Hydrogen-Permeable Tubular Membrane Reactor: Promoting Conversion and Product Selectivity for Non-Oxidative Activation of Methane over an FeSiO2Catalyst

Article abstract of DOI:10.1002/anie.201609991

Non-oxidative methane conversion over FeSiO₂catalyst was studied for the first time in a hydrogen (H₂) permeable tubular membrane reactor. The membrane reactor is composed of a mixed ionic–electronic SrCe_0.7Zr_0.2Eu_0.1O_3?δthin film (≈20 μm) supported on the outer surface of a one-end capped porous SrCe_0.8Zr_0.2O_3?δtube. Significant improvement in CH₄conversion was achieved upon H₂removal from the membrane reactor compared to that in a fixed-bed reactor. The FeSiO₂catalyst in the H₂permeable membrane reactor demonstrated a stable ≈30 % C₂₊single-pass yield, with up to 30 % CH₄conversion and 99 % selectivity to C₂(ethylene and acetylene) and aromatic (benzene and naphthalene) products, at the tested conditions. The selectivity towards C₂or aromatics was manipulated purposely by adding H₂into or removing H₂from the membrane reactor feed and permeate gas streams.

Full text of DOI:10.1002/anie.201609991

Angewandte
Communications
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International Edition: DOI: 10.1002/anie.201609991
German Edition: DOI: 10.1002/ange.201609991
Heterogeneous Catalysis
Hydrogen-Permeable Tubular Membrane Reactor: Promoting
Conversion and Product Selectivity for Non-Oxidative Activation of
Methane over an FeꢀSiO2 Catalyst
Mann Sakbodin, Yiqing Wu, Su Cheun Oh, Eric D. Wachsman,* and Dongxia Liu*
Abstract: Non-oxidative methane conversion over FeꢀSiO2
catalyst was studied for the first time in a hydrogen (H2)
permeable tubular membrane reactor. The membrane reactor
is composed of a mixed ionic–electronic SrCe0.7Zr0.2Eu0.1O3Àd
thin film ( ꢀ 20 mm) supported on the outer surface of a one-
end capped porous SrCe0.8Zr0.2O3Àd tube. Significant improve-
ment in CH4 conversion was achieved upon H2 removal from
the membrane reactor compared to that in a fixed-bed reactor.
The FeꢀSiO2 catalyst in the H2 permeable membrane reactor
demonstrated a stable ꢀ 30% C2+ single-pass yield, with up to
30% CH4 conversion and 99% selectivity to C2 (ethylene and
acetylene) and aromatic (benzene and naphthalene) products,
at the tested conditions. The selectivity towards C2 or aromatics
was manipulated purposely by adding H2 into or removing H2
from the membrane reactor feed and permeate gas streams.
conversion has been predicted when a H2 permeable mem-
brane was used in conjunction with a NMC catalyst, the
parallel experimental studies on NMC process in membrane
reactors were not favorable due to the lack of membranes
with sufficient H2 permeation flux and the accelerated
catalyst deactivation under H2 removal conditions.[6b,d,10]
Herein we report a tubular membrane reactor (Figure 1)
that is comprised of a mixed ionic–electronic conducting
SrCe0.7Zr0.2Eu0.1O3Àd membrane and the ironꢀsilica
(FeꢀSiO2) catalyst to improving CH4 conversion while
maintaining catalyst durability and selectivity to C2 and
aromatic products under H2 removal conditions. The
SrCe0.7Zr0.2Eu0.1O3Àd membrane was designed with thickness
around 20 mm with an active surface area of 12 cm2 supported
on 1 mm thick SrCe0.8Zr0.2O3Àd tube with a diameter of 6 mm
(Figure 1A,B). This type of tubular membrane reactors have
been studied for H2 production from water-gas shift and CO2
reforming of CH4 reactions in previous reports.[11] FeꢀSiO2
catalyst has lattice-confined single iron sites embedded in the
silica matrix, which has been demonstrated to have superior
NMC performance by Bao and co-authors.[12] The integration
of the FeꢀSiO2 (containing 0.5 wt% Fe) catalyst in the
SrCe0.7Zr0.2Eu0.1O3Àd membrane reactor for NMC showed an
enhancement in CH4 conversion compared to that in a fixed-
bed reactor. The NMC reaction showed up to 30% CH4
conversion, 99% selectivity to C2 and aromatics, and a long
catalyst lifetime at the tested conditions. The product
selectivity towards light hydrocarbon (acetylene and ethyl-
ene) or heavy aromatics (benzene and naphthalene) was
manipulated by adding H2 into or removing H2 from the
SrCe0.7Zr0.2Eu0.1O3Àd membrane reactor. The tubular mem-
brane reactor design increases the H2 permeable surface area
and avoids need for sealing of membrane in the high
temperature heating zone, leading to more stable and
higher H2 permeation compared to the disk-shaped mem-
brane design in most previous studies.[6] Figure 1C demon-
strates the set-up of the H2 permeable membrane reactor for
the NMC reactions. To our knowledge, this is the first time
active, stable and tunable product selectivity has been
realized for NMC over FeꢀSiO2 catalyst in a H2 permeable
membrane reactor.
M
ethane (CH4), an abundant natural resource, is the main
constituent of natural gas and oil-associated gases. Studies on
CH4 conversion have explored indirect conversion of CH4 to
synthesis gas (CO + H2) followed by Fischer–Tropsch syn-
thesis of higher hydrocarbons,[1] oxidative coupling of CH4 to
C2+ hydrocarbons,[2] and non-oxidative CH4 conversion
(NMC) to H2, light hydrocarbons and aromatics.[3] In com-
parison with the first two approaches, NMC is more simple
and selective given its unique capability in forming C2+
hydrocarbons and H2 while circumventing the intermediate
energy intensive steps.[1a,3a,4] However, kinetic and thermody-
namic constraints in NMC lead to low CH4 conversion at
practical reaction conditions.[5]
Considerable efforts have been placed on the develop-
ment of membrane reactors comprised of active catalysts and
H2 permeable membranes for NMC reactions.[6] The molyb-
denum/zeolite (Mo/ZSM-5) has been the most extensively
studied catalyst.[7] H2 or O2 permeable membranes, such as
metal alloys[8] and ionic/electronic conducting ceramics,[6d–f,9]
capable of H2 withdrawal from or O2 addition into the reactor
were exploited to alleviate the barriers for equilibrium
conversion. Although a substantial enhancement of the CH4
[*] M. Sakbodin, Y. Wu, S. C. Oh, E. D. Wachsman, D. Liu
Department of Chemical and Biomolecular Engineering, University
of Maryland, College Park, MD 20742 (USA)
E-mail: ewach@umd.edu
The H2 permeation through the SrCe0.7Zr0.2Eu0.1O3Àd
membrane in the membrane reactor was measured prior to
the catalysis tests. Figure 2A shows that the permeated H2
flux was increased with the H2 concentration on the feed side.
In addition, the H2 permeation flux increased as the temper-
ature increased due to the increase in ambipolar conductivity
of the SrCe0.7Zr0.2Eu0.1O3Àd membrane. A further analysis
shows that the H2 permeation flux was proportional to the
liud@umd.edu
E. D. Wachsman, D. Liu
University of Maryland Energy Research Center, University of Mary-
land, College Park, MD 20742 (USA)
Supporting information for this article can be found under:
http://dx.doi.org/10.1002/anie.201609991.
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differences are expected,
according to Wagner equa-
tion[13] and Figure 2, to lead
to an increase in CH4 con-
version.
The
percent
increase in CH4 conversion
from fixed-bed to mem-
brane reactors, comparing
Figure 3A and B, however,
showed a decreasing trend.
The discrepancy in CH4 con-
version between this analy-
sis and experimentally mea-
surement might be caused
by deposition of carbon spe-
cies on the membrane sur-
face in the catalyst activa-
tion stage that reduced the
H2 flux or by complex
Figure 1. H2 permeable tubular membrane reactor and experimental setup for NMC reaction. A) As-prepared
SrCe0.8Zr0.2O3Àd membrane tube, B) SEM image showing the cross-sectional image of membrane tube reactor
comprised of SrCe0.7Zr0.2Eu0.1O3Àd thin film on the porous SrCe0.8Zr0.2O3Àd tubular support, and C) assembly of
H2 permeable membrane reactor for CH4 conversion in NMC over FeꢀSiO2 catalyst.
chemistry in membrane reactor which involved multiple
types of hydrocarbon species influencing H2 permeation
dynamics. The production and permeation rates of H2 at each
reaction temperature have been quantified (Table S1, Sup-
porting Information). The enhancement in CH4 conversion
caused by H2 removal has been evaluated by considering
a right-hand side shift of the reaction equation (CH4 =
3/52C6H6 + 5/104C10H8 + 7/104C2H4 + 2/104C2H2 + 19/
13H2) according to the Le Chꢁtelierꢂs principle. The calcu-
lated CH4 conversion is nearly the same as those measured
(Table S1), which indicated the effectiveness of the H2
permeable membrane reactor in shifting the CH4 conversion
in the NMC chemistry.
Figure 2. H2 permeation flux through SrCe0.8Zr0.2O3Àd membrane in the
packed-bed membrane reactor as a function of A) temperature and
B) H2 partial pressure, respectively.
transmembrane H2 partial pressure gradient with a 1/4
dependence (Figure 2B). The Wagner equation[13] explains
Figure 3 also shows the effects of H2 removal on the
product selectivity of the NMC reaction. In the fixed-bed
reactor, the reaction was very selective toward C2 (ethylene,
acetylene and ethane, ca. 90%), and only small amount of
aromatics (< 10%) were formed at 1223 K. As the temper-
ature increased, the selectivity shifted from smaller C2
products to aromatics (benzene, toluene and naphthalene).
Comparing the product selectivities between the fixed-bed
and the H2 permeable membrane reactors, the membrane
reactor was slightly less selective for C2 and more selective for
aromatic products. The yields for both C2 and aromatics of the
membrane reactor are higher at all temperatures tested
compared to the fixed-bed reactor.
The manipulation of the sweep side environment which is
expected to influence the catalysis chemistry inside the
membrane reactor was carried out by flowing sweep He gas
at different flow rates (20, 50 and 100 mLminÀ1) and switch-
ing He to H2 sweep gas, respectively. Figure 4A shows that
CH4 conversion increased with an increase of He flow to
50 mLminÀ1 and doubled at 100 mLminÀ1 He flow compared
to that in fixed-bed reactor. The high sweep He flow carried
away more H2 through the membrane reactor. The CH4
conversion was calculated based on the permeated H2
(Table S2, Supporting Information), and matched well with
the measured conversion in the membrane reactor. For
comparison, H2 was purposely added back to the membrane
reactor by flowing H2 as sweep gas. The CH4 conversion was
the
H2
permeation
behaviors
through
the
SrCe0.7Zr0.2Eu0.1O3Àd membrane in the tubular reactor (Sec-
tion S2, Supporting Information).
The CH4 conversion and product selectivity as a function
of reaction temperature in both fixed-bed and H2 permeable
membrane reactors are shown in Figure 3. An increase in CH4
conversion with increasing temperature was observed in both
types of reactors due to the endothermic nature of the NMC
reaction. The simultaneous removal of H2 from the mem-
brane reactor shifted the reaction to the product side, and
thus increased the CH4 conversion. Higher H2 permeation
flux at higher temperature and higher H2 partial pressure
Figure 3. CH4 conversion and product selectivity over FeꢀSiO2 cata-
lyst A) in a fixed-bed and B) packed-bed membrane reactor at different
temperatures (space velocity=3200 mLgÀ1 hÀ1).
2
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Figure 4. CH4 conversion and product selectivity over FeꢀSiO2 cata-
lyst in a packed-bed membrane reactor at different A) He or B) H2
sweep gas flow rates (temperature=1303 K, space velocity=
3200 mLgÀ1 hÀ1).
slightly reduced (Figure 4A and B) because the reaction was
shifted to the reactant side according to Le Chꢁtelierꢂs
principle.
Figure 5. Long-term stability test of the packed-bed H2 permeable
The product selectivity towards C2 or aromatics was tuned
by varying the type of sweep gases and their flow rates. The
selectivity to naphthalene increased with increasing He flow
rate (Figure 4A) while the C2 and benzene products increased
with increasing H2 flow rates (Figure 4B). Bao and co-
authors[12] hypothesized that the lattice confined single Fe site
initiates CH4 dehydrogenation to generate methyl (CCH3) and
hydrogen (CH) radicals, which subsequently release from the
surface and undergo a series of gas-phase reactions to form
dehydrogenated and cyclized products. The manipulation of
sweep gas type influences the concentrations and types of
hydrogen species in the reactor which impacts the product
selectivity. A control experiment was done by co-feeding H2
in the CH4 feed in the fixed-bed reactor to examine the
influence of H2 addition through the membrane reactor. To
significantly mitigate naphthalene formation, a concentration
of ca. 15% H2 in the CH4 feed was needed, which led to
a severe reduction in CH4 conversion (Figure S3, Supporting
Information). The slight sacrifice of CH4 conversion but
tuning product to C2 and benzene compared to naphthalene is
unique for the NMC reaction in the H2 permeable
SrCe0.7Zr0.2Eu0.1O3Àd membrane reactor. On the other hand,
an increase in CH4 conversion and aromatic product forma-
tion were achieved with the H2 permeable membrane reactor
with He sweep gas flow. Both ends of products are attractive
chemicals used in industry. The employment of the H2
permeable membrane reactor in the present study could
shift the building block supplies from the CH4 catalysis
chemistry.
The stability of the FeꢀSiO2 catalyst in NMC reaction in
the H2 permeable membrane reactor was tested by running
the reaction at 1303 K for 60 hours. No obvious deactivation
was observed during this test (Figure 5). The CH4 conversion
remained at ꢀ 20% throughout this run at this tested reaction
condition. Selectivities to C2 (65%), benzene (18%) and
naphthalene (15%) were constant, and the total selectivity to
these products remained > 99%. In contrast, H2 removal
resulted in accelerated coking on the Mo/ZSM-5 catalyst in
other membrane reactors.[6e,8a] This has been a major obstacle
to realize a practical NMC reaction in H2 permeable
membrane reactors. In addition to the stability of the
FeꢀSiO2 catalyst, this long-term test also demonstrated the
tubular membrane reactor with the FeꢀSiO2 catalyst at 1303 K and
3200 mLgÀ1 hÀ1 space velocity.
stability of the SrCe0.7Zr0.2Eu0.1O3Àd tubular ceramic mem-
brane reactor under reducing hydrocarbon atmosphere. The
combination of high CH4 conversion, high and tunable
selectivity, and durability in the H2 permeable membrane
reactor is notable.
In summary, the integration of a mixed ionic–electronic
H2 permeable SrCe0.7Zr0.2Eu0.1O3Àd membrane and FeꢀSiO2
catalyst into a catalytic tubular membrane reactor was
demonstrated for the first time for NMC reaction. The
removal of H2 from NMC reactions led to a significant
increase in CH4 conversion. The product selectivity to C2 and
aromatics as well as catalyst durability were not influenced
significantly by the H2 removal, which is distinctly different
from all the previous studies[6e,8a] on H2 permeable membrane
reactor for NMC reactions. The present work is the first
successful demonstration of the H2 permeable ceramic
membrane reactor on shifting reaction equilibrium to benefit
CH4 conversion while not impacting product selectivity and
catalyst durability in NMC reactions. The capability of tuning
products towards C2 (ethylene and acetylene) or aromatic
(benzene and naphthalene) products with high single-pass
yields open up new possibilities for NMC processes. The
integration of FeꢀSiO2 catalyst in the high temperature H2
permeable SrCe0.7Zr0.2Eu0.1O3Àd tubular membrane reactor
enables new routes for transformation of CH4 into high value-
added chemicals and fuels.
Experimental Section
The H2 permeable membrane reactor was prepared by tape
casting of the SrCe0.8Zr0.2O3 slurry and rolling end-capped tubular-
type supports, and then followed by colloidal coating of a thin dense
SrCe0.7Zr0.2Eu0.1O3Àd layer on the supports. Details on the synthesis of
the membrane materials and the fabrication of the membrane reactor
are described in previous reports[11a,d,13] and in the Supporting
Information. Fe2SiO4 was firstly prepared via the sol–gel method
published by DeAngelis et al.[14] FeꢀSiO2 was synthesized by fusing
Fe2SiO4 and SiO2 at 1973 K for 6 hours in air. The tests for leakage, H2
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were described in details in the Supporting Information.
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Acknowledgements
We acknowledge support from the National Science Founda-
tion (NSF-CBET 1264599 and 1351384), Maryland Nano-
Center and its NispLab. The NispLab is supported in part by
the NSF as a MRSEC Shared Experimental Facility. M.S. and
Y.W. thank the Harry K. Wells and Hulka Energy Research
Fellowships, respectively, from University of Maryland
Energy Research Center (UMERC) for the support of their
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Keywords: FeꢀSiO2 · membrane reactor · natural gas ·
non-oxidative methane conversion · SrCe0.7Zr0.2Eu0.1O3Àd
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Manuscript received: October 12, 2016
Final Article published: && &&, &&&&
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Communications
Heterogeneous Catalysis
M. Sakbodin, Y. Wu, S. C. Oh,
E. D. Wachsman,*
D. Liu*
&&&& — &&&&
Hydrogen-Permeable Tubular Membrane
Reactor: Promoting Conversion and
Product Selectivity for Non-Oxidative
Activation of Methane over an FeꢀSiO2
Catalyst
Adding value to natural gas: A hydrogen-
permeable tubular ceramic membrane
reactor was developed enabling
FeꢀSiO2-catalyzed CH4 upgrading to
higher hydrocarbons. The FeꢀSiO2 cata-
lyst demonstrated a stable 30% C2+
single-pass yield, with up to 30% CH4
conversion and 99% selectivity to C2 and
aromatic products.
Angew. Chem. Int. Ed. 2016, 55, 1 – 5
ꢀ 2016 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
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