The development of inexpensive, active, and robust nonprecious metal electrocatalysts toward the oxygen evolution reaction (OER) in acid media is highly imperative for renewable energy conversion techniques, yet greatly challenging. Inspired by the vanadium-containing oxygen-fixing enzymes in haloperoxidase in nature, herein, the atomically dispersed V sites anchored on N-doped multichannel carbon nanofibers (designated as V@NMCNFs hereafter) are rationally designed as high-efficiency electrocatalyst for the acidic OER. Substantial characterizations validate that the local coordination microenvironment of the V site is identified as an asymmetrical penta-coordinated V-O₂N₃ moiety with axial VO coordination, which is further theoretically substantiated as an energetically favorable configuration with a reduced OER energy barrier by the density functional theory calculations. Consequently, the well-dispersed isolated V-O₂N₃ sites with exceptional intrinsic activity and unique nano-architecture furnish the well-designed V@NMCNFs with distinguished OER performance in a 0.5 m H₂SO₄ electrolyte, as reflected by the ultralow overpotential of 196 mV at 10 mA cm⁻² and remarkable long-term electrochemical durability, representing one of the most impressive nonprecious OER electrocatalysts to date. The synthetic methodology for SAC preparation and concept of electronic regulation proposed in this work offer perspectives to aid the design of other functional SAC systems with regulated coordination environments for efficient electrocatalysis.

中文翻译：

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多通道碳纳米纤维上具有轴向 V2O 配位的原子分散 V-O2N3 位点可在酸性介质中实现优异的电催化析氧

对于可再生能源转换技术而言，针对酸性介质中的析氧反应 (OER) 开发廉价、活性和稳健的非贵金属电催化剂是非常必要的，但也极具挑战性。受自然界中卤过氧化物酶中含钒固氧酶的启发，本文合理设计了锚定在 N 掺杂多通道碳纳米纤维（以下称为 V@NMCNFs）上的原子分散 V 位点作为酸性 OER 的高效电催化剂. 大量表征证实，V 位点的局部配位微环境被确定为具有轴向 V 的不对称五配位 VO ₂ N _3部分O 配位，通过密度泛函理论计算进一步在理论上证实为能量有利的配置，具有降低的 OER 能垒。因此，分散良好的孤立 VO ₂ N ₃位点具有出色的本征活性和独特的纳米结构，为精心设计的 V@NMCNF 提供了在 0.5  m H ₂ SO ₄电解质中具有出色的 OER 性能，如超低过电势所反映的10 毫安厘米时为 196 毫伏^-2以及卓越的长期电化学耐久性，是迄今为止最令人印象深刻的非贵金属 OER 电催化剂之一。这项工作中提出的 SAC 制备合成方法和电子调节概念为帮助设计其他具有调节协调环境的功能性 SAC 系统提供了视角，以实现高效电催化。