Electronic Spin Alignment within Homologous NiS2/NiSe2 Heterostructures to Promote Sulfur Redox Kinetics in Lithium‐Sulfur Batteries

• DOI: 10.1002/adma.202400810
• Publication Date: 2024-04-03T21:49:24Z
• Authors: Chen Huang; Jing Yu; Chao Yue Zhang; Zhibiao Cui; Jiakun Chen; Wei‐Hong Lai; Yao‐Jie Lei; Bingfei Nan; Xuan Lu; Ren He; Li Gong; Junshan Li; Canhuang Li; Xuede Qi; Qian Xue; Jin Yuan Zhou; Xueqiang Qi; Lluís Balcells; Jordi Arbiol; Andreu Cabot
• Keywords: hollow particle; homologous heterostructure; spin state; Lithium polysulfides; Nickel selenide; 02 engineering and technology; Hollow particle; Lithium-sulfur battery; Homologous heterostructure; lithium polysulfides; Spin state; nickel sulfide; lithium-sulfur battery; Nickel sulfide; 0210 nano-technology; nickel selenide

Abstract The catalytic activation of the Li‐S reaction is fundamental to maximize capacity and stability batteries (LSBs). Current research on catalysts mainly focuses optimizing energy levels promote adsorption conversion, while frequently overlooking electronic spin state influence charge transfer orbital interactions. Here, hollow NiS 2 /NiSe heterostructures encapsulated in a nitrogen‐doped carbon matrix (NiS @NC) are synthesized used as additive sulfur cathodes. heterostructure promotes splitting 3d orbital, driving Ni 3+ transformation from low high spin. This configuration raises level activates state. accelerates optimizes energy, lowering barrier polysulfides conversion. Benefiting these characteristics, LSBs based @NC/S cathodes exhibit initial (1458 mAh·g⁻ 1 at 0.1C), excellent rate capability (572 5C), stable cycling with an average decay only 0.025% per cycle 1C during 500 cycles. Even loadings (6.2 mg·cm⁻ ), capacities 1173 (7.27 mAh·cm⁻ ) measured 0.1C, 1058 retained after 300