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Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst
by
Dong, Pei
, Liu, Bin
, Spence, Stephanie L.
, Deng, Hao
, Ding, Hanping
, Ding, Dong
, Bian, Wenjuan
, Huang, Xiaozhou
, Wang, Lucun
, Lin, Feng
, Duan, Chuancheng
, Zhu, Pengxi
in
03 NATURAL GAS
/ 119/118
/ 147/135
/ 147/137
/ 147/143
/ 30 DIRECT ENERGY CONVERSION
/ 639/166/898
/ 639/301/299
/ 639/4077/4082
/ Alloys
/ Aromatic compounds
/ aromatics
/ Benzene
/ Bimetals
/ Bismuth base alloys
/ Carbon
/ Catalysis
/ Catalysts
/ Catalytic activity
/ Clusters
/ Direct conversion
/ heterogeneous catalysis
/ Humanities and Social Sciences
/ hydorgen
/ Hydrocarbons
/ Hydrogen
/ Intermediates
/ Methane
/ methane conversion
/ Molybdenum
/ multidisciplinary
/ Natural gas
/ Oligomerization
/ Science
/ Science (multidisciplinary)
/ trimetallic catalyst
/ Zeolites
2024
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Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst
by
Dong, Pei
, Liu, Bin
, Spence, Stephanie L.
, Deng, Hao
, Ding, Hanping
, Ding, Dong
, Bian, Wenjuan
, Huang, Xiaozhou
, Wang, Lucun
, Lin, Feng
, Duan, Chuancheng
, Zhu, Pengxi
in
03 NATURAL GAS
/ 119/118
/ 147/135
/ 147/137
/ 147/143
/ 30 DIRECT ENERGY CONVERSION
/ 639/166/898
/ 639/301/299
/ 639/4077/4082
/ Alloys
/ Aromatic compounds
/ aromatics
/ Benzene
/ Bimetals
/ Bismuth base alloys
/ Carbon
/ Catalysis
/ Catalysts
/ Catalytic activity
/ Clusters
/ Direct conversion
/ heterogeneous catalysis
/ Humanities and Social Sciences
/ hydorgen
/ Hydrocarbons
/ Hydrogen
/ Intermediates
/ Methane
/ methane conversion
/ Molybdenum
/ multidisciplinary
/ Natural gas
/ Oligomerization
/ Science
/ Science (multidisciplinary)
/ trimetallic catalyst
/ Zeolites
2024
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Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst
by
Dong, Pei
, Liu, Bin
, Spence, Stephanie L.
, Deng, Hao
, Ding, Hanping
, Ding, Dong
, Bian, Wenjuan
, Huang, Xiaozhou
, Wang, Lucun
, Lin, Feng
, Duan, Chuancheng
, Zhu, Pengxi
in
03 NATURAL GAS
/ 119/118
/ 147/135
/ 147/137
/ 147/143
/ 30 DIRECT ENERGY CONVERSION
/ 639/166/898
/ 639/301/299
/ 639/4077/4082
/ Alloys
/ Aromatic compounds
/ aromatics
/ Benzene
/ Bimetals
/ Bismuth base alloys
/ Carbon
/ Catalysis
/ Catalysts
/ Catalytic activity
/ Clusters
/ Direct conversion
/ heterogeneous catalysis
/ Humanities and Social Sciences
/ hydorgen
/ Hydrocarbons
/ Hydrogen
/ Intermediates
/ Methane
/ methane conversion
/ Molybdenum
/ multidisciplinary
/ Natural gas
/ Oligomerization
/ Science
/ Science (multidisciplinary)
/ trimetallic catalyst
/ Zeolites
2024
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Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst
Journal Article
Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst
2024
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Overview
Non-oxidative methane dehydro-aromatization reaction can co-produce hydrogen and benzene effectively on a molybdenum-zeolite based thermochemical catalyst, which is a very promising approach for natural-gas upgrading. However, the low methane conversion and aromatics selectivity and weak durability restrain the realistic application for industry. Here, a mechanism for enhancing catalysis activity on methane activation and carbon-carbon bond coupling has been found to promote conversion and selectivity simultaneously by adding platinum–bismuth alloy cluster to form a trimetallic catalyst on zeolite (Pt-Bi/Mo/ZSM-5). This bimetallic alloy cluster has synergistic interaction with molybdenum: the formed CH
3
*
from Mo
2
C on the external surface of zeolite can efficiently move on for C-C coupling on the surface of Pt-Bi particle to produce C
2
compounds, which are the key intermediates of oligomerization. This pathway is parallel with the catalysis on Mo inside the cage. This catalyst demonstrated 18.7% methane conversion and 69.4% benzene selectivity at 710 °C. With 95% methane/5% nitrogen feedstock, it exhibited robust stability with slow deactivation rate of 9.3% after 2 h and instant recovery of 98.6% activity after regeneration in hydrogen. The enhanced catalytic activity is strongly associated with synergistic interaction with Mo and ligand effects of alloys by extensive mechanism studies and DFT calculation.
Converting methane to hydrogen and aromatics is a route to upgrading natural gas into high value products. Here the authors report a high-performing synergistic trimetallic thermochemical catalyst, along with mechanistic insights into the process.
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