Research Article


2022, 15(2): 1288–1294


Fine-tuning of Pd-Rh core-shell catalysts by interstitial hydrogen doping for enhanced methanol oxidation

Xiaoyun Guo1, Zheng Hu1, Jianxin Lv1,2, Hui Li1,2, Qinghua Zhang3, Lin Gu3, Wei Zhou1, Jiangwei Zhang4 (✉), and Shi Hu1,2 (✉)

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1 Department of Chemistry, School of Science, Tianjin Key Laboratory of Molecular Optoelectronic Science, Tianjin University, Tianjin 300072, China
2 Institute of Energy, Hefei Comprehensive National Science Center, Hefei 230031, China
3 Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Science, Beijing 100190, China
4 Dalian National Laboratory for Clean Energy & State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics Chinese Academy of Sciences (CAS), Dalian 116023, China

Keywords: core-shell structure, electrocatalysis, methanol oxidation reaction, interstitial alloy, hydride
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Metal catalysts play an important role in the catalytic electrochemical processes and optimization of their performance is usually achieved through alloying with other metal atoms. Doping with interstitial hydrogen atoms is a special but effective way to regulate the electronic structure of host catalysts. Herein we demonstrate the intermixing of Pd and Rh atoms during the hydrogen-doping process of Pd@Rh core-shell nanocubes, forming an alloyed surface in Pd@Rh-H. The catalysts show enhanced performance in electrocatalytic methanol oxidation, as compared to commercial Pt/C and are even better than PdH@Rh core-shell nanocubes. The small structural differences between the two hydride catalysts are revealed by X-ray electron spectroscopy and pair distribution function analysis of electron diffraction. The theoretical calculation results show that Rh in Pd@Rh-H contains more negative charges than Rh in PdH@Rh, indicating more effective charge transfer in Pd@Rh-H. The d-band center (εd) of the Rh site in Pd@Rh-H shifts up, and the synergy between Rh and Pd optimizes the binding energy of CO and OH, inducing preferential catalytic activity. Our work provides guidance for the synthesis of high-performance catalysts by doping with interstitial atoms, which may provide a new strategy to fine-tune the electronic structure of other bimetallic nanoparticles.
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Fine-tuning of Pd-Rh core-shell catalysts by interstitial hydrogen doping for enhanced methanol oxidation. Nano Res. 2022, 15(2): 1288–1294

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