
evaluation since it can be affected by many factors particular
7618 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 7 6 1 6 e7 6 2 2
of each location. The study was carried out with Gabi 4.4
software [14] by using Ecoinvent 2.1 database [15].
In the stage of biomass production, all the cultivation
processes were considered: planting, land management,
biomass harvesting, forest or agricultural machinery, etc. In
the case of vine and almond pruning waste, requirements of
fertilizer and pesticides [14,16] were also taken into account.
For gasification stage, the inventory includes materials and
energy requirements for construction of gasification plant, for
operation and dismantling. The assumed lifetime of the plant
is 50 years. The gasifier is a fixed bed reactor operating at
1073 K according to information of Ecoinvent 2.1 database [15]
and experimental procedure described by Gañán et al. [5].
After gasification, a usual steam reformer is considered,
operating at 1100e1200 K and 30 bar with Ni/Al2O3 as catalyst,
assuming that 85% conversion is obtained. Non-converted
methane is treated as direct emission from the reformer to
the air in the base case. The wateregas shift reaction is carried
out in two fixed beds working at high and low temperature,
respectively, with intermediate cooling. Fe2O3eCr2O3eCuO is
used as catalyst for the high temperature stage, whereas
CuOeZnOeAl2O3 is used for the low temperature trans-
formation. Operation temperatures have been considered to
be 773 K and 573 K, respectively [17,18]. For H2 purification,
a conventional multi-bed PSA unit was considered working at
10 bar. Mass and energy balances corresponding to the
reformer, WGS reactor and PSA unit has been previously
described by Dufour et al. [17] and they are based on the data
published by Spath and Mann [18].
Each kind of evaluated biomass yields different amounts of
syngas which can have different composition. It is difficult to
fix these values, since there are several variables with a high
influence on the gasification processes [3]. For this study we
have selected data presented in Table 1 according to results
reported by Gañán et al. [5,6] Lapuerta et al. [7] and González
et al. [8]. Table 1 shows only the major components of the
gasification output. The nature of the remaining products is
very complex; propane, butane, toluene, benzene and other
VOC’s as well as some polycyclic aromatic hydrocarbons (PAH)
are the most usual compounds. Besides, small amount of NOx
and SOx coming from oxidation of nitrogen and sulfur of the
biomass are also present in this stream. For all the cases, these
by-products involve less than 10% of total volume.
Finally, Table 2 summarizes the main flows of mass and
energy for the different stages evaluated: biomass production,
gasification, reforming and WGS and purification by PSA. For
electricity calculation we have used the Spanish energy mix
corresponding to year 2010 [19].
The evaluation of the environmental feasibility was carried
out by using the following impact categories calculated
Table 1 e Yield and composition of gas as function of biomass gasified.
Biomass Gas production (Nm3/kg biomass) H2 (% mol)
Pine 1.9
Eucalyptus 1.8
Almond pruning 1.7
Vine pruning 2.0
according to CML2001 method: greenhouse gases emissions
(GHG), acidification and eutrophication. They were selected as
they can be considered the most appropriate and crop wastes.
Besides, the gross energy necessary for the production of
1 Nm3 of hydrogen was also estimated in order to determine
the most energy-efficient option.
2.2. Alternative scenarios
2.2.1. Influence of the by-products use
After gasification and treatment of syngas, non-converted CH4
can be recovered and used for reducing the energy demand of
the processes instead of be emitted to the atmosphere (like in
the base case). This option has been considered for the elab-
oration of the alternative scenario 1. The amount of recovered
methane was 0.005 kg CH4/Nm3 of H2 for almond pruning,
0.0064 kg CH4/Nm3 of H2 for vine pruning, 0.0087 kg CH4/Nm3
of H2 for eucalyptus and 0.0062 kg CH4/Nm3 of H2 for pine.
2.2.2. Environmental charges allocation
As known, the main objective of agricultural processes is the
production of the corresponding fruit (grape and almond) and
pruning wastes are by-products. In this sense, an obvious
possibility is to allocate all the cropping environmental
charges to fruit and none to pruning wastes. However,
nowadays these wastes are also considered as valuable
products for energy generation, so that, environmental
impacts coming from their production should be taken into
account. Obviously, the distribution of cultivation environ-
mental charges will have a high influence on the LCA results.
In this work, we have considered two different ways for
environmental charges allocation:
 Total environmental charges of cultivation are associated to
both products (fruit and pruning wastes). This allocation has
been used for the base scenario.
 Environmental charges of cultivation are distributed
according to products price: 1% of charges correspond to
almond pruning wastes and 10% of charges correspond to
vine pruning wastes. This allocation has been used for
building the alternative scenario 2.
3. Results and discussion
3.1. Environmental impacts of different feedstock: base
scenario
Fig. 2 shows GHG emissions produced in the different stages of
the gasification of all the evaluated feedstocks. As shown,
CO (% mol) CO2 (% mol) CH4 (% mol)
24.9 34.0 23.7 12.8
15.7 40.6 21.6 18.0
28.5 35.3 23.1 10.7
29.1 49.2 0.0 13.3
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 7 6 1 6 e7 6 2 2 7619

Table 2 e Main flows of mass and energy for the different stages evaluated (based on the production of the functional unit:
1 Nm3 of H2).
Process Stream Wood Water/Steam CO2 CO (Nm3) CH4a (Nm3) H2 (Nm3) Electricityb NGc (heat)
(kg) (kg) (kg) (MJ) (MJ)

Pine
Biomass production IN e e 2.66 e e e e e
OUT 1.32 e 0.72 e e e e e
Gasification IN 1.32 0.36 e e e e 0.24 e
OUT e e 0.57 0.37 0.14 0.26 e e
Reforming þ WGS IN e 0.50 0.57 0.37 0.14 0.26 0.32 12.2
OUT e e 1.40 0.01 0.01 1.00 e e
PSA IN e e 1.40 0.01 0.01 1.00 0.17 e
OUT e e 2.02 0.01 0.01 1.00 e e
Eucalyptus
Biomass production IN e e 2.74 e e e e
OUT 1.11 e 0.47 e e e e
Gasification IN 1.11 0.36 e e e e 0.24
OUT e e 0.53 0.40 0.16 0.18 e e
Reforming þ WGS IN e 0.55 0.53 0.40 0.16 0.18 0.35 12.2
OUT e e 1.57 0.02 0.02 1.00 e e
PSA IN e e 1.57 0.02 0.02 1.00 0.17 e
OUT e e 2.13 0.02 0.02 1.00 e e
Almond pruning
Biomass production IN e e 3.17 e e e e e
OUT 1.44 e 1.78 e e e e e
Gasification IN 1.44 0.36 e e e e 0.24 e
OUT e e 0.56 0.39 0.12 0.31 e e
Reforming þ WGS IN e 0.52 0.56 0.39 0.12 0.31 0.31 12.0
OUT e e 1.31 0.01 0.01 1.00 e e
PSA IN e e 1.31 0.01 0.01 1.00 0.17 e
OUT e e 1.97 0.01 0.01 1.00 e e
Vine pruning
Biomass production IN e e 2.19 e e e e e
OUT 1.01 e 1.23 e e e e e
Gasification IN 1.01 0.36 e e e e 0.24
OUT e e 0.05 0.44 0.12 0.26 e e
Reforming þ WGS IN e 0.55 0.05 0.44 0.12 0.26 0.35 12.2
OUT e e 0.05 0.01 0.01 1.00 e e
PSA IN e e 0.97 0.01 0.01 1.00 0.17 e
OUT e e 1.58 0.01 0.01 1.00 e e

a CH4 calorific power: 37.4 MJ/Nm.3.

b According to Spanish energy mix, year 2010 [19].
c NG: Natural Gas.

total CO2 emissions are higher for almond and vine pruning
than for forest raw materials. The utilization of fertilizers and
pesticides during the biomass growth step produce this trend
since pine and eucalyptus do not require them, whereas they
are usually employed for almond and grapevine cultivation.
The total balance of CO2 is negative for eucalyptus, indicating
that fixation of carbon during biomass growth [15] is higher
than those emissions corresponding to the rest of stages. In
this point, it must be considered that the CO2 balance has been
carried out without consider gasification by-products use.
This means that emissions coming from their combustion are
not included, making possible obtaining a negative value for
CO2. This situation occurs only for eucalyptus because of its
highest carbon fixation during biomass production.
The value of GHG emissions in gasification step for vine
pruning is remarkable. That is related with data of Table 1 [5],
because there is not a direct formation of CO2 during the
Fig. 2 e CO2 emissions produced by the different stages of gasification reaction and the output stream of the gasifier is
gasification processes. composed by CO and CH4, which are the inputs for the next
7620 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 7 6 1 6 e7 6 2 2

step and, thus, they do not contribute to GHG emissions.

Table 3 e NER values obtained for gasification processes
Besides, this raw material leads to the less negative CO2 of each feedstock.
balance in the cultivation step [15] due to two factors: the use
Biomass Pine Eucalyptus Almond pruning Vine pruning
of fertilizers and pesticides and the higher yield to gas of vine
pruning, being necessary less biomass for obtaining 1 Nm3 of NER value a
0.47 0.52 0.37 0.41
hydrogen. In this sense, if less biomass is cultivated, less CO2 a Calculated as: calorific power of the hydrogen (10.8 MJ/Nm3)/total
is fixed. These factors also involve that the vine pruning is the energy input (MJ) from Fig. 3. Only the energy of the syngas is
feedstock with the highest emissions of CO2. considered. Energy contained in liquid and solid gasification
Previous works [17,18,20] have reported GHG emissions products is not included.
associated with the production of 1 Nm3 of hydrogen by
means of conventional natural gas reforming. According to
the process (electricity and heat), but not the energy associated
these studies, this technology leads to 0.95 kg-eq. CO2 per Nm3
with the raw material, i.e., the natural gas which reacts with
of H2 indicating that the gasification of any raw materials
steam water in the reformer.
evaluated here leads to better results.
Fig. 4 shows the evaluation of the produced acidification (a)
Fig. 3 shows energy requirements of the different stages for
and eutrophication (b) for all the biomass sources. These two
all the evaluated raw materials. The main differences can be
additional indicators have been also included in this study
observed in the biomass production step. As for GHG emissions,
because of their relevance for cultivation processes. For acid-
the eucalyptus presents the best result since it has the lowest
ification, the stage with higher contribution is the biomass
energy input. Probably, this fact seems to be related to the lower
production for almond pruning, vine pruning and, in a lower
energy requirements associated with several operations during
extension, for pine. The lower energy requirements necessary
biomass production, such as planting or harvesting, which
for production and harvesting of eucalyptus [21,22] leads to the
require less energy than that corresponding to pine [21,22]. For
minimum acidification for this raw material. This result agrees
almond and vine pruning, the use of fertilizers and pesticides
with data of Fig. 3. With regards to eutrophication impact, vine
leads to higher energy consumptions. Considering the calorific
and almond pruning show worse environmental behavior
value of the hydrogen (10.8 MJ/Nm3) as the energy output of the
than forest material due to the use of fertilizers and pesticides
system, it is possible to estimate the net energy ratio (NER) for
each feedstock. It is important to remark that these values
would be lower than those obtained if total energy contained in
biomass were considered for calculation. That is, not only
energy coming from gas (included in this work) but also that
corresponding to liquid and solid gasification by-products (not
considered here). Anyway, NER values (see Table 3) are used
only for comparison purposes and not as an indicator of the
energy feasibility of these processes. As expected, net energy
ratios are higher for forestry wastes (near to 0.5) than for vine
and almond pruning which show NER around 0.4 due to their
higher energy requirements. According to previous works
[17,20], fuel input necessary for obtaining 1 Nm3 of H2 by means
of natural gas reforming is 18.8 MJ, leading to a NER value of 0.57
(slightly higher than that corresponding to eucalyptus wastes).
However, this input only considers the energy consumption of

Fig. 3 e Energy consumption of the different stages of Fig. 4 e Acidification (a) and eutrophication (b) impacts
gasification processes. produced by gasification of each feedstock.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 7 6 1 6 e7 6 2 2
for biomass growth. In fact, the biomass production is the stage
responsible of more than 95% of the total eutrophication
observed. Therefore, also for these impact categories it is
possible to distinguish two kinds of biomass sources: forestry,
with very low inputs for growing, and produce, which consume
higher amount of resources for biomass growth.
Finally, the contribution of hydrogen production by NG
reforming in these two categories has been also considered for
comparison purposes. Thus, the production of 1 Nm3 of H2 by
means of this conventional process leads to 0.0018 kg-eq SO2
and 0.00013 kg-eq of PO4. This acidification indicator is slightly
higher than that of forestry wastes gasification due to the
sulfur content of natural gas used as raw material. Regarding
to eutrophication, biomass gasification leads to a higher
impact due to agricultural practices.
3.2. Evaluation of different scenarios
Fig. 5 shows total CO2 emissions and energy requirements for
each feedstock under the different evaluated scenarios. As
expected, the recovery and use of non-converted methane
lead to a significant reduction of CO2 emissions since CH4 is
not emitted and, at the same time, a fraction of energy
consumption is avoided. This last effect can be observed by
comparing the energy requirements of the base case and
alternative scenario 1. It is remarkable that, under assump-
tions of alternative scenario 1, both feedstocks coming from
forestry lead to a negative CO2 balance (without consider solid
and liquids gasification by-products). Anyway, eucalyptus is
the most favorable raw material also in this case.
Regarding to alternative scenario 2, the allocation of envi-
ronmental impacts of cropping between fruits and pruning
wastes allows reducing more than a 25% the energy require-
ments for hydrogen production. This decrease is higher for
almond pruning since the market price of almond is higher
than that corresponding to grape. Therefore, the percentage of
environmental charges associated with almond pruning is
lower (1% for almond pruning and 10% for vine pruning, see
Fig. 5 e CO2 emissions and energy consumption of the
hydrogen production by gasification of the different
feedstocks under the three evaluated scenarios.
7621
Section 2.2). Besides, an important reduction of acidification
and eutrophication is observed, it corresponds to the lower
contribution of cultivation activities which need fertilizer and
pesticides. Both environmental impacts are reduced around
a 90% for vine pruning and a 99% for almond pruning.
However, the allocation of environmental charges for culti-
vation has a negative effect on the CO2 emissions. As observed
in Fig. 5, CO2 emissions of vine and almond pruning for the
alternative scenario 2 are higher than those obtained for the
other evaluated cases. These results are due to the fixation of
CO2, occurring during cultivation step, which should be also
distributed between fruits and pruning wastes according to
allocation percentages. Under this situation, the CO2 credit
associated with the biomass growing decreases a 90% for vine
pruning and a 99% for almond pruning, leading to an impor-
tant increase of total GHG emissions.
4. Conclusions
Evaluation of raw materials indicate that the main factors
which affect to the environmental behavior of biomass gasifi-
cation are yield to gas, carbon fixation during biomass growth
and requirements of fertilizers and pesticides. Considering all
these variables, feedstocks coming from forestry are more
environmental-friendly since they do not need cropping
procedures, only planting, harvesting and grinding operation
(which are also required for biomass coming from crops).
Among all the raw materials evaluated, eucalyptus presents the
most promising results because it combines a good behavior
during gasification (high yield to gas) and very low require-
ments for biomass growth, achieving a high carbon fixation.
The study of alternative scenarios has shown that the
recovery and use of valuable products such as non-converted
methane improve the environmental behavior of all the raw
materials. Finally, the allocation of environmental charges
corresponding to cultivation has not only positive effects on the
use of pruning wastes. Thus, an important reduction of energy
requirements and other environmental impacts such as acidi-
fication and eutrophication can be achieved, but the CO2 credit
associated with the biomass growing almost disappears,
leading to an important increase of total GHG emissions.
Acknowledgments
The authors thank “Ministerio de Ciencia e Innovación” for the
financial support through the research project ENE2008-05471.
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