4.8 Article

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

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 145, Issue 28, Pages 15109-15117

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.3c00262

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This study introduces a new class of PtPbBi/PtBi core/shell nanoplates as highly active and selective catalysts for formic acid oxidation reaction (FAOR) in direct formic acid fuel cells (DFAFC). These catalysts exhibit unprecedented specific and mass activities, with a selectivity for the dehydrogenation pathway. The PtPbBi/PtBi nanoplates demonstrate high power density and stable performance in a single DFAFC device, showing great potential for commercialization. This work is of significant importance for driving the development of DFAFCs.
Designingplatinum (Pt)-based formic acid oxidation reaction (FAOR)catalysts with high performance and high selectivity of direct dehydrogenationpathway for direct formic acid fuel cell (DFAFC) is desirable yetchallenging. Herein, we report a new class of surface-uneven PtPbBi/PtBicore/shell nanoplates (PtPbBi/PtBi NPs) as the highly active and selectiveFAOR catalysts, even in the complicated membrane electrode assembly(MEA) medium. They can achieve unprecedented specific and mass activitiesof 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 pathwayselectivity in the FAOR test. More importantly, the PtPbBi/PtBi NPscan reach the power density of 161.5 mW cm(-2), alongwith a stable discharge performance (45.8% decay of power densityat 0.4 V for 10 h), demonstrating great potential in a single DFAFCdevice. The in situ Fourier transform infrared spectroscopy(FTIR) and X-ray absorption spectroscopy (XAS) results collectivelyreveal a local electron interaction between PtPbBi and PtBi. In addition,the high-tolerance PtBi shell can effectively inhibit the production/adsorptionof CO, resulting in the complete presence of the dehydrogenation pathwayfor FAOR. This work demonstrates an efficient Pt-based FAOR catalystwith 100% direct reaction selectivity, which is of great significancefor driving the commercialization of DFAFC.

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