A Strongly Coupled Metal/Hydroxide Heterostructure Cascades Carbon Dioxide and Nitrate Reduction Reactions toward Efficient Urea Electrosynthesis.

Ye, W; Zhang, Y; Chen, L; Wu, F; Yao, Y; Wang, W; Zhu, G; Jia, G; Bai, Z; Dou, S; Gao, P; Wang, N; Wang, G

A Strongly Coupled Metal/Hydroxide Heterostructure Cascades Carbon Dioxide and Nitrate Reduction Reactions toward Efficient Urea Electrosynthesis.

Ye, W Zhang, Y Chen, L Wu, F Yao, Y Wang, W Zhu, G Jia, G Bai, Z Dou, S Gao, P Wang, N Wang, G

Permalink

Publisher:: Wiley
Publication Type:: Journal Article
Citation:: Angew Chem Int Ed Engl, 2024, 63, (48), pp. e202410105
Issue Date:: 2024-11-25

Open Access

Copyright Clearance Process

Recently Added
In Progress
Open Access

This item is open access.

Adobe PDF

Download Published versionAdobe PDF (1.71 MB)

View on publisher's site

View statistics

Full metadata record

Field	Value	Language
dc.contributor.author	Ye, W
dc.contributor.author	Zhang, Y
dc.contributor.author	Chen, L
dc.contributor.author	Wu, F
dc.contributor.author	Yao, Y
dc.contributor.author	Wang, W
dc.contributor.author	Zhu, G
dc.contributor.author	Jia, G
dc.contributor.author	Bai, Z
dc.contributor.author	Dou, S
dc.contributor.author	Gao, P
dc.contributor.author	Wang, N
dc.contributor.author	Wang, G https://orcid.org/0000-0003-4295-8578
dc.date.accessioned	2025-02-02T23:45:28Z
dc.date.available	2025-02-02T23:45:28Z
dc.date.issued	2024-11-25
dc.identifier.citation	Angew Chem Int Ed Engl, 2024, 63, (48), pp. e202410105
dc.identifier.issn	1433-7851
dc.identifier.issn	1521-3773
dc.identifier.uri	http://hdl.handle.net/10453/184803
dc.description.abstract	The direct coupling of nitrate ions and carbon dioxide for urea synthesis presents an appealing alternative to the Bosch-Meiser process in industry. The simultaneous activation of carbon dioxide and nitrate, however, as well as efficient C-N coupling on single active site, poses significant challenges. Here, we propose a novel metal/hydroxide heterostructure strategy based on synthesizing an Ag-CuNi(OH)2 composite to cascade carbon dioxide and nitrate reduction reactions for urea electrosynthesis. The strongly coupled metal/hydroxide heterostructure interface integrates two distinct sites for carbon dioxide and nitrate activation, and facilitates the coupling of CO (on silver, where denotes an active site) and *NH2 (on hydroxide) for urea formation. Moreover, the strongly coupled interface optimizes the water splitting process and facilitates the supply of active hydrogen atoms, thereby expediting the deoxyreduction processes essential for urea formation. Consequently, our Ag-CuNi(OH)2 composite delivers a high urea yield rate of 25.6 mmol gcat. -1 h-1 and high urea Faradaic efficiency of 46.1 %, as well as excellent cycling stability. This work provides new insights into the design of dual-site catalysts for C-N coupling, considering their role on the interface.
dc.format	Print-Electronic
dc.language	eng
dc.publisher	Wiley
dc.relation.ispartof	Angew Chem Int Ed Engl
dc.relation.isbasedon	10.1002/anie.202410105
dc.rights	info:eu-repo/semantics/openAccess
dc.subject	03 Chemical Sciences
dc.subject.classification	Organic Chemistry
dc.subject.classification	34 Chemical sciences
dc.title	A Strongly Coupled Metal/Hydroxide Heterostructure Cascades Carbon Dioxide and Nitrate Reduction Reactions toward Efficient Urea Electrosynthesis.
dc.type	Journal Article
utslib.citation.volume	63
utslib.location.activity	Germany
utslib.for	03 Chemical Sciences
pubs.organisational-group	University of Technology Sydney
pubs.organisational-group	University of Technology Sydney/Faculty of Science
pubs.organisational-group	University of Technology Sydney/Faculty of Science/School of Mathematical and Physical Sciences
pubs.organisational-group	University of Technology Sydney/UTS Groups
pubs.organisational-group	University of Technology Sydney/UTS Groups/Centre for Clean Energy Technology (CCET)
utslib.copyright.status	open_access	*
dc.rights.license	This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License (CC BY-NC-ND 4.0). To view a copy of this license, visit https://creativecommons.org/licenses/by-nc-nd/4.0/
dc.date.updated	2025-02-02T23:45:26Z
pubs.issue	48
pubs.publication-status	Published
pubs.volume	63
utslib.citation.issue	48

Abstract:

The direct coupling of nitrate ions and carbon dioxide for urea synthesis presents an appealing alternative to the Bosch-Meiser process in industry. The simultaneous activation of carbon dioxide and nitrate, however, as well as efficient C-N coupling on single active site, poses significant challenges. Here, we propose a novel metal/hydroxide heterostructure strategy based on synthesizing an Ag-CuNi(OH)2 composite to cascade carbon dioxide and nitrate reduction reactions for urea electrosynthesis. The strongly coupled metal/hydroxide heterostructure interface integrates two distinct sites for carbon dioxide and nitrate activation, and facilitates the coupling of *CO (on silver, where * denotes an active site) and *NH2 (on hydroxide) for urea formation. Moreover, the strongly coupled interface optimizes the water splitting process and facilitates the supply of active hydrogen atoms, thereby expediting the deoxyreduction processes essential for urea formation. Consequently, our Ag-CuNi(OH)2 composite delivers a high urea yield rate of 25.6 mmol gcat. -1 h-1 and high urea Faradaic efficiency of 46.1 %, as well as excellent cycling stability. This work provides new insights into the design of dual-site catalysts for C-N coupling, considering their role on the interface.

Please use this identifier to cite or link to this item:

http://hdl.handle.net/10453/184803