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.

中文翻译：

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铂-铅-铋/铂-铋核/壳纳米板实现了直接甲酸氧化催化的完整脱氢途径

为直接甲酸燃料电池（DFAFC）设计具有高性能和高选择性直接脱氢途径的铂（Pt）基甲酸氧化反应（FAOR）催化剂是理想但具有挑战性的。在此，我们报道了一类新型表面不均匀的 PtPbBi/PtBi 核/壳纳米板（PtPbBi/PtBi NP），作为高活性和选择性的FAOR催化剂，即使在复杂的膜电极组件（MEA）介质中也是如此。它们可以为FAOR实现前所未有的比活度和质量活度，分别为25.1 mA cm ^–2和7.4 A mg _Pt ^–1，分别比商业Pt/C高156倍和62倍，这是迄今为止FAOR催化剂的最高值。同时，它们在FAOR测试中表现出极弱的CO吸附和高脱氢途径选择性。更重要的是，PtPbBi/PtBi NPs可以达到161.5 mW cm ^–2的功率密度，并且具有稳定的放电性能（0.4 V下10 h功率密度衰减45.8%），在单个DFAFC器件中展现出巨大的潜力。原位傅里叶变换红外光谱 (FTIR) 和 X 射线吸收光谱 (XAS) 结果共同揭示了 PtPbBi 和 PtBi 之间的局域电子相互作用。此外，高耐受性的PtBi壳可以有效抑制CO的产生/吸附，从而导致FAOR脱氢途径的完全存在。该工作展示了一种高效的Pt基FAOR催化剂，其直接反应选择性为100%，对于推动DFAFC的商业化具有重要意义。