Revealing the Role of the Metal in Non-Precious-Metal Catalysts for Oxygen Reduction via Selective Removal of Fe,ACS Energy Letters

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Revealing the Role of the Metal in Non-Precious-Metal Catalysts for Oxygen Reduction via Selective Removal of Fe
ACS Energy Letters ( IF 19.3 ) Pub Date : 2018-03-07 00:00:00 , DOI: 10.1021/acsenergylett.8b00144
Jason A. Varnell ₁ , James S. Sotiropoulos ₁ , Therese M. Brown ₁ , Kiran Subedi ₂ , Richard T. Haasch ₃ , Charles E. Schulz ₄ , Andrew A. Gewirth _{1,

5}

Affiliation

Non-precious-metal catalysts have been investigated as alternatives to Pt-based oxygen reduction reaction catalysts for more than 50 years. While the incorporation of a metal is known to be necessary to generate a catalyst with high activity, the exact role of the metal is still not well-understood. In this work, we prepare an active oxygen reduction reaction catalyst containing Fe and then selectively remove the Fe from the catalyst while preserving the carbon and nitrogen species. By comparing the oxygen reduction reaction activity of the catalyst before and after treatment, we show that in the absence of Fe the carbon and nitrogen sites in the catalyst exhibit a larger overpotential and lower selectivity for the 4e^– reduction of oxygen in both acidic and alkaline conditions. These findings reveal the direct involvement of the metal in the active site of non-precious-metal catalysts and provide important guidance for future catalyst improvements.

中文翻译：

揭示了金属在非贵金属催化剂中通过选择性去除铁而减少氧的作用

50多年来，人们一直在研究非贵金属催化剂作为基于Pt的氧还原反应催化剂的替代品。尽管已知掺入金属对于产生具有高活性的催化剂是必需的，但是金属的确切作用仍未被很好地理解。在这项工作中，我们准备了一种含Fe的活性氧还原反应催化剂，然后在保留碳和氮物种的同时，选择性地从催化剂中除去Fe。通过在处理之前和之后比较催化剂的氧还原反应活性，我们表明，在不存在的Fe在催化剂中的碳和氮的位点表现出对于4更大的超电势和较低的选择性ë ^-在酸性和碱性条件下都可以减少氧气。这些发现揭示了金属直接参与了非贵金属催化剂的活性位，并为未来催化剂的改进提供了重要的指导。

更新日期：2018-03-07

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