Unraveling the effect of local dopant environment on NiO6 octahedron perturbation for enhanced oxygen evolution activity

IF 20.2 1区化学 Q1 CHEMISTRY, PHYSICAL

Applied Catalysis B: Environmental Pub Date : 2023-12-30 DOI:10.1016/j.apcatb.2023.123674

Junchen Yu , Haoyin Zhong , Qi Zhang , Chao Wu , Xin Zhang , Shanlin Li , Yongzhi Zhao , Hang An , Yifan Ma , Zhigen Yu , Shibo Xi , Xiaopeng Wang , Junmin Xue

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Abstract

The oxygen evolution reaction (OER) performance in cation-doped materials often exhibits a volcano-like relationship with dopant concentration. However, the influence of dopant content with its associated local environment on the electronic states of electrocatalysts remains unclear. Herein, V is incorporated into Ni(OH)₂ to study the underlying mechanism. It is revealed that evenly distributed V can effectively perturb the NiO₆ octahedron, leading to strong e_g * band broadening and more electronic states around the Fermi level. This phenomenon significantly enhances the electron transfer from electrocatalysts to external circuits. Conversely, the aggregation of V at higher dopant concentration exerts weaker influence on perturbing the NiO₆ octahedron. As a result of balance between V doping and aggregation, Ni_0.95V_0.05OOH, with the strongest NiO₆ octahedron distortion, effectuating a remarkably low overpotential of 258 mV at 10 mA cm⁻². Furthermore, such a structure-activity relationship is also extended to Fe-doped Ni(OH)₂, affirming the universality of the proposed mechanism.

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揭示局部掺杂环境对增强氧进化活性的 NiO6 八面体扰动的影响

阳离子掺杂材料的氧进化反应（OER）性能通常与掺杂剂浓度呈火山状关系。然而，掺杂剂含量及其相关局部环境对电催化剂电子状态的影响仍不清楚。在此，我们在 Ni(OH)2 中掺入了 V，以研究其基本机制。研究发现，均匀分布的 V 可以有效地扰动 NiO6 八面体，导致强烈的 eg ⁎ 带宽和费米水平附近更多的电子状态。这种现象大大增强了电子从电催化剂向外部电路的转移。相反，掺杂浓度较高时，V 的聚集对 NiO6 八面体的扰动影响较弱。由于 V 掺杂和聚集之间的平衡，Ni0.95V0.05OOH 的 NiO6 八面体畸变最强，在 10 mA cm-2 的条件下可产生 258 mV 的极低过电位。此外，这种结构-活性关系还扩展到了掺铁的 Ni(OH)2，从而证实了所提出机制的普遍性。

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来源期刊

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.