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; Ding Ma

doi:10.1038/s41467-021-27116-8

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
, Ding Ma

Surface Chemistry & Catalysis Group

Research output: Contribution to journal › Article › peer-review

142 Scopus citations

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.

Original language	English
Article number	6978
Journal	Nature Communications
Volume	12
Issue number	1
DOIs	https://doi.org/10.1038/s41467-021-27116-8
State	Published - Dec 2021

Funding

This work was financially supported by the Natural Science Foundation of China (21725301 (D.M.), 21932002 (D.M.), 21821004 (D.M.), 21991153 (D.M.), 21872163 (X.L.), 22072090 (X.L.), and 22002140 (L.L.)) and the National Key R&D Program of China (2017YFB0602200 (D.M.) and 2021YFC2101800 (S.Y.)), and Zhejiang Provincial Natural Science Foundation of China under Grant (LR21B030001 (S.Y.)). The experiments of AP-XPS carried out at the Chemistry Department of Brookhaven National Laboratory (BNL) were supported by the division of Chemical Science, Geoscience, and Bioscience, Office of Basic Energy Science of the U.S. Department of Energy (DOE) under contract No. DE-SC0012704. Use of the Advanced Photon Source (beamlines 9-BM, for XAS characterization) was supported by the U.S. DOE under contract no. DE-AC02-06CH11357. Young Elite Scientist Sponsorship Program by CAST, NO. 2019QNRC001 is also acknowledged by L.L. We also appreciate technical supports from Mr. Hiroaki Matsumoto and Mr. Chaobin Zeng, Hitachi High-Technologies (Shanghai) Co. Ltd, for HR-STEM characterization.

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10.1038/s41467-021-27116-8

Cite this

Lin, L., Liu, J., Liu, X., Gao, Z., Rui, N., Yao, S., Zhang, F., Wang, M., Liu, C., Han, L., Yang, F., Zhang, S., Wen, X. D., Senanayake, S. D., Wu, Y., Li, X., Rodriguez, J. A., & Ma, D. (2021). Reversing sintering effect of Ni particles on γ-Mo₂N via strong metal support interaction. Nature Communications, 12(1), Article 6978. https://doi.org/10.1038/s41467-021-27116-8

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title = "Reversing sintering effect of Ni particles on γ-Mo2N via strong metal support interaction",

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.",

author = "Lili Lin and Jinjia Liu and Xi Liu and Zirui Gao and Ning Rui and Siyu Yao and Feng Zhang and Maolin Wang and Chang Liu and Lili Han and Feng Yang and Sen Zhang and Wen, \{Xiao dong\} and Senanayake, \{Sanjaya D.\} and Yichao Wu and Xiaonian Li and Rodriguez, \{Jos{\'e} A.\} and Ding Ma",

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AU - Yao, Siyu

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AU - Wang, Maolin

AU - Liu, Chang

AU - Han, Lili

AU - Yang, Feng

AU - Zhang, Sen

AU - Wen, Xiao dong

AU - Senanayake, Sanjaya D.

AU - Wu, Yichao

AU - Li, Xiaonian

AU - Rodriguez, José A.

AU - Ma, Ding

PY - 2021/12

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N2 - 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.

AB - 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.

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

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