Reversing sintering effect of Ni particles on γ-Mo2N via strong metal support interaction

Lili Lin, Jinjia Liu, Xi Liu (), Zirui Gao, Ning Rui, Siyu Yao, Feng Zhang, Maolin Wang, Chang Liu, Lili Han, Feng Yang, Sen Zhang, Xiao-dong Wen, Sanjaya D. Senanayake, Yichao Wu, Xiaonian Li, José A. Rodriguez () and Ding Ma ()
Additional contact information
Lili Lin: Zhejiang University of Technology
Jinjia Liu: Chinese Academy of Sciences
Xi Liu: Shanghai Jiao Tong University
Zirui Gao: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University
Ning Rui: Brookhaven National Laboratory
Siyu Yao: Zhejiang University
Feng Zhang: State University of New York
Maolin Wang: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University
Chang Liu: University of Virginia
Lili Han: Brookhaven National Laboratory
Feng Yang: Southern University of Science and Technology
Sen Zhang: University of Virginia
Xiao-dong Wen: Chinese Academy of Sciences
Sanjaya D. Senanayake: Brookhaven National Laboratory
Yichao Wu: Zhejiang University of Technology
Xiaonian Li: Zhejiang University of Technology
José A. Rodriguez: Brookhaven National Laboratory
Ding Ma: College of Chemistry and Molecular Engineering and College of Engineering and BIC-ESAT Peking University

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: Abstract Reversing the thermal induced sintering phenomenon and forming high temperature stable fine dispersed metallic centers with unique structural and electronic properties is one of the ever-lasting targets of heterogeneous catalysis. Here we report that the dispersion of metallic Ni particles into under-coordinated two-dimensional Ni clusters over γ-Mo2N is a thermodynamically favorable process based on the AIMD simulation. A Ni-4nm/γ-Mo2N model catalyst is synthesized and used to further study the reverse sintering effect by the combination of multiple in-situ characterization methods, including in-situ quick XANES and EXAFS, ambient pressure XPS and environmental SE/STEM etc. The under-coordinated two-dimensional layered Ni clusters on molybdenum nitride support generated from the Ni-4nm/γ-Mo2N has been demonstrated to be a thermally stable catalyst in 50 h stability test in CO2 hydrogenation, and exhibits a remarkable catalytic selectivity reverse compared with traditional Ni particles-based catalyst, leading to a chemo-specific CO2 hydrogenation to CO.

Date: 2021
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DOI: 10.1038/s41467-021-27116-8

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