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

Dan Li; Yuefeng Zhang; Xiaomin Zhou; Chao Huang; Ying Wen; Liangliang Liu; Qingwei Li; Yue Xu; Yuzheng Wu; Qingdong Ruan; Yinghe Ma; Fangyu Xiong; Dezhi Xiao; Pei Liu; Guomin Wang; Babak Mehrjou; Bin Wang; Hao Li; Rongsheng Chen; Hongwei Ni; Zhiyuan Zeng; Paul K. Chu

doi:10.1016/j.jechem.2022.03.040

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

Dan Li, Yuefeng Zhang, Xiaomin Zhou, Chao Huang, Ying Wen, Liangliang Liu, Qingwei Li, Yue Xu, Yuzheng Wu, Qingdong Ruan, Yinghe Ma, Fangyu Xiong, Dezhi Xiao, Pei Liu, Guomin Wang, Babak Mehrjou, Bin Wang, Hao Li, Rongsheng Chen, Hongwei NiZhiyuan Zeng, Paul K. Chu

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

3 Citations (Scopus)

Abstract

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)₅O^- 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.

Original language	English
Pages (from-to)	150-158
Number of pages	9
Journal	Journal of Energy Chemistry
Volume	71
DOIs	https://doi.org/10.1016/j.jechem.2022.03.040
Publication status	Published - 2022 Aug
Externally published	Yes

Keywords

Active site
Dehydrogenation
Ni hydroxide
Plasma processing
Urea oxidization reaction

ASJC Scopus subject areas

Fuel Technology
Energy Engineering and Power Technology
Energy (miscellaneous)
Electrochemistry

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10.1016/j.jechem.2022.03.040

Cite this

Li, D., Zhang, Y., Zhou, X., Huang, C., Wen, Y., Liu, L., Li, Q., Xu, Y., Wu, Y., Ruan, Q., Ma, Y., Xiong, F., Xiao, D., Liu, P., Wang, G., Mehrjou, B., Wang, B., Li, H., Chen, R., ... Chu, P. K. (2022). Dynamic active sites on plasma engraved Ni hydroxide for enhanced electro-catalytic urea oxidation. Journal of Energy Chemistry, 71, 150-158. https://doi.org/10.1016/j.jechem.2022.03.040

Li, D, Zhang, Y, Zhou, X, Huang, C, Wen, Y, Liu, L, Li, Q, Xu, Y, Wu, Y, Ruan, Q, Ma, Y, Xiong, F, Xiao, D, Liu, P, Wang, G, Mehrjou, B, Wang, B, Li, H, Chen, R, Ni, H, Zeng, Z & Chu, PK 2022, 'Dynamic active sites on plasma engraved Ni hydroxide for enhanced electro-catalytic urea oxidation', Journal of Energy Chemistry, vol. 71, pp. 150-158. https://doi.org/10.1016/j.jechem.2022.03.040

@article{79449fdd92ea425db11c583d1697728a,

title = "Dynamic active sites on plasma engraved Ni hydroxide for enhanced electro-catalytic urea oxidation",

abstract = "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)5O- 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.",

keywords = "Active site, Dehydrogenation, Ni hydroxide, Plasma processing, Urea oxidization reaction",

author = "Dan Li and Yuefeng Zhang and Xiaomin Zhou and Chao Huang and Ying Wen and Liangliang Liu and Qingwei Li and Yue Xu and Yuzheng Wu and Qingdong Ruan and Yinghe Ma and Fangyu Xiong and Dezhi Xiao and Pei Liu and Guomin Wang and Babak Mehrjou and Bin Wang and Hao Li and Rongsheng Chen and Hongwei Ni and Zhiyuan Zeng and Chu, {Paul K.}",

note = "Funding Information: The authors acknowledge the financial support from City University of Hong Kong Strategic Research Grant (SRG) ( 7005505 ) and the National Natural Science Foundation of China ( 51601136 and 51604202 ). The authors would also thank Shiyanjia Lab (www.shiyanjia.com) for the TEM analysis. Publisher Copyright: {\textcopyright} 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences",

year = "2022",

month = aug,

doi = "10.1016/j.jechem.2022.03.040",

language = "English",

volume = "71",

pages = "150--158",

journal = "Journal of Energy Chemistry",

issn = "2095-4956",

publisher = "Elsevier BV",

}

TY - JOUR

T1 - Dynamic active sites on plasma engraved Ni hydroxide for enhanced electro-catalytic urea oxidation

AU - Li, Dan

AU - Zhang, Yuefeng

AU - Zhou, Xiaomin

AU - Huang, Chao

AU - Wen, Ying

AU - Liu, Liangliang

AU - Li, Qingwei

AU - Xu, Yue

AU - Wu, Yuzheng

AU - Ruan, Qingdong

AU - Ma, Yinghe

AU - Xiong, Fangyu

AU - Xiao, Dezhi

AU - Liu, Pei

AU - Wang, Guomin

AU - Mehrjou, Babak

AU - Wang, Bin

AU - Li, Hao

AU - Chen, Rongsheng

AU - Ni, Hongwei

AU - Zeng, Zhiyuan

AU - Chu, Paul K.

N1 - Funding Information: The authors acknowledge the financial support from City University of Hong Kong Strategic Research Grant (SRG) ( 7005505 ) and the National Natural Science Foundation of China ( 51601136 and 51604202 ). The authors would also thank Shiyanjia Lab (www.shiyanjia.com) for the TEM analysis. Publisher Copyright: © 2022 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences

PY - 2022/8

Y1 - 2022/8

N2 - 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)5O- 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.

AB - 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)5O- 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.

KW - Active site

KW - Dehydrogenation

KW - Ni hydroxide

KW - Plasma processing

KW - Urea oxidization reaction

UR - http://www.scopus.com/inward/record.url?scp=85129534911&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=85129534911&partnerID=8YFLogxK

U2 - 10.1016/j.jechem.2022.03.040

DO - 10.1016/j.jechem.2022.03.040

M3 - Article

AN - SCOPUS:85129534911

SN - 2095-4956

VL - 71

SP - 150

EP - 158

JO - Journal of Energy Chemistry

JF - Journal of Energy Chemistry

ER -

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

Abstract

Keywords

ASJC Scopus subject areas

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