Citation: Cui-mei ZHI, Rui-hong YANG, Chang-yu ZHOU, Gui-ru WANG, Jia-ying DING, Wen YANG. Unraveling the role of Ni₁₃ catalyst supported on ZrO₂ for CH₄ dehydrogenation: The d-band electron reservoir[J]. Journal of Fuel Chemistry and Technology, ;2022, 50(5): 601-610. doi: 10.1016/S1872-5813(21)60184-6 shu

Unraveling the role of Ni₁₃ catalyst supported on ZrO₂ for CH₄ dehydrogenation: The d-band electron reservoir

1.
College of Chemical and Biological Engineering, Shanxi Key Laboratory of High Value Utilization of Coal Gangue, Taiyuan University of Science and Technology, Taiyuan 030024, China
2.
Shanxi Health Vocational College, Taiyuan 030012, China
3.
Shanxi Key Laboratory of Metal Forming Theory and Technology, School of Material Science and Engineering, Taiyuan University of Science and Technology, Taiyuan 030024, China

Corresponding author: Chang-yu ZHOU, 201821060219@stu.tyust.edu.cn Wen YANG, yangwen@tyust.edu.cn
Received Date: 12 October 2021
Revised Date: 3 December 2021
Accepted Date: 3 December 2021
Available Online: 9 June 2022

Figures(7)

The activation of C−H bonds of CH₄ is a key step for the conversion of methane to chemical commodities. Loading Ni onto ZrO₂ is regarded as a relatively efficient way to harness the beneficial electronic property and the fine dispersion of the Ni catalyst for CH₄ dissociation. Herein we demonstrate the crucial role of Ni₁₃ catalyst supported on ZrO₂ for the dissociation of CH₄. The density functional theory (DFT) results show that the ZrO₂ supported Ni₁₃ stabilizes all species better and facilitates CH₄ activation. The stepwise dehydrogenations of CH₄ on Ni₁₃-ZrO₂(111) exhibits longer C−H bond lengths of ISs , lower E_a, and smaller displacements between the detaching H and the remaining CH_x fragment in TSs . In addition, they are also thermodynamically more feasible. However, without the ZrO₂ support on Ni₁₃, the opposite results are obtained. Consequently, the ZrO₂ modified Ni₁₃ is more superior to the original Ni₁₃ in CH₄ dehydrogenation. The electronic analysis combining DFT calculations confirmed that the larger overlap between C 2p and Ni 3d, and the electron transfer of Ni→C cause the weaker C 2p−H 1s hybridization. In addition, the reduction of electron transfer of H→C leads to a stronger interaction between Ni and C along with a weak C−H bond. Hence, the ZrO₂support serves as the d-band electron reservoir at Ni₁₃ and it is benefit to the activation of C−H bonds in CH₄ dehydrogenation.
- CH₄ dehydrogenation,
- Ni₁₃ catalyst,
- ZrO₂ support,
- d-band electron,
- electron transfer
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Unraveling the role of Ni13 catalyst supported on ZrO2 for CH4 dehydrogenation: The d-band electron reservoir

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Unraveling the role of Ni₁₃ catalyst supported on ZrO₂ for CH₄ dehydrogenation: The d-band electron reservoir