Affiliation:
1. State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 P. R. China
2. School of Chemical Engineering East China University of Science and Technology Shanghai 200237 China
3. Key Laboratory for Specially Functional Materials and Related Technology of the Ministry of Education East China University of Science and Technology Shanghai 200237 P. R. China
Abstract
AbstractCommercialization 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.
Funder
National Natural Science Foundation of China
Fundamental Research Funds for the Central Universities
Subject
Mechanical Engineering,Mechanics of Materials,General Materials Science