Tailoring Surface Electronic Structure of Spinel Co3O4 Oxide via Fe and Cu Substitution for Enhanced Oxygen Evolution Reaction

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2024-09-20 DOI:10.1021/acsmaterialslett.4c00857

Mahmoud G. Ahmed, Ying Fan Tay, Mengyuan Zhang, Sing Yang Chiam, Lydia H. Wong

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引用次数: 0

Abstract

Multimetal spinel oxides are promising candidates for the oxygen evolution reaction (OER) due to their ability to offer more accessible active sites and oxygen vacancies (O_vac). However, the utilization of redox-active species in spinel oxides is limited. Herein, we unveil an efficient multimetal spinel oxide using high-throughput methods. The oxide contains Fe and Cu substituted into Co sites following a stoichiometry of Fe_0.6Cu_0.6Co_1.8O₄. The dual cation substitution of Fe and Cu manipulates the electronic states and generates O_vac, thereby generating more accessible active species. This significantly improves the OH^– adsorption capacity on spinel oxide triggering a more favorable OER reaction with a low overpotential of 265 mV at 10 mA cm^–2 and high durability in an alkaline medium. Our work not only presents the utilization of a high-throughput approach to explore efficient catalysts with optimal composition but also provides useful insights into the modulation of electronic states for enhanced catalytic performance.

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通过铁和铜置换调整尖晶石 Co3O4 氧化物的表面电子结构以增强氧进化反应

多金属尖晶石氧化物能够提供更多的活性位点和氧空位（Ovac），因此是氧气进化反应（OER）的理想候选物质。然而，尖晶石氧化物中氧化还原活性物种的利用率有限。在此，我们利用高通量方法揭示了一种高效的多金属尖晶石氧化物。该氧化物中的 Fe 和 Cu 按照 Fe0.6Cu0.6Co1.8O4 的化学计量取代了 Co 的位点。Fe和Cu的双阳离子置换操纵了电子状态并产生了Ovac，从而产生了更容易获得的活性物种。这大大提高了尖晶石氧化物对 OH- 的吸附能力，引发了更有利的 OER 反应，在 10 mA cm-2 时过电位低至 265 mV，并且在碱性介质中具有很高的耐久性。我们的工作不仅展示了利用高通量方法探索具有最佳组成的高效催化剂的方法，而且还为调控电子状态以提高催化性能提供了有益的见解。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.