Enhancing Methanol Oxidation Reaction with Platinum‐based Catalysts using a N‐Doped Three‐dimensional Graphitic Carbon Support
Enhancing Methanol Oxidation Reaction with Platinum‐based Catalysts using a N‐Doped Three‐dimensional Graphitic Carbon Support
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DOI：
10.1002/cctc.202001162
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发表时间：
2020-12
期刊：
影响因子：
4.5
通讯作者：
Ayyappan Elangovan;Jiayi Xu;Archana Sekar;B. Liu;Jun Li
中科院分区：
文献类型：
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作者：
Ayyappan Elangovan;Jiayi Xu;Archana Sekar;B. Liu;Jun Li
氮掺杂的石墨碳材料已广泛用作甲醇氧化反应（莫尔）中的催化剂载体。在这项研究中，我们报告了三维结构的原位N掺杂的垂直排列的碳纳米纤维（VACNF）作为催化剂支持莫尔在酸性和碱性介质中的作用。在N掺杂的VACNF的侧壁处的丰富的石墨边缘位点强烈地锚沉积的铂族金属（PGM）催化剂并诱导PGM催化剂和载体之间的部分电子转移。密度泛函理论（DFT）计算揭示，强的金属-载体相互作用显著增加了OH的吸附能，特别是在N-掺杂位点附近，这有助于竞争和去除在莫尔期间产生的吸附的中间物质。与商业Vulcan碳载体相比，在N掺杂的VACNF载体上的PGM催化剂在较低的电势下表现出CO汽提，并表现出增强的电催化性能和更好的莫尔耐久性。
Nitrogen‐doped graphitic carbon materials have been widely used as a catalyst support in the methanol oxidation reaction (MOR). In this study, we report the role of three‐dimensionally architectured in‐situ N‐doped vertically aligned carbon nanofibers (VACNF) as a catalyst support for MOR in acidic and alkaline media. The abundant graphitic edge sites at the sidewall of N‐doped VACNF strongly anchor the deposited platinum group metal (PGM) catalysts and induce a partial electron transfer between the PGM catalysts and support. Density Functional Theory (DFT) calculations reveal that the strong metal‐support interaction substantially increases the adsorption energy of OH, particularly near the N‐doping sites, which helps to compete and remove the adsorbed intermediate species generated during MOR. The PGM catalysts on N‐doped VACNF support exhibits CO stripping at lower potentials comparing to the commercial Vulcan carbon support and presents an enhanced electrocatalytic performance and better durability for MOR.