Materials Science and Engineering Program & Texas Materials Institute (TMI), The University of Texas at Austin, Austin, TX 78712-1591, USA.
Department of Materials Science and Chemical Engineering, Stony Brook University, Stony Brook, NY 11794, USA.
Angew Chem Int Ed Engl. 2023 Jun 5;62(23):e202300943. doi: 10.1002/anie.202300943. Epub 2023 Apr 5.
Combined synchrotron X-ray nanotomography imaging, cryogenic electron microscopy (cryo-EM) and modeling elucidate how potassium (K) metal-support energetics influence electrodeposit microstructure. Three model supports are employed: O-functionalized carbon cloth (potassiophilic, fully-wetted), non-functionalized cloth and Cu foil (potassiophobic, nonwetted). Nanotomography and focused ion beam (cryo-FIB) cross-sections yield complementary three-dimensional (3D) maps of cycled electrodeposits. Electrodeposit on potassiophobic support is a triphasic sponge, with fibrous dendrites covered by solid electrolyte interphase (SEI) and interspersed with nanopores (sub-10 nm to 100 nm scale). Lage cracks and voids are also a key feature. On potassiophilic support, the deposit is dense and pore-free, with uniform surface and SEI morphology. Mesoscale modeling captures the critical role of substrate-metal interaction on K metal film nucleation and growth, as well as the associated stress state.
联合同步辐射 X 射线纳米断层成像、低温电子显微镜（cryo-EM）和建模阐明了钾（K）金属-载体能量学如何影响电沉积微观结构。采用了三种模型载体：O 功能化碳布（亲钾，完全润湿）、非功能化布和 Cu 箔（疏钾，不润湿）。纳米断层成像和聚焦离子束（cryo-FIB）横截面提供了循环电镀沉积物的互补三维（3D）图谱。疏钾载体上的电沉积是三相海绵状的，纤维状枝晶被固体电解质相间（SEI）覆盖，并散布着纳米孔（亚 10nm 至 100nm 尺度）。大的裂缝和空隙也是一个关键特征。在亲钾载体上，沉积物致密且无孔，表面和 SEI 形态均匀。介观模型捕捉到了基底-金属相互作用对 K 金属膜成核和生长以及相关应力状态的关键作用。
