Gao Nan, Li Chenyu, Xue Yanjie, Wang Yunpeng, Ma Haitao
School of Materials Science and Engineering, Dalian University of Technology, Dalian 116024, China.
School of Materials Science and Engineering, Dalian University of Technology, Dalian 116024, China.
J Colloid Interface Sci. 2025 Jan 15;678(Pt B):693-703. doi: 10.1016/j.jcis.2024.09.062. Epub 2024 Sep 7.
This paper introduced a novel continuous electrochemical synthesis strategy to address the challenges of slow ion/electron transport rates and low electrode reaction efficiency in Sn-based electrode materials. This approach leveraged the induction and confinement of bubble templates to assist atoms deposition, generating micron-sized tin skeletons. Subsequently, these skeletons were transformed into a secondary nanoporous structure through dissolution-deposition etching effects. From liquid-phase ions to metal skeletons to porous oxides, the sequential material transformations realized the innovative design of three-dimensional (3D) hierarchical structures. This strategy ingeniously exploited the diffusion advantages of the electrolyte in the micro-nano hierarchical structure to achieve the diffusion enhancement of ions, thus solving the "dead surface" problem in the energy storage process. This study revealed the thermodynamic and kinetic feasibility of the constructed 3D micro-nano hierarchical structure through electrochemical evaluations and theoretical calculations, and elucidated the constitutive relationship in which the electrochemical performance of the electrode materials was enhanced with decreasing pore size. In addition, design optimization of pore structures and modelling exploration of pore size limit values were conducted based on density functional theory (DFT) simulations. These simulations demonstrated the advantages of hierarchical structures with controllable pore sizes in facilitating electrolyte ion diffusion, predicting an optimal pore size of 55 μm for 3D hierarchical porous SnO electrodes. The integration of this innovative structural design with simulation insights offered significant implications for enhancing the sluggish electrode reaction kinetics of metal oxide electrode materials, advancing the controllable fabrication of high-performance energy storage devices.
本文介绍了一种新型的连续电化学合成策略，以应对锡基电极材料中离子/电子传输速率缓慢和电极反应效率低下的挑战。该方法利用气泡模板的诱导和限制作用来辅助原子沉积，生成微米级的锡骨架。随后，通过溶解-沉积蚀刻效应将这些骨架转变为二次纳米多孔结构。从液相离子到金属骨架再到多孔氧化物，材料的依次转变实现了三维（3D）分级结构的创新设计。该策略巧妙地利用了电解质在微纳分级结构中的扩散优势，实现了离子扩散增强，从而解决了储能过程中的“死表面”问题。本研究通过电化学评估和理论计算揭示了构建的3D微纳分级结构的热力学和动力学可行性，并阐明了电极材料的电化学性能随孔径减小而增强的本构关系。此外，基于密度泛函理论（DFT）模拟进行了孔结构的设计优化和孔径极限值的建模探索。这些模拟证明了孔径可控的分级结构在促进电解质离子扩散方面的优势，预测3D分级多孔SnO电极的最佳孔径为55μm。这种创新的结构设计与模拟见解的结合，对改善金属氧化物电极材料迟缓的电极反应动力学、推动高性能储能器件的可控制造具有重要意义。
