- Guo, Wei;
- Dun, Chaochao;
- Marcus, Matthew A;
- Venturi, Victor;
- Gainsforth, Zack;
- Yang, Feipeng;
- Feng, Xuefei;
- Viswanathan, Venkatasubramanian;
- Urban, Jeffrey J;
- Yu, Chang;
- Zhang, Qiuyu;
- Guo, Jinghua;
- Qiu, Jieshan
The past decade has witnessed the development of layered-hydroxide-based self-supporting electrodes, but the low active mass ratio impedes its all-around energy-storage applications. Herein, the intrinsic limit of layered hydroxides is broken by engineering F-substituted β-Ni(OH)2 (Ni-F-OH) plates with a sub-micrometer thickness (over 700 nm), producing a superhigh mass loading of 29.8 mg cm-2 on the carbon substrate. Theoretical calculation and X-ray absorption spectroscopy analysis demonstrate that Ni-F-OH shares the β-Ni(OH)2 -like structure with slightly tuned lattice parameters. More interestingly, the synergy modulation of NH4 + and F- is found to serve as the key enabler to tailor these sub-micrometer-thickness 2D plates thanks to the modification effects on the (001) plane surface energy and local OH- concentration. Guided by this mechanism, the superstructures of bimetallic hydroxides and their derivatives are further developed, revealing they are a versatile family with great promise. The tailored ultrathick phosphide superstructure achieves a superhigh specific capacity of 7144 mC cm-2 and a superior rate capability (79% at 50 mA cm-2 ). This work highlights a multiscale understanding of how exceptional structure modulation happens in low-dimensional layered materials. The as-built unique methodology and mechanisms will boost the development of advanced materials to better meet future energy demands.