Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

Yinuo Wang; Yian Wang; Qinglan Zhao; Hongming Xu; Shangqian Zhu; Fei Yang; Ernest P. Delmo; Xiaoyi Qiu; Chi Song; Juhee Jang; Tiehuai Li; Ping Gao; M. Danny Gu; Minhua Shao

doi:10.1016/j.jechem.2024.02.020

Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

Yinuo Wang, Yian Wang, Qinglan Zhao, Hongming Xu, Shangqian Zhu, Fei Yang, Ernest P. Delmo, Xiaoyi Qiu, Chi Song, Juhee Jang, Tiehuai Li, Ping Gao, M. Danny Gu, Minhua Shao^*

^*Corresponding author for this work

Department of Chemistry

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

10 Citations (Scopus)

Abstract

Urea generation through electrochemical CO₂ and NO₃⁻ co-reduction reaction (CO₂NO₃RR) is still limited by either the low selectivity or yield rate of urea. Herein, we report copper carbonate hydroxide (Cu₂(OH)₂CO₃) as an efficient CO₂NO₃RR electrocatalyst with an impressive urea Faradaic efficiency of 45.2% ± 2.1% and a high yield rate of 1564.5 ± 145.2 μg h⁻¹ mg_cat⁻¹. More importantly, H₂ evolution is fully inhibited on this electrocatalyst over a wide potential range between −0.3 and −0.8 V versus reversible hydrogen electrode. Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu₂(OH)₂CO₃ by combining the two intermediates, *COOH and *NHO. This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO₂NO₃RR, and provide guidance for rational design of more advanced catalysts. © 2024

Original language	English
Pages (from-to)	289-298
Journal	Journal of Energy Chemistry
Volume	93
Online published	27 Feb 2024
DOIs	https://doi.org/10.1016/j.jechem.2024.02.020
Publication status	Published - Jun 2024

Funding

This work was supported by the Research Grants Council (26206115, 16304821 and 16309418), the Southern Marine Science and Engineering Guangdong Laboratory (Guangzhou) (SMSEGL20SC01), and the Innovation and Technology Commission (grant no. ITC-CNERC14EG03) of the Hong Kong Special Administrative Region. Q.Z. and S.Z. acknowledge the Hong Kong Postdoctoral Fellowship Scheme (HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08). M.G. acknowledges the support from the Shenzhen fundamental research funding (JCYJ20210324115809026, 20200925154115001, JCYJ20200109141216566). The authors acknowledge N. Ho from HKUST for XPS measurements.

Research Keywords

C-N coupling
Co-reduction
Copper carbonate hydroxide
DFT calculation
Urea generation

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

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title = "Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts",

abstract = "Urea generation through electrochemical CO2 and NO3− co-reduction reaction (CO2NO3RR) is still limited by either the low selectivity or yield rate of urea. Herein, we report copper carbonate hydroxide (Cu2(OH)2CO3) as an efficient CO2NO3RR electrocatalyst with an impressive urea Faradaic efficiency of 45.2% ± 2.1% and a high yield rate of 1564.5 ± 145.2 μg h−1 mgcat−1. More importantly, H2 evolution is fully inhibited on this electrocatalyst over a wide potential range between −0.3 and −0.8 V versus reversible hydrogen electrode. Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu2(OH)2CO3 by combining the two intermediates, *COOH and *NHO. This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO2NO3RR, and provide guidance for rational design of more advanced catalysts. {\textcopyright} 2024",

keywords = "C-N coupling, Co-reduction, Copper carbonate hydroxide, DFT calculation, Urea generation",

author = "Yinuo Wang and Yian Wang and Qinglan Zhao and Hongming Xu and Shangqian Zhu and Fei Yang and Delmo, {Ernest P.} and Xiaoyi Qiu and Chi Song and Juhee Jang and Tiehuai Li and Ping Gao and {Danny Gu}, M. and Minhua Shao",

year = "2024",

month = jun,

doi = "10.1016/j.jechem.2024.02.020",

language = "English",

volume = "93",

pages = "289--298",

journal = "Journal of Energy Chemistry",

issn = "2095-4956",

publisher = "Elsevier B.V.",

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TY - JOUR

T1 - Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

AU - Wang, Yinuo

AU - Wang, Yian

AU - Zhao, Qinglan

AU - Xu, Hongming

AU - Zhu, Shangqian

AU - Yang, Fei

AU - Delmo, Ernest P.

AU - Qiu, Xiaoyi

AU - Song, Chi

AU - Jang, Juhee

AU - Li, Tiehuai

AU - Gao, Ping

AU - Danny Gu, M.

AU - Shao, Minhua

PY - 2024/6

Y1 - 2024/6

N2 - Urea generation through electrochemical CO2 and NO3− co-reduction reaction (CO2NO3RR) is still limited by either the low selectivity or yield rate of urea. Herein, we report copper carbonate hydroxide (Cu2(OH)2CO3) as an efficient CO2NO3RR electrocatalyst with an impressive urea Faradaic efficiency of 45.2% ± 2.1% and a high yield rate of 1564.5 ± 145.2 μg h−1 mgcat−1. More importantly, H2 evolution is fully inhibited on this electrocatalyst over a wide potential range between −0.3 and −0.8 V versus reversible hydrogen electrode. Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu2(OH)2CO3 by combining the two intermediates, *COOH and *NHO. This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO2NO3RR, and provide guidance for rational design of more advanced catalysts. © 2024

AB - Urea generation through electrochemical CO2 and NO3− co-reduction reaction (CO2NO3RR) is still limited by either the low selectivity or yield rate of urea. Herein, we report copper carbonate hydroxide (Cu2(OH)2CO3) as an efficient CO2NO3RR electrocatalyst with an impressive urea Faradaic efficiency of 45.2% ± 2.1% and a high yield rate of 1564.5 ± 145.2 μg h−1 mgcat−1. More importantly, H2 evolution is fully inhibited on this electrocatalyst over a wide potential range between −0.3 and −0.8 V versus reversible hydrogen electrode. Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu2(OH)2CO3 by combining the two intermediates, *COOH and *NHO. This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO2NO3RR, and provide guidance for rational design of more advanced catalysts. © 2024

KW - C-N coupling

KW - Co-reduction

KW - Copper carbonate hydroxide

KW - DFT calculation

KW - Urea generation

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U2 - 10.1016/j.jechem.2024.02.020

DO - 10.1016/j.jechem.2024.02.020

M3 - RGC 21 - Publication in refereed journal

SN - 2095-4956

VL - 93

SP - 289

EP - 298

JO - Journal of Energy Chemistry

JF - Journal of Energy Chemistry

ER -

Efficient C-N coupling in electrocatalytic urea generation on copper carbonate hydroxide electrocatalysts

Abstract

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Research Keywords

RGC Funding Information

UN SDGs

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