Theoretical Investigation of Single-, Double-, and Triple- p-block Metals Anchored on g-CN Monolayer for Oxygen Electrocatalysis

Yanan Zhou; Li Sheng; Lanlan Chen; Wenhua Zhang; Jinlong Yang

doi:10.1021/acs.jpclett.4c02399

Theoretical Investigation of Single-, Double-, and Triple- p-block Metals Anchored on g-CN Monolayer for Oxygen Electrocatalysis

J Phys Chem Lett. 2024 Nov 7:11454-11461. doi: 10.1021/acs.jpclett.4c02399. Online ahead of print.

Authors

Yanan Zhou¹, Li Sheng², Lanlan Chen³, Wenhua Zhang³, Jinlong Yang⁴

Affiliations

¹ School of Material Science and Chemical Engineering, Institute of Mass Spectrometry, Ningbo University, Ningbo, Zhejiang 315211, China.
² Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.
³ Key Laboratory of Materials for Energy Conversion, Chinese Academy of Sciences (CAS), Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, Anhui 230026, China.
⁴ Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China.

PMID: 39509545
DOI: 10.1021/acs.jpclett.4c02399

Abstract

The design and development of highly active non-noble metal electrocatalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are crucial for metal-air batteries. In this work, the electrocatalytic performance of different p-block metal (PM = Sn, Sb, Pb and Bi) atoms embedded in the g-CN monolayer (PM_x@g-CN, x = 1-3) for the OER and ORR was systematically investigated by density functional theory (DFT). The strong interaction between PM_x atoms and g-CN substrates indicates the good stability of PM_x@g-CN catalysts. Among all the designed catalysts, Bi₃@g-CN is found to be a promising bifunctional electrocatalyst for both the OER and ORR with the calculated overpotential η^OER and η^ORR of 0.23 and 0.25 V, respectively. With the atomic active sites of PM_x increasing from x = 1 to 3, the OER and ORR catalytic activity is enhanced. The correlations between the overpotentials of the OER/ORR and Bader charge values of the anchored PM_x atoms of the catalysts were established. Our findings contribute to searching for noble metal-free bifunctional electrocatalysts and shed light on the rational design of atomic active sites on electrocatalysts.