Wang, X;
Niu, H;
Wan, X;
Wang, A;
Wang, FR;
Guo, Y;
(2022)
Impact of Coordination Environment on Single-Atom-Embedded C3N for Oxygen Electrocatalysis.
ACS Sustainable Chemistry and Engineering
, 10
(23)
pp. 7692-7701.
10.1021/acssuschemeng.2c01648.
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Abstract
Herein, utilizing density functional theory (DFT) calculations, we have assessed the feasibility of single-atom-embedded C3N with various coordination environments of TM-C3, TM-C2N1, TM-C4, and TM-C2N2 for oxygen electrocatalysis. It has been proved that most TM-CxNy candidates are stable and all of them possess metallic features to ensure fast electron transfer. Importantly, Co-C2N2 is a bifunctional noble-free single-atom catalyst with low OER/ORR overpotentials (0.33/0.39 V). Furthermore, the impact of the coordination environment on the adsorption trend is revealed by the electronic properties of TM-CxNy. Considering that TM-d electron counts are multiplied by the sum of TM and C/N electronegativity, we propose a universal descriptor and offer more understanding of the coordination-activity correlation. Our findings not only show promising single-atom-embedded C3N candidates for oxygen electrocatalysis but also deeply unveil the impact of the coordination environment on catalytic activity.
| Type: | Article |
|---|---|
| Title: | Impact of Coordination Environment on Single-Atom-Embedded C3N for Oxygen Electrocatalysis |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acssuschemeng.2c01648 |
| Publisher version: | https://doi.org/10.1021/acssuschemeng.2c01648 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Science & Technology, Physical Sciences, Technology, Chemistry, Multidisciplinary, Green & Sustainable Science & Technology, Engineering, Chemical, Chemistry, Science & Technology - Other Topics, Engineering, first-principles calculations, single -atom catalysts, coordination environment, oxygen electrocatalysis, descriptor, EVOLUTION REACTION, REDUCTION REACTION, HYDROGEN, METAL, CATALYSTS, MONOLAYERS, NANOPARTICLES, ADSORPTION, CHALLENGES, PRINCIPLE |
| UCL classification: | UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering UCL > Provost and Vice Provost Offices > UCL BEAMS UCL |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10153448 |
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