Interfacial Charge‐Transfer Kinetics Regulate Na <sub>2</sub> S Deposition by Recycled V Single‐Atom Catalysts for Durable Na–S Batteries
Abstract
ABSTRACT Na 2 S, as the terminal discharge product of room‐temperature sodium–sulfur (Na–S) batteries, is electronically and ionically insulating. When it deposits as a compact film on the cathode, the cathode will become passivated, hindering electron transport and inhibiting further sulfur conversion reactions. Existing catalyst strategies promote the formation of Na 2 S thermodynamically by enhancing polysulfide adsorption, but this does not address the kinetics passivation issue. Here, we adopt the exchange current density ( j 0 ) as a kinetic descriptor of the Na 2 S nucleation mode. Finite‐element simulations reveal that increasing j 0 drives the nucleation pathway from progressive to instantaneous nucleation. The deposit morphology then evolves from a compact passivating film to uniformly dispersed nanoparticles, and ion and electron transport channels are preserved. This pathway prevents Na 2 S aggregation and electrode passivation, maintaining electrochemical activity at deep discharge. Guided by this kinetic insight, nitrogen‐doped porous carbon‐supported V single‐atom catalysts (NPC‐V SACs) with high apparent j 0 were fabricated, and instantaneous Na 2 S nucleation was achieved on their surfaces. The resulting Na–S battery retains 976.3 mAh g −1 after 200 cycles at 0.2 A g −1 , with a decay rate of only 0.08% per cycle. This work establishes a kinetic design perspective for regulating Na 2 S nucleation in durable Na–S batteries.
Article Details
Authors (17)
Guangxuan Wu
School of Energy (National Industry‐Education Platform for Energy Storage) School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials Tianjin University Tianjin People's Republic of China
Zhihui Zhou
State Key Laboratory of Physical Chemistry of Solid Surfaces, Key Laboratory for Chemical Biology of Fujian Province, The MOE Key Laboratory of Spectrochemical Analysis and Instrumentation, Department of Chemical Biology, College of Chemistry and Chemical Engineering, State Key Laboratory of Vaccines for Infectious Diseases, Fujian Provincial Key Laboratory of Innovative Drug Target Research, School of Pharmaceutical Sciences, School of Life Sciences, Faculty of Medicine and Life Sciences
Yeteng Lu
School of Energy (National Industry‐Education Platform for Energy Storage) School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials Tianjin University Tianjin People's Republic of China
Zhoujie Lao
Yuhan Ma
Nan Xiao
School of Energy (National Industry‐Education Platform for Energy Storage) School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials Tianjin University Tianjin People's Republic of China
Ning Wang
Congqin Zheng
Suzhou Nuclear Power Research Institute Jiangsu People's Republic of China
Shuiyong Wang
Suzhou Nuclear Power Research Institute Jiangsu People's Republic of China
Enzuo Liu
School of Materials Science and Engineering and Tianjin Key Laboratory of Composites and Functional Materials
Xiang Zhang
Chunsheng Shi
School of Energy (National Industry‐Education Platform for Energy Storage) School of Materials Science and Engineering and Tianjin Key Laboratory of Composite and Functional Materials Tianjin University Tianjin People's Republic of China
Chunnian He
Wenbin Hu
Naiqin Zhao
Wanxiang Zhao
Suzhou Nuclear Power Research Institute Jiangsu People's Republic of China
Biao Chen
Department of Chemical Physics, School of Chemistry and Materials Science, Hefei National Research Center for Physical Sciences at the Microscale