Enhanced Electroactivity for Overall Water Splitting and Oxygen Potential of Pt/Carbon Nanotubes Functionalized with Cu Organometallic Complex

Abstract

Developing cost‐effective technology for overall electrochemical water splitting requires multifunctional nanocatalysts with reduced Pt‐content. In this work, (5 wt%) Pt/carbon nanotubes (Pt/CNT) functionalized with the [(C 6 H 2 (CH 3 ) 3 ) 2 Cu] (labeled as Pt/CNT Cu‐mes ) and [(η 6 ‐C 6 H 5 OCH 2 CH 2 OH)RuCl 2 ] 2 (labeled as Pt/CNT Ru‐dim ) organometallic complexes are implemented for electrochemical water splitting. Pt/CNT Cu‐mes shows high performance for hydrogen/oxygen evolution reaction (HER/OER), and oxygen reduction reactions, while the catalytic activity of Pt/CNT Ru‐dim is limited to HER only. Pt/CNT Cu‐mes outperformed 20% Pt/C for the HER and the OER, while sustaining a comparable behavior for the ORR, after accelerated degradation tests. Moreover, Pt/CNT Cu‐mes showed water splitting overpotential () and oxygen potential () comparable (cycle 1) and enhanced (cycle 3000) related to 20% Pt/C. Additionally, the polarization curve of a Pt/CNT Cu‐mes ||Pt/CNT Cu‐mes electrolyzer showed a higher performance and stability compared to one 20% Pt/C||20% Pt/C. The high performance of Pt/CNT Cu‐mes is ascribed to the development of Pt‐Cu alloyed phases and Cu oxides due to functionalization, which in turn led to a modification of its Pt electronic structure as confirmed by the shift of Pt 0 species and upshifting of d‐band center, and a contraction of its interplanar distance, compared to non‐alloyed Pt. Thus, Pt/CNT Cu‐mes revealed a high potential for water splitting/oxygen reactions applications.

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Identifiers

DOI

10.1002/ente.202402438

Journal

Energy Technology

Year

2025