Li Linlin, Huang Aoming, Jiang Hongcheng, Li Yan, Pan Xiansong, Chen Tsung-Yi, Chen Han-Yi, Peng Shengjie
College of Materials Science and Technology, Nanjing University of Aeronautics and Astronautics, Nanjing, 210016, China.
Department of Materials Science and Engineering, National Tsing Hua University, Taiwan, 30013, China.
Angew Chem Int Ed Engl. 2024 Nov 4;63(45):e202412077. doi: 10.1002/anie.202412077. Epub 2024 Sep 24.
Sub-nanoclusters with ultra-small particle sizes are particularly significant to create advanced energy storage materials. Herein, Sn sub-nanoclusters encapsulated in nitrogen-doped multichannel carbon matrix (denoted as Sn-SCs@MCNF) are designed by a facile and controllable route as flexible anode for high-performance potassium ion batteries (PIBs). The uniformly dispersed Sn sub-nanoclusters in multichannel carbon matrix can be precisely identified, which ensure us to clarify the size influence on the electrochemical performance. The sub-nanoscale effect of Sn-SCs@MCNF restrains electrode pulverization and enhances the K diffusion kinetics, leading to the superior cycling stability and rate performance. As freestanding anode in PIBs, Sn-SCs@MCNF manifests superior K storage properties, such as exceptional cycling stability ( around 331 mAh g after 150 cycles at 100 mA g) and rate capability. Especially, the Sn-SCs@MCNF||KFe[Fe(CN)] full cell demonstrates impressive reversible capacity of around 167 mAh g at 0.4 A g even after 200 cycles. Theoretical calculations clarify that the ultrafine Sn sub-nanoclusters are beneficial for electron transfer and contribute to the lower energy barriers of the intermediates, thereby resulting in promising electrochemical performance. Comprehensive investigation for the intrinsic K storage process of Sn-SCs@MCNF is revealed by in situ analysis. This work provides vital guidance to design sub-nanoscale functional materials for high-performance energy-storage devices.
具有超小粒径的亚纳米团簇对于制备先进的储能材料尤为重要。在此，通过一种简便且可控的方法设计出封装在氮掺杂多通道碳基质中的锡亚纳米团簇（表示为Sn-SCs@MCNF），作为高性能钾离子电池（PIB）的柔性负极。可以精确识别多通道碳基质中均匀分散的锡亚纳米团簇，这使我们能够阐明尺寸对电化学性能的影响。Sn-SCs@MCNF的亚纳米级效应抑制了电极粉化并增强了钾扩散动力学，从而带来卓越的循环稳定性和倍率性能。作为PIB中的独立负极，Sn-SCs@MCNF表现出优异的钾存储性能，如出色的循环稳定性（在100 mA g下150次循环后约为331 mAh g）和倍率能力。特别是，Sn-SCs@MCNF||KFe[Fe(CN)]全电池即使在200次循环后，在0.4 A g下仍表现出约167 mAh g的令人印象深刻的可逆容量。理论计算表明，超细锡亚纳米团簇有利于电子转移，并有助于降低中间体的能垒，从而产生有前景的电化学性能。通过原位分析揭示了对Sn-SCs@MCNF固有钾存储过程的全面研究。这项工作为设计用于高性能储能装置的亚纳米级功能材料提供了重要指导。
