A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

Chade Lv; Carmen Lee; Lixiang Zhong; Hengjie Liu; Jiawei Liu; Lan Yang; Chunshuang Yan; Wei Yu; Huey Hoon Hng; Zeming Qi; Li Song; Shuzhou Li; Kian Ping Loh; Qingyu Yan; Guihua Yu

doi:10.1021/acsnano.2c01956

A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

Chade Lv (Co-first Author)
, Carmen Lee (Co-first Author)
, Lixiang Zhong
, Hengjie Liu
, Jiawei Liu
, Lan Yang
, Chunshuang Yan^*
, Wei Yu
, Huey Hoon Hng
, Zeming Qi
, Li Song
, Shuzhou Li
, Kian Ping Loh
, Qingyu Yan^*
, Guihua Yu^*

^*Corresponding author for this work

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

301 Citations (Scopus)

Abstract

Synthesizing urea from nitrate and carbon dioxide through an electrocatalysis approach under ambient conditions is extraordinarily sustainable. However, this approach still lacks electrocatalysts developed with high catalytic efficiencies, which is a key challenge. Here, we report the high-efficiency electrocatalytic synthesis of urea using indium oxyhydroxide with oxygen vacancy defects, which enables selective C−N coupling toward standout electrocatalytic urea synthesis activity. Analysis by operando synchrotron radiation−Fourier transform infrared spectroscopy showcases that *CO₂NH₂ protonation is the potential-determining step for the overall urea formation process. As such, defect engineering is employed to lower the energy barrier for the protonation of the *CO₂NH₂ intermediate to accelerate urea synthesis. Consequently, the defect-engineered catalyst delivers a high Faradaic efficiency of 51.0%. In conjunction with an in-depth study on the catalytic mechanism, this design strategy may facilitate the exploration of advanced catalysts for electrochemical urea synthesis and other sustainable applications. © 2022 American Chemical Society.

Original language	English
Pages (from-to)	8213-8222
Number of pages	10
Journal	ACS Nano
Volume	16
Issue number	5
Online published	1 Apr 2022
DOIs	https://doi.org/10.1021/acsnano.2c01956
Publication status	Published - 24 May 2022
Externally published	Yes

Funding

C.Y. acknowledges funding supported by the National Natural Science Foundation of China (Grant 52101246) and the Fundamental Research Funds for the Central Universities (Grant 5710010721). Q.Y. acknowledges funding support from Singapore MOE AcRF Tier 1 Grant 2020-T1-001-031 and Singapore A*STAR project A19D9a0096. G.Y. acknowledges funding support from the Camille Dreyfus Teacher-Scholar Award and Welch Foundation Award F-1861. The authors acknowledge computing resources from the National Supercomputing Centre, Singapore. This work is also supported by the Users with Excellence program of Hefei Science Center of CAS (2020HSC-UE003) and the Fundamental Research Funds for the Central Universities (WK2310000099). We greatly thank the Facility for Analysis, Characterization, Testing and Simulation (FACTS) of Nanyang Technological University, Singapore, for the use of their TEM, SEM, and XRD equipment. We acknowledge NTU Center of High Field NMR Spectroscopy and Imaging. We also thank the National Synchrotron Radiation Laboratory for help with the characterizations.

Research Keywords

C−N coupling
defect engineering
electrocatalysis
indium oxyhydroxide
urea synthesis

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title = "A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions",

abstract = "Synthesizing urea from nitrate and carbon dioxide through an electrocatalysis approach under ambient conditions is extraordinarily sustainable. However, this approach still lacks electrocatalysts developed with high catalytic efficiencies, which is a key challenge. Here, we report the high-efficiency electrocatalytic synthesis of urea using indium oxyhydroxide with oxygen vacancy defects, which enables selective C−N coupling toward standout electrocatalytic urea synthesis activity. Analysis by operando synchrotron radiation−Fourier transform infrared spectroscopy showcases that *CO2NH2 protonation is the potential-determining step for the overall urea formation process. As such, defect engineering is employed to lower the energy barrier for the protonation of the *CO2NH2 intermediate to accelerate urea synthesis. Consequently, the defect-engineered catalyst delivers a high Faradaic efficiency of 51.0\%. In conjunction with an in-depth study on the catalytic mechanism, this design strategy may facilitate the exploration of advanced catalysts for electrochemical urea synthesis and other sustainable applications. {\textcopyright} 2022 American Chemical Society.",

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doi = "10.1021/acsnano.2c01956",

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T1 - A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

AU - Lv, Chade

AU - Lee, Carmen

AU - Zhong, Lixiang

AU - Liu, Hengjie

AU - Liu, Jiawei

AU - Yang, Lan

AU - Yan, Chunshuang

AU - Yu, Wei

AU - Hng, Huey Hoon

AU - Qi, Zeming

AU - Song, Li

AU - Li, Shuzhou

AU - Loh, Kian Ping

AU - Yan, Qingyu

AU - Yu, Guihua

PY - 2022/5/24

Y1 - 2022/5/24

N2 - Synthesizing urea from nitrate and carbon dioxide through an electrocatalysis approach under ambient conditions is extraordinarily sustainable. However, this approach still lacks electrocatalysts developed with high catalytic efficiencies, which is a key challenge. Here, we report the high-efficiency electrocatalytic synthesis of urea using indium oxyhydroxide with oxygen vacancy defects, which enables selective C−N coupling toward standout electrocatalytic urea synthesis activity. Analysis by operando synchrotron radiation−Fourier transform infrared spectroscopy showcases that *CO2NH2 protonation is the potential-determining step for the overall urea formation process. As such, defect engineering is employed to lower the energy barrier for the protonation of the *CO2NH2 intermediate to accelerate urea synthesis. Consequently, the defect-engineered catalyst delivers a high Faradaic efficiency of 51.0%. In conjunction with an in-depth study on the catalytic mechanism, this design strategy may facilitate the exploration of advanced catalysts for electrochemical urea synthesis and other sustainable applications. © 2022 American Chemical Society.

AB - Synthesizing urea from nitrate and carbon dioxide through an electrocatalysis approach under ambient conditions is extraordinarily sustainable. However, this approach still lacks electrocatalysts developed with high catalytic efficiencies, which is a key challenge. Here, we report the high-efficiency electrocatalytic synthesis of urea using indium oxyhydroxide with oxygen vacancy defects, which enables selective C−N coupling toward standout electrocatalytic urea synthesis activity. Analysis by operando synchrotron radiation−Fourier transform infrared spectroscopy showcases that *CO2NH2 protonation is the potential-determining step for the overall urea formation process. As such, defect engineering is employed to lower the energy barrier for the protonation of the *CO2NH2 intermediate to accelerate urea synthesis. Consequently, the defect-engineered catalyst delivers a high Faradaic efficiency of 51.0%. In conjunction with an in-depth study on the catalytic mechanism, this design strategy may facilitate the exploration of advanced catalysts for electrochemical urea synthesis and other sustainable applications. © 2022 American Chemical Society.

KW - C−N coupling

KW - defect engineering

KW - electrocatalysis

KW - indium oxyhydroxide

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A Defect Engineered Electrocatalyst that Promotes High-Efficiency Urea Synthesis under Ambient Conditions

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