Liu Zeyan, Zhao Zipeng, Peng Bosi, Duan Xiangfeng, Huang Yu
Department of Materials Science and Engineering, University of California, Los Angeles, California 90095, United States.
Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095, United States.
J Am Chem Soc. 2020 Oct 21;142(42):17812-17827. doi: 10.1021/jacs.0c07696. Epub 2020 Sep 30.
Increasing the platinum utilization efficiency is the key to the advancement and broad dissemination of proton-exchange-membrane fuel cells (PEMFCs). Central to the task is the creation of highly active and durable Pt-based catalysts for the cathodic oxygen reduction reaction (ORR), which demands a comprehensive understanding of the ORR processes on these catalysts under reaction conditions. Past efforts have accumulated a vast wealth of knowledge of the ORR on extended Pt and Pt-alloy model surfaces. While the knowledge has been applied to understanding and designing ORR catalysts, it has also been recognized that these understandings cannot always translate into nanoscale systems. In this Perspective, we will review the progress that the theoretical descriptor has evolved to reconcile the observed differences between extended and nanoscale Pt surfaces, and we highlight the needs in advancing both characterizations and theories in order to understand ORR in the more complex Pt-alloy nanocatalysts. Particularly, understanding the dynamic structure-composition-function relation of Pt-alloy nanocatalysts during ORR demands concerted efforts in precision synthesis, advanced atomistic-scale in situ characterization, and comprehensive computational models.
提高铂的利用效率是质子交换膜燃料电池（PEMFC）取得进展并广泛推广的关键。这项任务的核心是制备用于阴极氧还原反应（ORR）的高活性、耐用的铂基催化剂，这需要全面了解这些催化剂在反应条件下的ORR过程。过去的研究积累了大量关于外延铂和铂合金模型表面ORR的知识。虽然这些知识已被用于理解和设计ORR催化剂，但人们也认识到，这些理解并不总能转化到纳米尺度体系中。在这篇展望文章中，我们将回顾理论描述符在调和外延铂表面和纳米尺度铂表面之间观察到的差异方面所取得的进展，并强调推进表征和理论研究的必要性，以便理解更为复杂的铂合金纳米催化剂中的ORR。特别是，要理解铂合金纳米催化剂在ORR过程中的动态结构-组成-功能关系，需要在精确合成、先进的原子尺度原位表征和全面的计算模型方面共同努力。
