Pt-based oxygen reduction reaction catalysts: from single crystal electrode to nanostructured extended surface

doi:10.11949/0438-1157.20231215

Abstract

Abstract:

The development of low-cost, high-performance oxygen reduction platinum-based catalysts is still an important direction in promoting the commercialization of proton exchange membrane fuel cells (PEMFC). The investigations of the single crystal electrode surface showed the factors such as the atomic arrangement, strain between lattices, and coordination environment of the Pt metal are responsible for the activity of oxygen reduction reaction. However, the knowledge gained from extended surfaces of single crystal electrodes cannot entirely guide the design of nanocatalysts due to the see-saw relationship between activity and utilization arising from size effects in nanoparticles. By simulating the properties of single crystal electrodes at the nanoscale, it is possible to expand surface properties and achieve the two-win results to some extent. This paper reviews the theoretical and experimental results regarding the use of extended surface catalysts for the oxygen reduction reaction, and the insights into the remaining challenges and research directions of nanocatalysts are also proposed.

Key words: oxygen reduction, fuel cell, single crystal electrode, nanocatalysts, electrochemistry, hydrogen

摘要：

开发低成本、高性能的氧还原铂基催化剂仍然是目前推动质子交换膜燃料电池（PEMFC）商业化进程的重要方向。在拓展单晶电极表面的相关研究中，活性金属铂的原子排布、应力应变、周边配位环境等因素都被认为对氧还原的性能具有重要影响。然而，在规整表面的单晶电极上得到的经验并不能完全指导纳米催化剂的设计，这是因为纳米颗粒存在着尺寸效应带来的活性-利用率的矛盾关系。通过在纳米尺度上模拟单晶电极的性质，构造纳米薄膜材料及二维晶面可控的纳米材料，可以一定程度上实现拓展表面性质。结合本课题组的研究工作，本文总结了拓展表面催化剂用于氧还原反应的理论和实验结果，探讨了纳米催化剂的发展和目前存在的问题，并对今后的研究方向进行了展望。

关键词: 氧还原, 燃料电池, 单晶电极, 纳米催化剂, 电化学, 氢

CLC Number:

TQ 035

Mingze SUN, Helai HUANG, Zhiqiang NIU. Pt-based oxygen reduction reaction catalysts: from single crystal electrode to nanostructured extended surface[J]. CIESC Journal, 2024, 75(4): 1256-1269.

孙铭泽, 黄鹤来, 牛志强. 铂基氧还原催化剂：从单晶电极到拓展表面纳米材料[J]. 化工学报, 2024, 75(4): 1256-1269.

Figures/Tables 6

Fig.1 2e- and 4e- mechanisms of ORR (a); Scaling relationship of *OOH and *OH intermediates (b)[27]; Volcano plot of ORR (c)[28]

Fig.2 Origin of the increase of ORR activity by step sites (a)[39]; Increase of ORR activities for defective Pt(111) cavity (b)[40]; Schematic illustration of strain effect (c)[44]; Specific activity (d) as well as theory calculation (e) of Pt and Pt3M electrodes[45]

Fig.3 Relationship between particle size and terrace site fraction (a)[71]; Influence of low Pt loading for ORR activity especially at high current density (b)[72]

Fig.2 Schematic illustration of the preperation and structure of NSTF catalyst (a)[84]; Schematic illustration of the synthesis of aerogel (b)[85]; Schematic illustration of the synthesis of meso-structured Pt (c)[89]

Fig.5 HAADF-STEM image of an individual octahedral nanocage (a); Specific activities and mass activities at 0.9 V (RHE) of octahedral nanocages, cubic nanocages, and TKK Pt/C (b)[96]; TEM image of PtPb/Pt hexagonal nanoplates (c); Specific activities and mass activities of hexagonal nanoplates after stability test (d)[97]

Fig.6 Schematic illustration of the synthesis of extended PtCuNi catalyst (a); Representative HAADF-STEM image of Cu@PtNi core-shell nanowire (b); EDS elemental mapping of Cu@PtNi core-shell nanowire (c); Specific activities and mass activities at 0.9 V （RHE） of extended PtCuNiAu, extended PtCuNi, PtCuNi NPs and commercial Pt/C (d); H2-air fuel cell polarization and power density plots of commercial Pt/C and extended PtCuNi (e)[102]

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