Boosting electrocatalytic nitrate-to-ammonia conversion via plasma enhanced CuCo alloy-substrate interaction

Angjian Wu; Yimeng Zhou; Jiabao Lv; Delong Zhang; Yaqi Peng; Qiulin Ye; Pengcheng Fu; Weitao Wang; Xiaoqing Lin; Shaojun Liu; Mengxia Xu; Zhifu Qi; Songqiang Zhu; Wei Zhu; Jianhua Yan; Xin Tu; Xiaodong Li

doi:10.1021/acssuschemeng.2c04249

Boosting electrocatalytic nitrate-to-ammonia conversion via plasma enhanced CuCo alloy-substrate interaction

Angjian Wu, Yimeng Zhou, Jiabao Lv, Delong Zhang, Yaqi Peng, Qiulin Ye, Pengcheng Fu, Weitao Wang, Xiaoqing Lin, Shaojun Liu, Mengxia Xu, Zhifu Qi, Songqiang Zhu, Wei Zhu, Jianhua Yan, Xin Tu, Xiaodong Li

Department of Chemical and Environmental Engineering

Research output: Journal Publication › Article › peer-review

28 Citations (Scopus)

Abstract

Electrocatalytic conversion of widely distributed nitrate from industrial wastewater into value-added ammonia was proposed as an attractive and sustainable alternative to harvesting green ammonia. Herein, CuCo alloys were facilely synthesized for nitrate conversion, while nonthermal Ar-plasma was employed to enhance the adhesion strength between the electrocatalyst and substrate interface via regulating the surface hydrophobicity and roughness. Based on Ar-plasma treatment, a high ammonia yield rate (5129.29 μg cm-2 h-1) was achieved using Cu30Co70 electrocatalyst -0.47 V vs RHE, while nearly 100% of Faradaic efficiency was achieved using Cu50Co50 electrocatalyst at -0.27 V vs RHE (reversible hydrogen electrode). Validated by in situ spectroscopy and density functional theory calculations, the high activity of the CuCo alloy was derived from the regulation of Co to weaken the strong adsorption capacity of Cu and the shift of the d-band center to lower the energy barrier, while Ar-plasma modification promoted the formation of*NO to boost nitrate conversion.

Original language	English
Pages (from-to)	14539-14548
Number of pages	10
Journal	ACS Sustainable Chemistry and Engineering
Volume	10
Issue number	44
DOIs	https://doi.org/10.1021/acssuschemeng.2c04249
Publication status	Published - 7 Nov 2022

Keywords

ammonia synthesis
CuCo alloy electrocatalyst
DFT calculation
nitrate reduction
nonthermal plasma

ASJC Scopus subject areas

General Chemistry
Environmental Chemistry
General Chemical Engineering
Renewable Energy, Sustainability and the Environment

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acssuschemeng.2c04249

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Wu, A., Zhou, Y., Lv, J., Zhang, D., Peng, Y., Ye, Q., Fu, P., Wang, W., Lin, X., Liu, S., Xu, M., Qi, Z., Zhu, S., Zhu, W., Yan, J., Tu, X., & Li, X. (2022). Boosting electrocatalytic nitrate-to-ammonia conversion via plasma enhanced CuCo alloy-substrate interaction. ACS Sustainable Chemistry and Engineering, 10(44), 14539-14548. https://doi.org/10.1021/acssuschemeng.2c04249

@article{796b64dc896843ea8c48de82054dfa0d,

title = "Boosting electrocatalytic nitrate-to-ammonia conversion via plasma enhanced CuCo alloy-substrate interaction",

abstract = "Electrocatalytic conversion of widely distributed nitrate from industrial wastewater into value-added ammonia was proposed as an attractive and sustainable alternative to harvesting green ammonia. Herein, CuCo alloys were facilely synthesized for nitrate conversion, while nonthermal Ar-plasma was employed to enhance the adhesion strength between the electrocatalyst and substrate interface via regulating the surface hydrophobicity and roughness. Based on Ar-plasma treatment, a high ammonia yield rate (5129.29 μg cm-2 h-1) was achieved using Cu30Co70 electrocatalyst -0.47 V vs RHE, while nearly 100% of Faradaic efficiency was achieved using Cu50Co50 electrocatalyst at -0.27 V vs RHE (reversible hydrogen electrode). Validated by in situ spectroscopy and density functional theory calculations, the high activity of the CuCo alloy was derived from the regulation of Co to weaken the strong adsorption capacity of Cu and the shift of the d-band center to lower the energy barrier, while Ar-plasma modification promoted the formation of*NO to boost nitrate conversion.",

keywords = "ammonia synthesis, CuCo alloy electrocatalyst, DFT calculation, nitrate reduction, nonthermal plasma",

author = "Angjian Wu and Yimeng Zhou and Jiabao Lv and Delong Zhang and Yaqi Peng and Qiulin Ye and Pengcheng Fu and Weitao Wang and Xiaoqing Lin and Shaojun Liu and Mengxia Xu and Zhifu Qi and Songqiang Zhu and Wei Zhu and Jianhua Yan and Xin Tu and Xiaodong Li",

note = "Funding Information: This work is supported by the National Nature Science Foundation of China (51976191, 51806193), the Ecological civilization project, Zhejiang University, the Pioneer R&D Program of Zhejiang Province-China (2022C03040), and the Fundamental Research Funds for the Central Universities (226-2022-00091). Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

year = "2022",

month = nov,

day = "7",

doi = "10.1021/acssuschemeng.2c04249",

language = "English",

volume = "10",

pages = "14539--14548",

journal = "ACS Sustainable Chemistry and Engineering",

issn = "2168-0485",

publisher = "American Chemical Society",

number = "44",

}

Wu, A, Zhou, Y, Lv, J, Zhang, D, Peng, Y, Ye, Q, Fu, P, Wang, W, Lin, X, Liu, S, Xu, M, Qi, Z, Zhu, S, Zhu, W, Yan, J, Tu, X & Li, X 2022, 'Boosting electrocatalytic nitrate-to-ammonia conversion via plasma enhanced CuCo alloy-substrate interaction', ACS Sustainable Chemistry and Engineering, vol. 10, no. 44, pp. 14539-14548. https://doi.org/10.1021/acssuschemeng.2c04249

TY - JOUR

T1 - Boosting electrocatalytic nitrate-to-ammonia conversion via plasma enhanced CuCo alloy-substrate interaction

AU - Wu, Angjian

AU - Zhou, Yimeng

AU - Lv, Jiabao

AU - Zhang, Delong

AU - Peng, Yaqi

AU - Ye, Qiulin

AU - Fu, Pengcheng

AU - Wang, Weitao

AU - Lin, Xiaoqing

AU - Liu, Shaojun

AU - Xu, Mengxia

AU - Qi, Zhifu

AU - Zhu, Songqiang

AU - Zhu, Wei

AU - Yan, Jianhua

AU - Tu, Xin

AU - Li, Xiaodong

N1 - Funding Information: This work is supported by the National Nature Science Foundation of China (51976191, 51806193), the Ecological civilization project, Zhejiang University, the Pioneer R&D Program of Zhejiang Province-China (2022C03040), and the Fundamental Research Funds for the Central Universities (226-2022-00091). Publisher Copyright: © 2022 American Chemical Society.

PY - 2022/11/7

Y1 - 2022/11/7

N2 - Electrocatalytic conversion of widely distributed nitrate from industrial wastewater into value-added ammonia was proposed as an attractive and sustainable alternative to harvesting green ammonia. Herein, CuCo alloys were facilely synthesized for nitrate conversion, while nonthermal Ar-plasma was employed to enhance the adhesion strength between the electrocatalyst and substrate interface via regulating the surface hydrophobicity and roughness. Based on Ar-plasma treatment, a high ammonia yield rate (5129.29 μg cm-2 h-1) was achieved using Cu30Co70 electrocatalyst -0.47 V vs RHE, while nearly 100% of Faradaic efficiency was achieved using Cu50Co50 electrocatalyst at -0.27 V vs RHE (reversible hydrogen electrode). Validated by in situ spectroscopy and density functional theory calculations, the high activity of the CuCo alloy was derived from the regulation of Co to weaken the strong adsorption capacity of Cu and the shift of the d-band center to lower the energy barrier, while Ar-plasma modification promoted the formation of*NO to boost nitrate conversion.

AB - Electrocatalytic conversion of widely distributed nitrate from industrial wastewater into value-added ammonia was proposed as an attractive and sustainable alternative to harvesting green ammonia. Herein, CuCo alloys were facilely synthesized for nitrate conversion, while nonthermal Ar-plasma was employed to enhance the adhesion strength between the electrocatalyst and substrate interface via regulating the surface hydrophobicity and roughness. Based on Ar-plasma treatment, a high ammonia yield rate (5129.29 μg cm-2 h-1) was achieved using Cu30Co70 electrocatalyst -0.47 V vs RHE, while nearly 100% of Faradaic efficiency was achieved using Cu50Co50 electrocatalyst at -0.27 V vs RHE (reversible hydrogen electrode). Validated by in situ spectroscopy and density functional theory calculations, the high activity of the CuCo alloy was derived from the regulation of Co to weaken the strong adsorption capacity of Cu and the shift of the d-band center to lower the energy barrier, while Ar-plasma modification promoted the formation of*NO to boost nitrate conversion.

KW - ammonia synthesis

KW - CuCo alloy electrocatalyst

KW - DFT calculation

KW - nitrate reduction

KW - nonthermal plasma

UR - http://www.scopus.com/inward/record.url?scp=85140635753&partnerID=8YFLogxK

U2 - 10.1021/acssuschemeng.2c04249

DO - 10.1021/acssuschemeng.2c04249

M3 - Article

AN - SCOPUS:85140635753

SN - 2168-0485

VL - 10

SP - 14539

EP - 14548

JO - ACS Sustainable Chemistry and Engineering

JF - ACS Sustainable Chemistry and Engineering

IS - 44

ER -

Boosting electrocatalytic nitrate-to-ammonia conversion via plasma enhanced CuCo alloy-substrate interaction

Abstract

Keywords

ASJC Scopus subject areas

UN SDGs

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