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 Ni^*

Zhiyuan Zeng^*, Paul K. Chu^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

48 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
Journal	Journal of Energy Chemistry
Volume	71
Online published	1 Apr 2022
DOIs	https://doi.org/10.1016/j.jechem.2022.03.040
Publication status	Published - Aug 2022

Research Keywords

Active site
Dehydrogenation
Ni hydroxide
Plasma processing
Urea oxidization reaction

Access Output

10.1016/j.jechem.2022.03.040

Other Access Options

Check CityUHK Library

Permanent Link

Right click to copy link

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

@article{88eaf6b1425749e7a0aeed07d5d2962a,

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.\}",

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 B.V.",

}

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

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.

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 - https://www.scopus.com/pages/publications/85129534911

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85129534911&origin=recordpage

U2 - 10.1016/j.jechem.2022.03.040

DO - 10.1016/j.jechem.2022.03.040

M3 - RGC 21 - Publication in refereed journal

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

Research Keywords

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Cite this