Co-infiltration and dynamic formation of Pd3ZnCx intermetallic carbide by syngas boosting selective hydrogenation of acetylene

Huan Chen, Lulu Li, Zhi-Jian Zhao, Bing Yang (), Yafeng Zhang, Xiaoyan Liu, Qingqing Gu, Zhounan Yu, Xiaofeng Yang, Jinlong Gong (), Aiqin Wang () and Tao Zhang ()
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Huan Chen: Dalian University of Technology
Lulu Li: Tianjin University
Zhi-Jian Zhao: Tianjin University
Bing Yang: Chinese Academy of Sciences
Yafeng Zhang: Chinese Academy of Sciences
Xiaoyan Liu: Chinese Academy of Sciences
Qingqing Gu: Chinese Academy of Sciences
Zhounan Yu: Chinese Academy of Sciences
Xiaofeng Yang: Chinese Academy of Sciences
Jinlong Gong: Tianjin University
Aiqin Wang: Chinese Academy of Sciences
Tao Zhang: Dalian University of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Transition metal carbide shows excellent performance in selective hydrogenation of acetylene, however, the carburization of Pd-based intermetallic compounds remains infeasible. Here we report the successful synthesis of an unprecedented Pd3ZnCx intermetallic carbide, via co-infiltration of zinc and carbon in one-step carburization by syngas. Utilizing state-of-the-art in situ characterizations and theoretical calculation, we unveil the dynamic evolution of Pd3ZnCx during carburization, forming a Pd3Zn like cubic phase carbide structure. A unique transitional state (Pdt) with low content of Zn/C co-infiltration is clearly identified facilitating phase transition and sustain incorporation of carbon and zinc at elevated temperatures. The Pd3ZnCx carbide shows by far the best catalytic performance in the selective hydrogenation of acetylene with a high selectivity (>90%) even at a high H2/C2H2 ratio. Our results therefore provide a co-infiltration strategy and dynamic insights for the one-step synthesis of Pd based intermetallic carbides, towards high-performance intermetallic compound for selective hydrogenation of acetylene.

Date: 2024
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DOI: 10.1038/s41467-024-54274-2

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