Specific construction of asymmetric carbon-nickel-chlorine single-atom sites via carbon vacancy engineering for efficient CO2 electroreduction

Qi Hao, Qi Tang, Lirong Zheng, Kai Liu (), Junxiu Wu () and Jun Lu ()
Additional contact information
Qi Hao: Zhejiang University
Qi Tang: Changchun
Lirong Zheng: Chinese Academy of Sciences
Kai Liu: Westlake University
Junxiu Wu: Zhejiang University
Jun Lu: Zhejiang University

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Breaking the structural symmetry of active sites in single-atom catalysts (SACs) allows efficient regulation of the electron distribution around the metal centers, holding great promise for promoting their performance in electrocatalytic carbon dioxide reduction reaction (ECO2RR). Herein, we propose a vacancy-engineering strategy for constructing asymmetric carbon-nickel-chlorine (C–Ni–Cl) sites in Ni SAC (Ni1-C/Cl). In strongly acidic media (pH=1), Ni1-C/Cl achieves Faradaic efficiency over 98% for carbon monoxide (CO) product at the operated current density of 500 mA cm−2. In situ X-ray absorption spectra reveal that during electrocatalysis, the C3–Ni–Cl sites exhibit potential-dependent structure evolutions, which can optimize their adsorption configurations for the reactive species. Theoretical calculations demonstrate that the Ni–C/Ni–Cl co-coordination induces the asymmetric electron distribution in C3–Ni–Cl sites, resulting in the regulation of the electronic properties of the Ni centers, thereby optimizing the reaction pathway of CO2-to-CO on these single-atom sites. This work extends the synthesis of SACs containing asymmetric single-atom sites, provides insights into designing industrial-oriented electrocatalysts toward other important electrocatalytic reactions.

Date: 2025
References: Add references at CitEc
Citations:

Downloads: (external link)
https://www.nature.com/articles/s41467-025-62287-8 Abstract (text/html)

Related works:
This item may be available elsewhere in EconPapers: Search for items with the same title.

Export reference: BibTeX RIS (EndNote, ProCite, RefMan) HTML/Text

Persistent link: https://EconPapers.repec.org/RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-62287-8

Ordering information: This journal article can be ordered from
https://www.nature.com/ncomms/

DOI: 10.1038/s41467-025-62287-8

Access Statistics for this article

Nature Communications is currently edited by Nathalie Le Bot, Enda Bergin and Fiona Gillespie

More articles in Nature Communications from Nature
Bibliographic data for series maintained by Sonal Shukla () and Springer Nature Abstracting and Indexing ().