Direct conversion of methane to aromatics and hydrogen via a heterogeneous trimetallic synergistic catalyst

Pengxi Zhu, Wenjuan Bian, Bin Liu, Hao Deng, Lucun Wang, Xiaozhou Huang, Stephanie L. Spence, Feng Lin, Chuancheng Duan, Dong Ding (), Pei Dong () and Hanping Ding ()
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Pengxi Zhu: Idaho National Laboratory
Wenjuan Bian: Idaho National Laboratory
Bin Liu: Idaho National Laboratory
Hao Deng: Idaho National Laboratory
Lucun Wang: Idaho National Laboratory
Xiaozhou Huang: George Mason University
Stephanie L. Spence: Virginia Tech
Feng Lin: Virginia Tech
Chuancheng Duan: Kansas State University
Dong Ding: Idaho National Laboratory
Pei Dong: George Mason University
Hanping Ding: Idaho National Laboratory

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract 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 CH3* from Mo2C on the external surface of zeolite can efficiently move on for C-C coupling on the surface of Pt-Bi particle to produce C2 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.

Date: 2024
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DOI: 10.1038/s41467-024-47595-9

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