Balancing elementary steps enables coke-free dry reforming of methane

Jiaqi Yu, Tien Le, Dapeng Jing, Eli Stavitski, Nicholas Hunter, Kanika Lalit, Denis Leshchev, Daniel E. Resasco, Edward H. Sargent (), Bin Wang () and Wenyu Huang ()
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Jiaqi Yu: Iowa State University
Tien Le: University of Oklahoma
Dapeng Jing: Iowa State University
Eli Stavitski: Brookhaven National Laboratory
Nicholas Hunter: Iowa State University
Kanika Lalit: Iowa State University
Denis Leshchev: Brookhaven National Laboratory
Daniel E. Resasco: University of Oklahoma
Edward H. Sargent: Northwestern University
Bin Wang: University of Oklahoma
Wenyu Huang: Iowa State University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Balancing kinetics, a crucial priority in catalysis, is frequently achieved by sacrificing activity of elementary steps to suppress side reactions and enhance catalyst stability. Dry reforming of methane (DRM), a process operated at high temperature, usually involves fast C-H activation but sluggish carbon removal, resulting in coke deposition and catalyst deactivation. Studies focused solely on catalyst innovation are insufficient in addressing coke formation efficiently. Herein, we develop coke-free catalysts that balance kinetics of elementary steps for overall thermodynamics optimization. Beginning from a highly active cobalt aluminum oxide (CoAl2O4) catalyst that is susceptible to severe coke formation, we substitute aluminum (Al) with gallium (Ga), reporting a CoAl0.5Ga1.5O4-R catalyst that performs DRM stably over 1000 hours without observable coke deposition. We find that Ga enhances DRM stability by suppressing C-H activation to balance carbon removal. A series of coke-free DRM catalysts are developed herein by partially substituting Al from CoAl2O4 with other metals.

Date: 2023
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DOI: 10.1038/s41467-023-43277-0

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