Design of Efficient Oxygen Reduction Reaction Catalysts with Single Transition Metal Atom on N-Doped Graphdiyne
Min Zou, Jing Yang, Yue X, Yanan Yuan, Zhongmei Che, Mei Li, Bo Li, Jiaxi Cui, Wei Hu, Shuai Wang, Jun Jiang, Chuanyi Jia
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 (Δ G *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.