@article{Li2026, 
author = {Hongyang Li and Jianjun Zhang and Yingrui Ding and Zhanpeng Huang and Pengsen Qian and Fanyang Sun and Huimin Wang and Gaoran Li},
title = {Undercoordination engineering of chromium single-atom catalyst with optimized d-p hybridization for lithium-sulfur batteries},
year = {2026},
journal = {Nano Research},
volume = {19},
number = {1},
pages = {94907915},
keywords = {lithium-sulfur batteries, single-atom catalysts, coordination structure, orbital hybridization, sulfur electrocatalysis},
url = {https://www.sciopen.com/article/10.26599/NR.2025.94907915},
doi = {10.26599/NR.2025.94907915},
abstract = {Sluggish sulfur redox kinetics remain a critical bottleneck in the advancement of high-performance lithium-sulfur batteries (LSBs). Single-atom catalysts (SACs) offer a promising solution to this limitation, particularly when their coordination structures are carefully engineered. Here, we develop a chromium-based SAC featuring a unique undercoordinated CrN3 configuration to boost sulfur electrochemistry. Compared with conventional CrN4, the CrN3 motif lowers 3d orbital occupancy and meanwhile activates the in-plane hybridizations with S 3p orbitals upon interaction with polysulfides, contributing to moderate adsorption strength and reduced energy barriers for bidirectional sulfur conversions. Additionally, the integration of the two-dimensional (2D) porous framework ensures abundant electrochemically active surfaces and efficiently exposed active sites. As a result, CrN3-based cells demonstrate fast and durable sulfur redox reactions, enabling an ultralow capacity decay of 0.0075% per cycle over 1000 cycles and a high-rate capability of 651.9 mAh·g−1 at 5 C. The CrN3 catalyst retains robust catalytic efficiency under demanding conditions, delivering a high areal capacity of 5.53 mAh·cm−2 at high sulfur loading and lean electrolyte. This work establishes a compelling paradigm of SAC coordination engineering for designing advanced sulfur electrocatalysts for next-generation LSBs.}
}