Citation: Wenjuan Yang, Junjun Li, Xiaoya Cui, Chenhuai Yang, Yiting Liu, Xianwei Zeng, Zhicheng Zhang, Qitao Zhang. Fine-tuning inverse metal-support interaction boosts electrochemical transformation of methanol into formaldehyde based on density functional theory[J]. Chinese Chemical Letters, ;2021, 32(8): 2489-2494. doi: 10.1016/j.cclet.2020.12.057 shu

Fine-tuning inverse metal-support interaction boosts electrochemical transformation of methanol into formaldehyde based on density functional theory

Wenjuan Yang ^{a, d} ,
Junjun Li ^b ,
Xiaoya Cui ^c ,
Chenhuai Yang ^b ,
Yiting Liu ^a ,
Xianwei Zeng ^e ,
Zhicheng Zhang ^b,, ,
Qitao Zhang ^a,,

a.
SZU-NUS Collaborative Innovation Centre for Optoelectronic Science & Technology, International Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology of Ministry of Education, Institute of Microscale Optoelectronics, Shenzhen University, Shenzhen 518060, China
b.
Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Department of Chemistry, School of Science, Tianjin University & Collaborative Innovation Centre of Chemical Science and Engineering, Tianjin 300072, China
c.
Centre for Programmable Materials, School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798, Singapore
d.
Hanshan Normal University, Chaozhou 521041, China
e.
ZheJiang Fenghong New Material Co., Ltd., Huzhou 313300, China

Corresponding author: Zhicheng Zhang, zczhang19@tju.edu.cn Qitao Zhang, qitao-zhang@szu.edu.cn
Received Date: 28 October 2020
Revised Date: 27 November 2020
Accepted Date: 29 December 2020
Available Online: 5 January 2021

Figures(4)

Different from traditional metal-support heterogenous catalysts, inverse heterogeneous catalysts, in which the surface of metal is decorated by metal oxide, have recently attracted increasing interests owing to the unique interfacial effect and electronic structure. However, a deep insight into the effect of metal-oxide interaction on the catalytic performance still remains a great challenge. In our work, an inverse hematite/palladium (Fe₂O₃/Pd) hybrid nanostructure, i.e., the active Fe₂O₃ ultrathin oxide layers partially covering on the surface of Pd nanoparticles (NPs), exhibited superior electrocatalytic performance towards methanol oxidation reaction (MOR) as compared to the bare Pd NPs based on density functional theory calculation. The charge could transfer from Pd to Fe₂O₃ driven by the built-in potential at the interface of Pd and Fe₂O₃, which favors the downshift of d band center of Pd. With the assistance of interfacial hydroxyl OH*, the cleavage of OH and CH in CH₃OH could take place much easily with lower barrier energy on Fe₂O₃/Pd than that on pure Pd via two electrons transferring reaction pathways. Our results highlight that the synergy of Pd and Fe₂O₃ at the interface could facilitate the electrochemical transformation of methanol into formaldehyde assisted with interfacial hydroxyl OH*.
- Inverse metal-support interaction,
- Heterostructure,
- Fe₂O₃/Pd,
- Electrochemical methanol oxidation,
- DFT
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