用于电化学水氧化的尖晶石氧化物的表面重构策略。
Navigating surface reconstruction of spinel oxides for electrochemical water oxidation.
机构信息
Faculty of Materials Science and Energy Engineering/Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055, P. R. China.
Shenzhen Key Laboratory of Energy Materials for Carbon Neutrality, Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, Shenzhen, 518055, P. R. China.
出版信息
Nat Commun. 2023 Apr 28;14(1):2467. doi: 10.1038/s41467-023-38017-3.
Understanding and mastering the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity. Herein, we demonstrate that surface reconstruction of spinel oxides originates from the metal-oxygen covalency polarity in the M-O-M backbone. A stronger M-O covalency relative to M-O covalency is found beneficial for a more thorough reconstruction towards oxyhydroxides. The structure-reconstruction relationship allows precise prediction of the reconstruction ability of spinel pre-catalysts, based on which the reconstruction degree towards the in situ generated oxyhydroxides can be controlled. The investigations of oxyhydroxides generated from spinel pre-catalysts with the same reconstruction ability provide guidelines to navigate the cation selection in spinel pre-catalysts design. This work reveals the fundamentals for manipulating the surface reconstruction of spinel pre-catalysts for water oxidation.
理解和掌握水氧化电催化剂的结构演变，为精细调整其催化活性奠定了基础。在此，我们证明尖晶石氧化物的表面重构源于 M-O-M 骨架中的金属-氧共价极性。与 M-O 共价相比，更强的 M-O 共价有利于更彻底的向氧氢氧化物的重构。结构-重构关系允许对尖晶石前催化剂的重构能力进行精确预测，在此基础上可以控制其对原位生成的氧氢氧化物的重构程度。对具有相同重构能力的尖晶石前催化剂生成的氧氢氧化物的研究为在尖晶石前催化剂设计中进行阳离子选择提供了指导。这项工作揭示了用于操纵水氧化尖晶石前催化剂表面重构的基本原理。
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