Dynamic active sites on plasma engraved Ni hydroxide for enhanced electro-catalytic urea oxidation

被引：34

作者：

Li, Dan ^{[1
,2
]}

Zhang, Yuefeng ^{[1
,2
]}

Zhou, Xiaomin ^{[1
,2
]}

Huang, Chao ^{[1
,2
]}

Wen, Ying ^{[3
]}

Liu, Liangliang ^{[1
,2
]}

Li, Qingwei ^{[1
,2
]}

Xu, Yue ^{[1
,2
]}

Wu, Yuzheng ^{[1
,2
]}

Ruan, Qingdong ^{[1
,2
]}

Ma, Yinghe ^{[1
,2
]}

Xiong, Fangyu ^{[1
,2
]}

Xiao, Dezhi ^{[1
,2
]}

Liu, Pei ^{[1
,2
]}

Wang, Guomin ^{[1
,2
]}

Mehrjou, Babak ^{[1
,2
]}

Wang, Bin ^{[1
,2
]}

Li, Hao ^{[4
]}

Chen, Rongsheng ^{[3
]}

Ni, Hongwei ^{[3
]}

Zeng, Zhiyuan ^{[1
,2
]}

Chu, Paul K. ^{[1
,2
]}

机构：

[1] City Univ Hong Kong, Dept Phys, Dept Mat Sci & Engn, Kowloon, Tat Chee Ave, Hong Kong 999077, Peoples R China

[2] City Univ Hong Kong, Dept Biomed Engn, Kowloon, Tat Chee Ave, Hong Kong 999077, Peoples R China

[3] Wuhan Univ Sci & Technol, State Key Lab Refractories & Met, Wuhan 430081, Hubei, Peoples R China

[4] Tech Univ Denmark, Catalysis Theory Ctr, Dept Phys, DK-2800 Lyngby, Denmark

来源：

JOURNAL OF ENERGY CHEMISTRY | 2022年 / 71卷

基金：

中国国家自然科学基金;

关键词：

Urea oxidization reaction; Ni hydroxide; Plasma processing; Dehydrogenation; Active site; NITROGEN-CYCLE; RAMAN; MECHANISM; ELECTROOXIDATION; SPECTROSCOPY; PHASES; FILMS;

D O I：

10.1016/j.jechem.2022.03.040

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

The urea oxidization reaction (UOR) is an important anodic reaction in electro-catalytic energy conversion. However, the sluggish reaction kinetics and complex catalyst transformation in electrocatalysis require activity improvement and better mechanistic understanding of the state-of-the-art Ni(OH)(2) catalyst. Herein, by utilizing low-temperature argon (Ar) plasma processing, tooth-wheel Ni(OH)(2) nanosheets self-supported on Ni foam (Ni(OH)(2)-Ar) are demonstrated to have improved UOR activity compared to conventional Ni(OH)(2). The theoretical assessment confirms that the edge has a smaller cation vacancy formation energy than the basal plane, consequently explaining the structural formation. Operando and quasi-operando methods are employed to investigate the dynamic evolution of the Ni(OH)(2) film in UOR. The crucial dehydrogenation products of Ni(OH)(5)O- intermediates are identified to be stable on the etched edge and explain the enhanced UOR in the low potential region. In addition, the dynamic active sites are monitored to elucidate the reaction mechanism in different potential ranges. (C) 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by ELSEVIER B.V. and Science Press. All rights reserved.

引用

页码：150 / 158

页数：9

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