文献类型：期刊文献

英文题名：Enhanced Electron Delocalization within Coherent Nano-Heterocrystal Ensembles for Optimizing Polysulfide Conversion in High-Energy-Density Li-S Batteries

作者：Zhao, Zhiqiang[1];Pan, Yukun[1];Yi, Shan[1];Su, Zhe[1];Chen, Hongli[1];Huang, Yanan[1];Niu, Bo[1];Long, Donghui[1,2,3];Zhang, Yayun[1,2,3]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Key Lab Specially Funct Mat & Related Technol, Minist Educ, Shanghai 200237, Peoples R China

年份：2024

卷号：36

期号：13

外文期刊名：ADVANCED MATERIALS

收录：;EI(收录号：20240115302544);WOS:【SCI-EXPANDED(收录号:WOS:001132896400001)】；

基金：Z.Z. and Y.P. contributed equally to the work. This work was financially supported by National Natural Science Foundation of China (No. 22008073, No. 21878091, No. 22078100, No. 52102098), Shanghai Sailing Program (No. 20YF1410600), Fundamental Research Funds for the Central Universities, and Shanghai Talent Development Fund (2021021). The authors would like to thank Shiyanjia Lab () for the XPS analysis.

语种：英文

外文关键词：catalytic conversion; coherent nano-heterocrystal; electron delocalization; lithium-sulfur battery; polysulfide adsorption

摘要：Commercialization of high energy density Lithium-Sulfur (Li-S) batteries is impeded by challenges such as polysulfide shuttling, sluggish reaction kinetics, and limited Li+ transport. Herein, a jigsaw-inspired catalyst design strategy that involves in situ assembly of coherent nano-heterocrystal ensembles (CNEs) to stabilize high-activity crystal facets, enhance electron delocalization, and reduce associated energy barriers is proposed. On the catalyst surface, the stabilized high-activity facets induce polysulfide aggregation. Simultaneously, the surrounded surface facets with enhanced activity promote Li2S deposition and Li+ diffusion, synergistically facilitating continuous and efficient sulfur redox. Experimental and DFT computations results reveal that the dual-component hetero-facet design alters the coordination of Nb atoms, enabling the redistribution of 3D orbital electrons at the Nb center and promoting d-p hybridization with sulfur. The CNE, based on energy level gradient and lattice matching, endows maximum electron transfer to catalysts and establishes smooth pathways for ion diffusion. Encouragingly, the NbN-NbC-based pouch battery delivers a Weight energy density of 357 Wh kg-1, thereby demonstrating the practical application value of CNEs. This work unveils a novel paradigm for designing high-performance catalysts, which has the potential to shape future research on electrocatalysts for energy storage applications. Construction of coherent nano-heterocrystal ensembles (CNEs) aims to achieve enhanced electron delocalization, ensure stability of high-activity crystal facets, improve catalytic efficiency, and lower the energy barriers for sulfur species conversion. The synergistic optimization of multi-reactive facets facilitates efficient conversion of polysulfides, offering a new approach for the development of high-energy-density and long-life Li-S batteries.image