Amplified Interfacial Effect in an Atomically Dispersed RuOx‐on‐Pd 2D Inverse Nanocatalyst for High‐Performance Oxygen Reduction

• Published in: Angewandte Chemie International Edition Vol. 60; no. 29; pp. 16093 - 16100
• Main Authors: Lyu, Zixi, Zhang, Xia‐Guang, Wang, Yucheng, Liu, Kai, Qiu, Chunyu, Liao, Xinyan, Yang, Weihua, Xie, Zhaoxiong, Xie, Shuifen
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 12.07.2021
• Edition: International ed. in English
• Subjects: Catalysts; Chemical reduction; Density functional theory; Dispersion; Electrocatalysts; electronic modulation; Fabrication; Fuel cells; Interfaces; Nanocatalysis; Nanostructure; non-platinum electrocatalysts; Oxygen; oxygen reduction reaction; Oxygen reduction reactions; Palladium; Platinum; RuOx/Pd interface
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.202104013

Atomically dispersed oxide‐on‐metal inverse nanocatalysts provide a blueprint to amplify the strong oxide–metal interactions for heterocatalysis but remain a grand challenge in fabrication. Here we report a 2D inverse nanocatalyst, RuOx‐on‐Pd nanosheets, by in situ creating atomically dispersed RuOx/Pd interfaces densely on ultrathin Pd nanosheets via a one‐pot synthesis. The product displays unexpected performance toward the oxygen reduction reaction (ORR) in alkaline medium, which represents 8.0‐ and 22.4‐fold enhancement in mass activity compared to the state‐of‐the‐art Pt/C and Pd/C catalysts, respectively, showcasing an excellent Pt‐alternative cathode electrocatalyst for fuel cells and metal–air batteries. Density functional theory calculations validate that the RuOx/Pd interface can accumulate partial charge from the 2D Pd host and subtly change the adsorption configuration of O2 to facilitate the O−O bond cleavage. Meanwhile, the d‐band center of Pd nanosubstrates is effectively downshifted, realizing weakened oxygen binding strength. An atomically dispersed RuOx‐on‐Pd ultrathin 2D inverse nanocatalyst with amplified oxide/metal interface effects may serve as an excellent Pt‐alternative cathode electrocatalyst for fuel cells and metal–air batteries.