利用电子再分布策略抑制 CeO2/NiCo2S4 异质结构中硫的浸出,实现高效氧气进化

IF 20.2 1区 化学 Q1 CHEMISTRY, PHYSICAL Applied Catalysis B: Environmental Pub Date : 2023-12-23 DOI:10.1016/j.apcatb.2023.123659
Peng Wang, Xiao Han, Ping Bai, Jiarong Mu, Yihua Zhao, Jinlu He, Yiguo Su
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引用次数: 0

摘要

开发高活性、高稳定性的过渡金属瑀(TMCs)电催化剂以实现氧进化反应(OER)仍然是一项挑战。在此,我们报告了一种电子再分配机制,该机制涉及 CeO2/NiCo2S4 异质结构中电子从 Ce 转移到 Ni 和 Co 所引发的金属-硫(M-S)键稳定,从而有效抑制了 OER 过程中硫从 CeO2/NiCo2S4 中的浸出。此外,调制良好的异质界面使氧中间产物具有最佳的吸附亲和力,降低了 OER 的能垒。因此,CeO2/NiCo2S4 表现出卓越的 OER 活性,在 10 mA-cm-2 和 100 mA-cm-2 条件下,过电位分别为 146 mV 和 271 mV。更重要的是,CeO2/NiCo2S4 在 500 mA-cm-2 下具有超过 200 小时的出色耐久性,超过了单个 NiCo2S4 和大多数已报道的基于 TMCs 的电催化剂。这项工作为实现基于 TMCs 的 OER 电催化剂在高活性和稳定性方面的良好兼容性提供了新的见解。
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Utilizing an electron redistribution strategy to inhibit the leaching of sulfur from CeO2/NiCo2S4 heterostructure for high-efficiency oxygen evolution

Developing highly active and robust transition metal chalcogenides (TMCs) electrocatalysts toward oxygen evolution reaction (OER) remains a challenge. Herein, we report an electron redistribution mechanism that involves the metal-sulfur (M-S) bond stabilization triggered by electron transfer from Ce to Ni and Co in CeO2/NiCo2S4 heterostructure, thereby effectively inhibiting the leaching of sulfur from CeO2/NiCo2S4 during the OER process. Moreover, the well-modulated heterogeneous interface enables optimal adsorption affinity for oxygen intermediates and reduces the energy barrier of OER. As a result, CeO2/NiCo2S4 exhibits superior OER activity with ultralow overpotentials of 146 and 271 mV at 10 and 100 mA cm−2, respectively. More importantly, CeO2/NiCo2S4 possesses excellent durability for over 200 h at 500 mA cm−2, surpassing individual NiCo2S4 and most of the reported TMCs-based electrocatalysts. This work provides new insights for achieving good compatibility of TMCs-based OER electrocatalysts in terms of high activity and stability.

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来源期刊
Applied Catalysis B: Environmental
Applied Catalysis B: Environmental 环境科学-工程:化工
CiteScore
38.60
自引率
6.30%
发文量
1117
审稿时长
24 days
期刊介绍: Applied Catalysis B: Environment and Energy (formerly Applied Catalysis B: Environmental) is a journal that focuses on the transition towards cleaner and more sustainable energy sources. The journal's publications cover a wide range of topics, including: 1.Catalytic elimination of environmental pollutants such as nitrogen oxides, carbon monoxide, sulfur compounds, chlorinated and other organic compounds, and soot emitted from stationary or mobile sources. 2.Basic understanding of catalysts used in environmental pollution abatement, particularly in industrial processes. 3.All aspects of preparation, characterization, activation, deactivation, and regeneration of novel and commercially applicable environmental catalysts. 4.New catalytic routes and processes for the production of clean energy, such as hydrogen generation via catalytic fuel processing, and new catalysts and electrocatalysts for fuel cells. 5.Catalytic reactions that convert wastes into useful products. 6.Clean manufacturing techniques that replace toxic chemicals with environmentally friendly catalysts. 7.Scientific aspects of photocatalytic processes and a basic understanding of photocatalysts as applied to environmental problems. 8.New catalytic combustion technologies and catalysts. 9.New catalytic non-enzymatic transformations of biomass components. The journal is abstracted and indexed in API Abstracts, Research Alert, Chemical Abstracts, Web of Science, Theoretical Chemical Engineering Abstracts, Engineering, Technology & Applied Sciences, and others.
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