Platinum-Lead-Bismuth/Platinum-Bismuth Core/Shell Nanoplate Achieves Complete Dehydrogenation Pathway for Direct Formic Acid Oxidation Catalysis

Xinrui Hu; Zhengyi Xiao; Weizhen Wang; Lingzheng Bu; Zhengchao An; Shangheng Liu; Chih-Wen Pao; Changhong Zhan; Zhiwei Hu; Zhiqing Yang; Yucheng Wang; Xiaoqing Huang

doi:10.1021/jacs.3c00262

Platinum-Lead-Bismuth/Platinum-Bismuth Core/Shell Nanoplate Achieves Complete Dehydrogenation Pathway for Direct Formic Acid Oxidation Catalysis

J Am Chem Soc. 2023 Jul 19;145(28):15109-15117. doi: 10.1021/jacs.3c00262. Epub 2023 Jun 8.

Authors

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
² Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China.
³ College of Energy, Xiamen University, Xiamen 361102, China.
⁴ National Synchrotron Radiation Research Center, Hsinchu 30076, Taiwan.
⁵ College of Chemistry, Max Planck Institute for Chemical Physics of Solids, Nothnitzer Strasse 40, Dresden 01187, Germany.
⁶ Ji Hua Laboratory, Foshan 528200, China.

PMID: 37289521
DOI: 10.1021/jacs.3c00262

Abstract

Designing platinum (Pt)-based formic acid oxidation reaction (FAOR) catalysts with high performance and high selectivity of direct dehydrogenation pathway for direct formic acid fuel cell (DFAFC) is desirable yet challenging. Herein, we report a new class of surface-uneven PtPbBi/PtBi core/shell nanoplates (PtPbBi/PtBi NPs) as the highly active and selective FAOR catalysts, even in the complicated membrane electrode assembly (MEA) medium. They can achieve unprecedented specific and mass activities of 25.1 mA cm^-2 and 7.4 A mg_Pt^-1 for FAOR, 156 and 62 times higher than those of commercial Pt/C, respectively, which is the highest for a FAOR catalyst by far. Simultaneously, they show highly weak adsorption of CO and high dehydrogenation pathway selectivity in the FAOR test. More importantly, the PtPbBi/PtBi NPs can reach the power density of 161.5 mW cm^-2, along with a stable discharge performance (45.8% decay of power density at 0.4 V for 10 h), demonstrating great potential in a single DFAFC device. The in situ Fourier transform infrared spectroscopy (FTIR) and X-ray absorption spectroscopy (XAS) results collectively reveal a local electron interaction between PtPbBi and PtBi. In addition, the high-tolerance PtBi shell can effectively inhibit the production/adsorption of CO, resulting in the complete presence of the dehydrogenation pathway for FAOR. This work demonstrates an efficient Pt-based FAOR catalyst with 100% direct reaction selectivity, which is of great significance for driving the commercialization of DFAFC.