CeO2-Induced Interfacial Co2+ Octahedral Sites and Oxygen Vacancies for Water Oxidation

IF 13.6 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2019-06-19 DOI:10.1021/acscatal.9b01819

Bocheng Qiu, Cong Wang, Ning Zhang, Lejuan Cai, Yujie Xiong, Yang Chai*

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引用次数: 212

Abstract

Electrocatalytic oxygen evolution reaction (OER) is a key process in electrochemical energy conversion and storage. Cobalt-containing spinel oxides are promising candidates for OER, but suffer from cation deficiency during OER, because of the high stability and reversibility of the spinel structure. Herein, we combine catalytically inactive CeO₂ and spinel structure Co₃O₄ (CeO₂/Co₃O₄) by a built-in p–n heterojunction. The strongly coupled p–n heterojunction interface allows a rapid interfacial charge transfer from CeO₂ to Co₃O₄, which leads to a high concentration of oxygen vacancies and the generation of Co²⁺ octahedral (Co²⁺(O_h)) sites from the reduction of Co³⁺(O_h) at the CeO₂/Co₃O₄ interface. Consequently, the CeO₂/Co₃O₄ interface with the optimal ratio of Ce/Co exhibits high OER activity with an overpotential of only 265 mV at the current density of 10 mA cm^–2, a Tafel slope of 68.1 mV dec^–1, and long-term durability in an alkaline medium.

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水氧化中ceo2诱导的界面Co2+八面体位和氧空位

电催化析氧反应(OER)是电化学能量转换和存储的关键过程。含钴尖晶石氧化物是很有前途的OER候选材料，但由于尖晶石结构的高稳定性和可逆性，在OER过程中存在阳离子缺乏的问题。本文通过内置p-n异质结将催化活性不强的CeO2与尖晶石结构的Co3O4 (CeO2/Co3O4)结合。强耦合的p-n异质结界面使得界面电荷从CeO2快速转移到Co3O4，从而导致高浓度的氧空位和CeO2/Co3O4界面上Co3+(Oh)的还原生成Co2+八面体(Co2+(Oh))位。因此，具有最佳Ce/Co比的CeO2/Co3O4界面具有较高的OER活性，在电流密度为10 mA cm-2时过电位仅为265 mV, Tafel斜率为68.1 mV dec1，并且在碱性介质中具有长期耐用性。

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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.