<br>MOF 衍生的磷化钴网络中的氧桥钴-铬原子对作为有效活性位点，在碱性介质中实现协同电催化水分解,Advanced Science

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MOF 衍生的磷化钴网络中的氧桥钴-铬原子对作为有效活性位点，在碱性介质中实现协同电催化水分解
Advanced Science ( IF 14.3 ) Pub Date : 2023-11-23 , DOI: 10.1002/advs.202306678
Zepeng Lv ₁ , Huakui Zhang ₂ , Chenhui Liu ₂ , Shaolong Li ₂ , Jianxun Song ₁ , Jilin He ₁

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电化学水分解为“绿色氢”的产生提供了最有前途的途径。即便如此，提高非贵金属催化剂，特别是双功能电催化剂的电催化性能仍然是一个难题。在此，为了加速氢和氧的析出反应，提出了一种通过MOF介导合成的锚定在磷化钴上的氧桥钴铬（Co-O-Cr）双位点催化剂。利用3d轨道的填充特性和催化活性位点的调制局域电子结构，精心设计的催化剂仅需要1.53 V的外部电压即可在水分解过程中提供20 mA cm ^-2的电流密度来自优异的 HER 和 OER 活性，在 10 mA cm ^-2的电流密度下分别具有 87 和 203 mV 的低过电势。此外，密度泛函理论（DFT）计算被用来阐明机理研究，包括H ₂ O在Co-O-Cr部分表面的加速吸附和解离过程、下移的d带中心、降低的能垒开放教育资源（OER）等。这项工作为优化能量转换的催化活性提供了设计方向。

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Oxygen-Bridged Cobalt–Chromium Atomic Pair in MOF-Derived Cobalt Phosphide Networks as Efficient Active Sites Enabling Synergistic Electrocatalytic Water Splitting in Alkaline Media

Electrochemical water splitting offers a most promising pathway for “green hydrogen” generation. Even so, it remains a struggle to improve the electrocatalytic performance of non-noble metal catalysts, especially bifunctional electrocatalysts. Herein, aiming to accelerate the hydrogen and oxygen evolution reactions, an oxygen-bridged cobalt–chromium (Co-O-Cr) dual-sites catalyst anchored on cobalt phosphide synthesized through MOF-mediation are proposed. By utilizing the filling characteristics of 3d orbitals and modulated local electronic structure of the catalytic active site, the well-designed catalyst requires only an external voltage of 1.53 V to deliver the current density of 20 mA cm⁻² during the process of water splitting apart from the superb HER and OER activity with a low overpotential of 87 and 203 mV at a current density of 10 mA cm⁻², respectively. Moreover, density functional theory (DFT) calculations are utilized to unravel mechanistic investigations, including the accelerated adsorption and dissociation process of H₂O on the Co-O-Cr moiety surface, the down-shifted d-band center, a lowered energy barrier for the OER and so on. This work offers a design direction for optimizing catalytic activity toward energy conversion.

更新日期：2023-11-23

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