A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions

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-efficienc...

Full description

Saved in:
Bibliographic Details
Main Authors: Lv, Chade, Lee, Carmen, Zhong, Lixiang, Liu, Hengjie, Liu, Jiawei, Yang, Lan, Yan, Chunshuang, Yu, Wei, Hng, Huey Hoon, Qi, Zeming, Song, Li, Li, Shuzhou, Loh, Kian Ping, Yan, Qingyu, Yu, Guihua
Other Authors: School of Materials Science and Engineering
Format: Article
Language:English
Published: 2022
Subjects:
Online Access:https://hdl.handle.net/10356/161873
Tags: Add Tag
No Tags, Be the first to tag this record!
Institution: Nanyang Technological University
Language: English
id sg-ntu-dr.10356-161873
record_format dspace
spelling sg-ntu-dr.10356-1618732022-09-22T07:17:31Z A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions Lv, Chade Lee, Carmen Zhong, Lixiang Liu, Hengjie Liu, Jiawei Yang, Lan Yan, Chunshuang Yu, Wei Hng, Huey Hoon Qi, Zeming Song, Li Li, Shuzhou Loh, Kian Ping Yan, Qingyu Yu, Guihua School of Materials Science and Engineering Engineering::Materials Electrocatalysis C−N Coupling 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. Agency for Science, Technology and Research (A*STAR) Ministry of Education (MOE) 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 TeacherScholar 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). 2022-09-22T07:17:30Z 2022-09-22T07:17:30Z 2022 Journal Article Lv, C., Lee, C., Zhong, L., Liu, H., Liu, J., Yang, L., Yan, C., Yu, W., Hng, H. H., Qi, Z., Song, L., Li, S., Loh, K. P., Yan, Q. & Yu, G. (2022). A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions. ACS Nano, 16(5), 8213-8222. https://dx.doi.org/10.1021/acsnano.2c01956 1936-0851 https://hdl.handle.net/10356/161873 10.1021/acsnano.2c01956 35362943 2-s2.0-85128172229 5 16 8213 8222 en 2020-T1-001-031 A19D9a0096 ACS Nano © 2022 American Chemical Society. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Engineering::Materials
Electrocatalysis
C−N Coupling
spellingShingle Engineering::Materials
Electrocatalysis
C−N Coupling
Lv, Chade
Lee, Carmen
Zhong, Lixiang
Liu, Hengjie
Liu, Jiawei
Yang, Lan
Yan, Chunshuang
Yu, Wei
Hng, Huey Hoon
Qi, Zeming
Song, Li
Li, Shuzhou
Loh, Kian Ping
Yan, Qingyu
Yu, Guihua
A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions
description 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.
author2 School of Materials Science and Engineering
author_facet School of Materials Science and Engineering
Lv, Chade
Lee, Carmen
Zhong, Lixiang
Liu, Hengjie
Liu, Jiawei
Yang, Lan
Yan, Chunshuang
Yu, Wei
Hng, Huey Hoon
Qi, Zeming
Song, Li
Li, Shuzhou
Loh, Kian Ping
Yan, Qingyu
Yu, Guihua
format Article
author Lv, Chade
Lee, Carmen
Zhong, Lixiang
Liu, Hengjie
Liu, Jiawei
Yang, Lan
Yan, Chunshuang
Yu, Wei
Hng, Huey Hoon
Qi, Zeming
Song, Li
Li, Shuzhou
Loh, Kian Ping
Yan, Qingyu
Yu, Guihua
author_sort Lv, Chade
title A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions
title_short A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions
title_full A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions
title_fullStr A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions
title_full_unstemmed A defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions
title_sort defect engineered electrocatalyst that promotes high-efficiency urea synthesis under ambient conditions
publishDate 2022
url https://hdl.handle.net/10356/161873
_version_ 1745574618209452032