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

被引:56
作者
Hu, Xinrui [1 ]
Xiao, Zhengyi [1 ]
Wang, Weizhen [2 ]
Bu, Lingzheng [6 ]
An, Zhengchao [1 ]
Liu, Shangheng [1 ]
Pao, Chih-Wen [3 ]
Zhan, Changhong [1 ]
Hu, Zhiwei [4 ]
Yang, Zhiqing [5 ]
Wang, Yucheng [1 ]
Huang, Xiaoqing [1 ]
机构
[1] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Xiamen 361005, Peoples R China
[2] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
[3] Natl Synchrotron Radiat Res Ctr, Hsinchu 30076, Taiwan
[4] Max Planck Inst Chem Phys Solids, Coll Chem, D-01187 Dresden, Germany
[5] Ji Hua Lab, Foshan 528200, Peoples R China
[6] Xiamen Univ, Coll Energy, Xiamen 361102, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金;
关键词
OXYGEN REDUCTION; ELECTROCATALYSTS; METHANOL; MECHANISM; CARBON;
D O I
10.1021/jacs.3c00262
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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.
引用
收藏
页码:15109 / 15117
页数:9
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