Hydrogen-Intercalation-Induced Lattice Expansion of Pd@Pt Core-Shell Nanoparticles for Highly Efficient Electrocatalytic Alcohol Oxidation

Guigao Liu; Wei Zhou; Yiru Ji; Bo Chen; Gengtao Fu; Qinbai Yun; Shuangming Chen; Yunxiang Lin; Peng-Fei Yin; Xiaoya Cui; Jiawei Liu; Fanqi Meng; Qinghua Zhang; Li Song; Lin Gu; Hua Zhang

doi:10.1021/jacs.1c05856

Hydrogen-Intercalation-Induced Lattice Expansion of Pd@Pt Core-Shell Nanoparticles for Highly Efficient Electrocatalytic Alcohol Oxidation

J Am Chem Soc. 2021 Jul 28;143(29):11262-11270. doi: 10.1021/jacs.1c05856. Epub 2021 Jul 19.

Authors

Guigao Liu^{1

2}, Wei Zhou³, Yiru Ji⁴, Bo Chen¹, Gengtao Fu⁵, Qinbai Yun¹, Shuangming Chen⁶, Yunxiang Lin^{6

7}, Peng-Fei Yin¹, Xiaoya Cui⁸, Jiawei Liu⁸, Fanqi Meng⁴, Qinghua Zhang⁴, Li Song⁶, Lin Gu^{4

9

10}, Hua Zhang^{1

11

12}

Affiliations

¹ Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong, China.
² National Special Superfine Powder Engineering Research Center, School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, Nanjing, Jiangsu 210094, China.
³ Department of Applied Physics, Tianjin Key Laboratory of Low Dimensional Materials Physics, Preparing Technology Faculty of Science, Tianjin University, Tianjin 300072, China.
⁴ Institute of Physics, Beijing National Laboratory for Condensed Matter Physics, Chinese Academy of Sciences, Beijing 100190, China.
⁵ School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore 637459 Singapore.
⁶ National Synchrotron Radiation Laboratory, CAS Centre for Excellence in Nanoscience, University of Science and Technology of China, Hefei, Anhui 230029, China.
⁷ Institutes of Physical Science and Information Technology, Anhui University, Hefei 230601, China.
⁸ Center for Programmable Materials, School of Materials Science and Engineering, Nanyang Technological University, 50 Nanyang Avenue, Singapore 639798, Singapore.
⁹ School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
¹⁰ Songshan Lake Materials Laboratory, Dongguan, Guangdong 523808, China.
¹¹ Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Kowloon,Hong Kong, China.
¹² Shenzhen Research Institute, City University of Hong Kong, Shenzhen 518057, China.

PMID: 34281338
DOI: 10.1021/jacs.1c05856

Abstract

Lattice engineering on specific facets of metal catalysts is critically important not only for the enhancement of their catalytic performance but also for deeply understanding the effect of facet-based lattice engineering on catalytic reactions. Here, we develop a facile two-step method for the lattice expansion on specific facets, i.e., Pt(100) and Pt(111), of Pt catalysts. We first prepare the Pd@Pt core-shell nanoparticles exposed with the Pt(100) and Pt(111) facets, respectively, via the Pd-seeded epitaxial growth, and then convert the Pd core to PdH_0.43 by hydrogen intercalation. The lattice expansion of the Pd core induces the lattice enlargement of the Pt shell, which can significantly promote the alcohol oxidation reaction (AOR) on both Pt(100) and Pt(111) facets. Impressively, Pt mass specific activities of 32.51 A mg_Pt^-1 for methanol oxidation and 14.86 A mg_Pt^-1 for ethanol oxidation, which are 41.15 and 25.19 times those of the commercial Pt/C catalyst, respectively, have been achieved on the Pt(111) facet. Density functional theory (DFT) calculations indicate that the remarkably improved catalytic performance on both the Pt(100) and the Pt(111) facets through lattice expansion arises from the enhanced OH adsorption. This work not only paves the way for lattice engineering on specific facets of nanomaterials to enhance their electrocatalytic activity but also offers a promising strategy toward the rational design and preparation of highly efficient catalysts.

Publication types

Research Support, Non-U.S. Gov't