Amplified Interfacial Effect on Atomically Dispersed RuOx-on-Pd 2D Inverse Nanocatalysts for High-Performance Oxygen Reduction

• Published in: Angewandte Chemie International Edition 2021-04
• Main Authors: Lyu, Zixi, Zhang, Xia-Guang, Wang, Yucheng, Liu, Kai, Qiu, Chunyu, Liao, Xinyan, Yang, Weihua, Xie, Zhaoxiong, Xie, Shuifen
• Format: Article
• Language: English
• ISSN: 1521-3773
• DOI: 10.1002/anie.202104013

Atomically dispersed oxide-on-metal inverse nanocatalysts provide a practicable blueprint to amplify the strong oxide-metal interactions for heterocatalysis but remain a grand challenge in fabrication. Here we report a 2D inverse nanocatalyst, named RuOx-on-Pd nanosheets, by in-situ creating atomically dispersed RuOx/Pd interfaces densely on ultrathin Pd nanosheets via a one-pot synthesis. The products deliver unexpected performance toward oxygen reduction reaction (ORR) in alkaline, which represents 8.0- and 22.4-fold enhancements in mass activity compared to the state-of-the-art Pt/C and Pd/C, respectively, showcasing an excellent Pt-alternative cathode electrocatalyst for fuel cells and metal-air batteries. Density functional theory calculations validate that the RuOx/Pd interfaces can accumulate partial charge from the 2D Pd hosts and subtly change the adsorption configuration of O2 to facilitate the O-O bond fracture. Meanwhile, the d-band center of Pd nanosubstrates is factually down-shifted for weakening the oxygen binding strength, tandemly motivating the excellent ORR catalysis on the RuOx-on-Pd nanosheets.