School of Chemistry, South China Normal University, Guangzhou, 510006, China.
Henan Key Laboratory of Crystalline Molecular Functional Materials, Henan International Joint Laboratory of Tumor Theranostical Cluster Materials, Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China.
Nat Commun. 2023 Mar 31;14(1):1792. doi: 10.1038/s41467-023-37530-9.
Catalysts capable of electrochemical overall water splitting in acidic, neutral, and alkaline solution are important materials. This work develops bifunctional catalysts with single atom active sites through a pyrolysis-free route. Starting with a conjugated framework containing Fe sites, the addition of Ni atoms is used to weaken the adsorption of electrochemically generated intermediates, thus leading to more optimized energy level sand enhanced catalytic performance. The pyrolysis-free synthesis also ensured the formation of well-defined active sites within the framework structure, providing ideal platforms to understand the catalytic processes. The as-prepared catalyst exhibits efficient catalytic capability for electrochemical water splitting in both acidic and alkaline electrolytes. At a current density of 10 mA cm, the overpotential for hydrogen evolution and oxygen evolution is 23/201 mV and 42/194 mV in 0.5 M HSO and 1 M KOH, respectively. Our work not only develops a route towards efficient catalysts applicable across a wide range of pH values, it also provides a successful showcase of a model catalyst for in-depth mechanistic insight into electrochemical water splitting.
能够在酸性、中性和碱性溶液中进行电化学全水分解的催化剂是重要的材料。这项工作通过一种无热解的方法开发了具有单原子活性位的双功能催化剂。从含有 Fe 位点的共轭框架开始，添加 Ni 原子用于削弱电化学生成中间体的吸附，从而导致更优化的能级和增强的催化性能。无热解合成还确保了在框架结构内形成了明确定义的活性位，为理解催化过程提供了理想的平台。所制备的催化剂在酸性和碱性电解质中都表现出高效的电化学水分解催化能力。在 10 mA cm 的电流密度下，在 0.5 M HSO 和 1 M KOH 中，析氢和析氧的过电位分别为 23/201 mV 和 42/194 mV。我们的工作不仅开发了一种适用于宽 pH 值范围的高效催化剂的途径，还为深入了解电化学水分解的机制提供了一个成功的模型催化剂范例。
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