Bimetallic Ni <sub>3</sub> Fe/Ni <sub>2</sub> Fe <sub>2</sub> N Catalyst With Optimized <i>d</i> ‐Band Center for High‐Efficiency Lithium–Sulfur Batteries
Abstract
ABSTRACT Lithium–sulfur batteries (LSBs) face significant challenges for practical application, primarily due to the sluggish reaction kinetics and pronounced shuttle effect of lithium polysulfides (LiPSs). This study proposes a synergistic strategy involving doping engineering and controlled nitridation‐induced electronic state modulation to fabricate a Ni 3 Fe/Ni 2 Fe 2 N composite as an efficient sulfur host material. This rational design integrates the strong catalytic activity of the metal alloy (Ni 3 Fe) with the high electrical conductivity of the nitride (Ni 2 Fe 2 N), enabling effective anchoring and conversion of polysulfides. Density functional theory (DFT) calculations and analysis results of XAFS and XPS confirm that an upshifted d‐ band center and modulated electronic states significantly enhance reaction kinetics and catalytic activity. In situ Raman spectroscopy and DRT analysis directly demonstrate the exceptional capability of the material to suppress the polysulfide shuttle effect. The battery exhibits remarkable cycling stability, achieving 1000 cycles with an ultralow decay rate of 0.045% per cycle. The outstanding performance is retained even under conditions as harsh as a high sulfur loading (4.3 mg cm −2 ) and low temperature (−10°C). This work not only presents a high‐performance catalyst but also provides new insights into the design of LSB catalysts via electronic state modulation.
Article Details
Authors (15)
Xiuyun Fan
Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical Engineering Liaocheng University Liaocheng P. R. China
Xiyu He
Key Laboratory of Colloid and Interface Chemistry (Ministry of Education) School of Chemistry and Chemical Engineering Shandong University Jinan China
Bin Wang
Lingtong Kong
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China
Muhammad Mamoor
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China
Yueyue Kong
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China
Dedong Wang
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China
Lu Wang
Guangmeng Qu
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China
Zhongxin Jing
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China
MingYu Dou
Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Chemistry and Chemical Engineering Liaocheng University Liaocheng P. R. China
Fengbo Wang
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China
Jianmin Dou
Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology School of Energy Science and Technology Liaocheng University Liaocheng, Shandong China
Pengtu Zhang
School of Chemical Engineering Shandong Institute of Petroleum and Chemical Technology Dongying China
Liqiang Xu
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Material, Shandong University, Jinan 250100, China