학술논문
Electronic Spin Alignment within Homologous NiS 2 /NiSe 2 Heterostructures to Promote Sulfur Redox Kinetics in Lithium-Sulfur Batteries.
Document Type
Academic Journal
Author
Huang C; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; Department of Chemistry, University of Barcelona, Barcelona, 08028, Spain.; Yu J; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, Barcelona, Catalonia, 08193, Spain.; Zhang CY; Key Laboratory for Magnetism and Magnetic Materials of the Ministry of Education & School of Physical Science & Technology, Lanzhou University, Lanzhou, 730000, China.; Cui Z; School of Chemistry, South China Normal University, Guangzhou, 510006, P. R. China.; Chen J; Analysis and Testing Center, South China Normal University, Guangzhou, 510006, China.; Lai WH; Institute for Superconducting and Electronic Materials, Australian Institute of Innovative Materials, Innovation Campus, University of Wollongong, Wollongong, NSW, 2500, Australia.; Lei YJ; Institute for Superconducting and Electronic Materials, Australian Institute of Innovative Materials, Innovation Campus, University of Wollongong, Wollongong, NSW, 2500, Australia.; Nan B; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; Lu X; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; He R; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; Gong L; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; Department of Chemistry, University of Barcelona, Barcelona, 08028, Spain.; Li J; Institute for Advanced Study, Chengdu University, Chengdu, 610106, China.; Li C; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; Department of Chemistry, University of Barcelona, Barcelona, 08028, Spain.; Qi X; College of Chemistry and Chemical Engineering, Chongqing University of Technology, Chongqing, 400054, China.; Xue Q; College of Chemistry and Chemical Engineering, Chongqing University of Technology, Chongqing, 400054, China.; Zhou JY; Key Laboratory for Magnetism and Magnetic Materials of the Ministry of Education & School of Physical Science & Technology, Lanzhou University, Lanzhou, 730000, China.; Qi X; College of Chemistry and Chemical Engineering, Chongqing University of Technology, Chongqing, 400054, China.; Balcells L; Institut de Ciència de Materials de Barcelona, Campus de la UAB, Bellaterra, Catalonia, 08193, Spain.; Arbiol J; Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Campus UAB, Bellaterra, Barcelona, Catalonia, 08193, Spain.; ICREA Pg. Lluis Companys, Barcelona, Catalonia, 08010, Spain.; Cabot A; Catalonia Institute for Energy Research-IREC, Sant Adrià de Besòs, Barcelona, 08930, Spain.; ICREA Pg. Lluis Companys, Barcelona, Catalonia, 08010, Spain.
Source
Publisher: Wiley-VCH Country of Publication: Germany NLM ID: 9885358 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1521-4095 (Electronic) Linking ISSN: 09359648 NLM ISO Abbreviation: Adv Mater Subsets: MEDLINE
Subject
Language
English
Abstract
The catalytic activation of the Li-S reaction is fundamental to maximize the capacity and stability of Li-S batteries (LSBs). Current research on Li-S catalysts mainly focuses on optimizing the energy levels to promote adsorption and catalytic conversion, while frequently overlooking the electronic spin state influence on charge transfer and orbital interactions. Here, hollow NiS 2 /NiSe 2 heterostructures encapsulated in a nitrogen-doped carbon matrix (NiS 2 /NiSe 2 @NC) are synthesized and used as a catalytic additive in sulfur cathodes. The NiS 2 /NiSe 2 heterostructure promotes the spin splitting of the 3d orbital, driving the Ni 3+ transformation from low to high spin. This high spin configuration raises the electronic energy level and activates the electronic state. This accelerates the charge transfer and optimizes the adsorption energy, lowering the reaction energy barrier of the polysulfides conversion. Benefiting from these characteristics, LSBs based on NiS 2 /NiSe 2 @NC/S cathodes exhibit high initial capacity (1458 mAh·g⁻ 1 at 0.1C), excellent rate capability (572 mAh·g⁻ 1 at 5C), and stable cycling with an average capacity decay rate of only 0.025% per cycle at 1C during 500 cycles. Even at high sulfur loadings (6.2 mg·cm⁻ 2 ), high initial capacities of 1173 mAh·g⁻ 1 (7.27 mAh·cm⁻ 2 ) are measured at 0.1C, and 1058 mAh·g⁻ 1 is retained after 300 cycles.
(© 2024 Wiley‐VCH GmbH.)
(© 2024 Wiley‐VCH GmbH.)