Design of Efficient Oxygen Reduction Reaction Catalysts with Single Transition Metal Atom on N-Doped Graphdiyne

Min Zou; Jing Yang; Xiaolong Yue; Yanan Yuan; Zhongmei Che; Mei Li; Bo Li; Jiaxi Cui; Wei Hu; Shuai Wang; Jun Jiang; Chuanyi Jia

doi:10.1021/acs.jpclett.3c02649

Design of Efficient Oxygen Reduction Reaction Catalysts with Single Transition Metal Atom on N-Doped Graphdiyne

J Phys Chem Lett. 2023 Nov 2;14(43):9624-9632. doi: 10.1021/acs.jpclett.3c02649. Epub 2023 Oct 23.

Authors

Min Zou^{1

2}, Jing Yang³, Xiaolong Yue¹, Yanan Yuan¹, Zhongmei Che¹, Mei Li¹, Bo Li², Jiaxi Cui⁴, Wei Hu¹, Shuai Wang¹, Jun Jiang⁵, Chuanyi Jia²

Affiliations

¹ School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Science), Jinan, Shandong 250353, China.
² Guizhou Provincial Key Laboratory of Computational Nano-Material Science, Institute of Applied Physics, Guizhou Education University, Guiyang, Guizhou 550018, China.
³ Shijiazhuang Key Laboratory of Low Carbon Energy Materials, College of Chemical Engineering, Shijiazhuang University, Shijiazhuang, Hebei 050035, China.
⁴ Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China.
⁵ Key Laboratory of Precision and Intelligent Chemistry, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, Anhui 230026, China.

PMID: 37870322
DOI: 10.1021/acs.jpclett.3c02649

Abstract

The revelation of the underlying structure-property relationship of single-atom catalysts (SACs) is a fundamental issue in the oxygen reduction reaction (ORR). Here we present systematic theoretical and experimental investigations of various N-doped graphdiyne (NGDY) supported transition metals (TMs) to shed light on this relationship. Calculation results indicate that the TMs' comprehensive activities follow the order of Pd@NGDY > Ni@NGDY > Co@NGDY > Fe@NGDY, which fits well with our experimental conclusion. Moreover, detailed structure-property relationship (194 in total) analysis suggests that the key-species binding stability (ΔG_*OH), the d-orbital center (ε_d/ε_d-a) and charge transfer (ΔQ_TM/ΔQ_TM-a) of the active metal before/after reactants adsorption and the bond length of TM-O (L_TM-O) as descriptors can well reflect the intermediate binding stability or ORR activity on different TM-SACs. Specifically, the change trend of catalytic activity is opposite to that of intermediate binding stability, meaning that too strongly bonded *OOH, *O, and *OH intermediates are unfavorable for ORR.