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Boosting Formate Electrooxidation by Heterostructured PtPd Alloy and Oxides Nanowires
Advanced Materials ( IF 29.4 ) Pub Date : 2024-04-16 , DOI: 10.1002/adma.202403664
Tian‐Jiao Wang 1, 2, 3 , Li‐Bo Sun 3, 4 , Xuan Ai 1 , Pei Chen 1 , Yu Chen 1 , Xin Wang 4, 5
Affiliation  

Direct formate fuel cells (DFFCs) receive increasing attention as promising technologies for the future energy mix and environmental sustainability, as formate can be made from carbon dioxide utilization and is carbon neutral. Herein, heterostructured platinum-palladium alloy and oxides nanowires (PtPd-ox NWs) with abundant defect sites are synthesized through a facile self-template method and demonstrated high activity toward formate electrooxidation reaction (FOR). The electronic tuning arising from the heterojunction between alloy and oxides influence the work function of PtPd-ox NWs. The sample with optimal work function reveals the favorable adsorption behavior for intermediates and strong interaction in the dp orbital hybridization between Pt site and oxygen in formate, favoring the FOR direct pathway with a low energy barrier. Besides the thermodynamic regulation, the heterostructure can also provide sufficient hydroxyl species to facilitate the formation of carbon dioxide due to the ability of combining absorbed hydrogen and carbon monoxide at adjacent active sites, which contributes to the improvement of FOR kinetics on PtPd-ox NWs. Thus, heterostructured PtPd-ox NWs achieve dual regulation of FOR thermodynamics and kinetics, exhibiting remarkable performance and demonstrating potential in practical systems.

中文翻译:

通过异质结构 PtPd 合金和氧化物纳米线促进甲酸盐电氧化

直接甲酸盐燃料电池(DFFC)作为未来能源结构和环境可持续性的有前途的技术而受到越来越多的关注,因为甲酸盐可以利用二氧化碳制成,并且是碳中性的。在此,通过简单的自模板方法合成了具有丰富缺陷位点的异质结构铂钯合金和氧化物纳米线(PtPd-ox NW),并表现出对甲酸盐电氧化反应(FOR)的高活性。合金和氧化物之间的异质结产生的电子调谐影响 PtPd-ox 纳米线的功函数。具有最佳功函数的样品显示出对中间体有利的吸附行为以及甲酸盐中Pt位点与氧之间的d - p轨道杂化中的强相互作用,有利于具有低能垒的FOR直接途径。除了热力学调节之外,异质结构还可以提供足够的羟基物质,以促进二氧化碳的形成,因为它能够在相邻的活性位点结合吸收的氢气和一氧化碳,这有助于改善PtPd-ox NWs上的FOR动力学。因此,异质结构的PtPd-ox NWs实现了FOR热力学和动力学的双重调节,表现出卓越的性能并在实际系统中展示了潜力。
更新日期:2024-04-16
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