Bai, Z;
Jiang, XZ;
Luo, KH;
(2025)
Enhanced CO2 electrochemical reduction on single-atom catalysts with optimized environmental, central and axial chemical ambient.
Journal of Colloid and Interface Science
, 686
pp. 1188-1199.
10.1016/j.jcis.2025.02.015.
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Abstract
Single-atom catalysts (SACs) have received significant research interests for electrocatalytic CO2 reduction reaction (CO2RR) to produce valuable chemicals. Designing optimal SACs for CO2RR is a great challenge because of the strong scaling relationship among the many carbon-containing intermediates. In this study, we designed high-performance SACs, breaking the scaling relationship through changing environmental nonmetals, central atoms and axial nonmetals together via a series of density functional theory (DFT) calculations. After screening through configuration stabilities, CO and CO2 adsorption energy, limiting potential of H2, product adsorption energy, limiting potential of products, energy barrier of C–C coupling process and AIMD simulations, we finally observed ten optimal SACs (Ti-N4-B, Ti-N4-Si, Ti-CN3-Si, Ti-CN2O(1)-S, Sc-C2NO(1)-B, Sc-C2NO(1)-Si, Ti-BCN2(2)-N, Sc-CN2O(3)-Si, Ru-C2NO(3)-C and Ti-BONC-C) after considering 4311 possible configurations with high activity and selectivity for HCOOH, CH4 and C2H6O formation. Among them, Ti-N4-B, Ru-C2NO(3)-C, and Sc-C2NO(1)-B have the lowest overpotentials for producing HCOOH, CH4, and C2H6O with UL of −0.2 V, −0.29 V, and −0.51 V, respectively. Subsequently, electronic analysis is implemented to provide a more comprehensive explanation at the electronic level for the enhanced CO2RR performance of the discovered SACs. Our research demonstrates that the performance of SACs on CO2RR can be significantly enhanced and altered by the combination of environmental nonmetals, central atoms, and axial nonmetals in a rational design. Importantly, it also establishes a design principle for the rapid screening of prospective catalysts for CO2RR with high activity and selectivity.
| Type: | Article |
|---|---|
| Title: | Enhanced CO2 electrochemical reduction on single-atom catalysts with optimized environmental, central and axial chemical ambient |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1016/j.jcis.2025.02.015 |
| Publisher version: | https://doi.org/10.1016/j.jcis.2025.02.015 |
| Language: | English |
| Additional information: | © 2025 The Authors. Published by Elsevier Inc. under a Creative Commons license (http://creativecommons.org/licenses/by/4.0/). |
| Keywords: | Single atom catalysts, AIMD, Electrocatalytic CO2 reduction, Density functional theory, Coordination sphere |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Mechanical Engineering |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10205297 |
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