Hu Xinrui, An Zhengchao, Wang Weizhen, Lin Xin, Chan Ting-Shan, Zhan Changhong, Hu Zhiwei, Yang Zhiqing, Huang Xiaoqing, Bu Lingzheng
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China.
J Am Chem Soc. 2023 Sep 6;145(35):19274-19282. doi: 10.1021/jacs.3c04580. Epub 2023 Aug 16.
To promote the commercialization of direct formic acid fuel cell (DFAFC), it is vital to explore new types of direct formic acid oxidation (FAOR) catalysts with high activity and direct pathway. Here, we report the synthesis of intermetallic platinum-lead/platinum nanoplates inlaid with sub-monolayer antimony oxide surface (PtPb/Pt@sub-SbO NPs) for efficient catalytic applications in FAOR. Impressively, they can achieve the remarkable FAOR specific and mass activities of 28.7 mA cm and 7.2 A mg, which are 151 and 60 times higher than those of the state-of-the-art commercial Pt/C, respectively. Furthermore, the X-ray photoelectron spectroscopy and X-ray absorption spectroscopy results collectively reveal the optimization of the local coordination environment by the surface sub-monolayer SbO, along with the electron transfer from Pb and Sb to Pt, driving the predominant dehydrogenation process. The sub-monolayer SbO on the surface can effectively attenuate the CO generation, largely improving the FAOR performance of PtPb/Pt@sub-SbO NPs. This work develops a class of high-performance Pt-based anodic catalyst for DFAFC via constructing the unique intermetallic core/sub-monolayer shell structure.
为推动直接甲酸燃料电池（DFAFC）的商业化，探索具有高活性和直接反应途径的新型直接甲酸氧化（FAOR）催化剂至关重要。在此，我们报道了镶嵌有亚单层氧化锑表面的金属间铂 - 铅/铂纳米片（PtPb/Pt@sub - SbO NPs）的合成，用于FAOR中的高效催化应用。令人印象深刻的是，它们可实现28.7 mA cm²和7.2 A mg⁻¹的显著FAOR比活性和质量活性，分别比最先进的商业Pt/C高151倍和60倍。此外，X射线光电子能谱和X射线吸收光谱结果共同揭示了表面亚单层SbO对局部配位环境的优化，以及从Pb和Sb到Pt的电子转移，推动了主要的脱氢过程。表面的亚单层SbO可有效减弱CO的生成，极大地提高了PtPb/Pt@sub - SbO NPs的FAOR性能。这项工作通过构建独特的金属间核/亚单层壳结构，开发了一类用于DFAFC的高性能Pt基阳极催化剂。
