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金属前驱体在制备用于氧还原反应的双原子催化剂中的作用。

Role of the Metal Precursor in Preparing Dual-Atom Catalysts for the Oxygen Reduction Reaction.

作者信息

Zhu Xiu, Liu Genlin, Tao Xiafang, Huang Pengwei, Wang Qing, Chen Guangbo, Yang Juan, Zhang Liang, Zhou Yazhou

机构信息

School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, Jiangsu, China.

Institute of Functional Nano & Soft Materials (FUNSOM), Soochow University, Suzhou 215123, Jiangsu, China.

出版信息

ACS Omega. 2023 Oct 24;8(44):41708-41717. doi: 10.1021/acsomega.3c06005. eCollection 2023 Nov 7.

Abstract

Dual-atom catalysts (DACs) have arisen as a novel type of heterogeneous catalyst that extends from single-atom catalysts (SACs) by incorporating two kinds of metals. These materials have demonstrated enhanced performance when compared to SACs. The choice of metal precursors plays an important role in the synthesis of DACs. Here, we choose Fe and Co as DAC models and study types, contents, molar ratios of two precursors, and oxygen reduction reaction (ORR) activity. The Fe,Co DACs were synthesized by an adsorption-annealing approach, using nitrogen-doped graphitic carbon (NC) as the support. As a result, the adsorption ability of metal precursors on the support determines the metal loadings in Fe and Co DACs, leading to differences in ORR performance. The Fe precursors win the adsorption competitions in most cases, resulting in a much higher loading than that of Co precursors. Importantly, it is difficult to increase the precursor content by simply increasing the initial amount. Choosing the right combination of metal precursors, such as ferrocene and cobalt chloride, can yield Fe,Co DACs with enhanced ORR performance..

摘要

双原子催化剂(DACs)作为一种新型的多相催化剂应运而生,它是通过引入两种金属从单原子催化剂(SACs)扩展而来的。与单原子催化剂相比,这些材料已展现出更高的性能。金属前驱体的选择在双原子催化剂的合成中起着重要作用。在此,我们选择铁和钴作为双原子催化剂模型,研究两种前驱体的类型、含量、摩尔比以及氧还原反应(ORR)活性。铁钴双原子催化剂采用吸附退火法合成,以氮掺杂石墨碳(NC)为载体。结果表明,金属前驱体在载体上的吸附能力决定了铁钴双原子催化剂中的金属负载量,从而导致氧还原反应性能的差异。在大多数情况下,铁前驱体在吸附竞争中胜出,导致其负载量远高于钴前驱体。重要的是,简单增加初始量很难提高前驱体含量。选择合适的金属前驱体组合,如二茂铁和氯化钴,能够制备出具有增强氧还原反应性能的铁钴双原子催化剂。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/0d7c/10633877/5e3fbc6e9666/ao3c06005_0001.jpg

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