Enabling Efficient Oxygen Reduction Reaction with Pt Single Atoms on Carbide: A Phosphorus-Doped Mo<sub>2</sub>C Interface Strategy.

Shi, Changwei; Jiang, Xingmao; Qi, Xueqiang; Xing, Congcong; Fan, Xiaolei; Chen, Zhuo; Wang, Xiang; Cabot, Andreu · Nano Lett · 2025

basic_science · Level V

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Abstract

Developing efficient and cost-effective oxygen reduction reaction (ORR) catalysts is a critical process in electrochemical energy conversion technologies. Here, we report a new heterostructured electrocatalyst composed of phosphorus-doped Mo<sub>2</sub>C coupled with atomically dispersed Pt sites (Pt/P-Mo<sub>2</sub>C). This is realized through a confined polymerization approach using heteropolyacid-pyrrole complexes and subsequent covalent anchoring. Phosphorus doping plays a crucial role in enhancing the interfacial electron density and enabling strong electronic interactions with Pt atoms. The results showed that the interfacial electronic structure of Pt is significantly modulated, with a downshifted d-band center that optimizes the adsorption/desorption energetics of ORR intermediates. As a result, Pt/P-Mo<sub>2</sub>C demonstrates outstanding ORR activity in alkaline media, achieving a half-wave potential (<i>E</i><sub>1/2</sub>) of 0.91 V along with excellent stability. This work presents a generic strategy for integrating single-atom noble metals with carbide supports and highlights the role of interfacial electron engineering in the design of next-generation ORR electrocatalysts.