Yang Xue, Sun Xiaoning, Qi Jindi, Zhang Jiaqi, Zheng Xinqi, Zhang Xiaodong, Lei Fengcai, Sun Xu, Tang Bo, Xie Junfeng
College of Chemistry, Chemical Engineering and Materials Science, Key Laboratory of Molecular and Nano Probes of Ministry of Education, Collaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of Shandong, Institute of Molecular and Nano Science, Shandong Normal University, Jinan, Shandong, 250014, PR China.
Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, Anhui, 230026, PR China.
J Colloid Interface Sci. 2025 Jan;677(Pt B):406-416. doi: 10.1016/j.jcis.2024.08.055. Epub 2024 Aug 10.
Exploring advanced electrocatalyst for the oxygen evolution reaction (OER) is of great importance in pursuing efficient and sustainable hydrogen production via electrolytic water splitting. Considering the structure-activity-stability relationship for designing advanced OER catalysts, two-dimensional (2D) porous catalyst with single crystallinity is deemed to be an ideal platform which could simultaneously endow enriched active sites, facile mass and charge transport ability as well as robust structural stability. Herein, we proposed a facile 2D confined topotactic phase transformation approach, which realizes the fabrication of highly porous single-crystalline CoO nanosheets with in-situ surface modification of amorphous Co-Pi active species. Benefitted from the highly exposed undercoordinated cobalt sites, facilitated mass transport and facile 2D charge transfer pathway, the Co-Pi/CoO hybrid porous nanosheets display enhanced OER activity with obvious pre-oxidation-induced activation. In addition, the operational stability was significantly improved owing to the strengthened structural stability which effectively buffers the internal strains and avoids the structural collapse during the electrochemical process. This work proposed a facile and mild method for the synthesis of amorphous/single-crystalline hybrid porous materials, and the achievement of synergistic modulation of active site density and charge transfer ability via targeted microstructural construction will shed light on catalyst design in the future.
探索用于析氧反应(OER)的先进电催化剂对于通过电解水分解实现高效且可持续的制氢至关重要。考虑到设计先进OER催化剂的结构-活性-稳定性关系,具有单晶性的二维(2D)多孔催化剂被认为是一个理想的平台,它可以同时赋予丰富的活性位点、便捷的质量和电荷传输能力以及强大的结构稳定性。在此,我们提出了一种简便的二维受限拓扑相变方法,该方法实现了具有非晶态Co-Pi活性物种原位表面改性的高度多孔单晶CoO纳米片的制备。受益于高度暴露的低配位钴位点、促进的质量传输和便捷的二维电荷转移途径,Co-Pi/CoO混合多孔纳米片表现出增强的OER活性,并具有明显的预氧化诱导活化作用。此外,由于结构稳定性增强,有效缓冲了内部应变并避免了电化学过程中的结构坍塌,其操作稳定性得到了显著提高。这项工作提出了一种简便温和的方法来合成非晶态/单晶混合多孔材料,并且通过有针对性的微观结构构建实现活性位点密度和电荷转移能力的协同调制将为未来的催化剂设计提供思路。