Phase engineering of defective copper selenide toward robust lithium-sulfur batteries

The shuttling of soluble lithium polysulfides (LiPS) and the sluggish Li–S conversion kinetics are two main barriers toward the practical application of lithium–sulfur batteries (LSBs). Herein, we propose the addition of copper selenide nanoparticles at the cathode to trap LiPS and accelerate the Li...

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Detalles Bibliográficos
Autores: Yang, Dawei, Li, Mengyao, Zheng, Xuejiao, Han, Xu, Zhang, Chaoqi, Jacas Biendicho, Jordi|||0000-0001-5981-6168, Llorca Piqué, Jordi|||0000-0002-7447-9582, Wang, Jiaao, Hao, Hongchang, Li, Junshan, Henkelman, Graeme, Arbiol, Jordi, Morante, Joan Ramon, Mitlin, David, Chou, Shu-Lei, Cabot, Andreu
Tipo de recurso: artículo
Fecha de publicación:2022
País:España
Institución:Universitat Politècnica de Catalunya (UPC)
Repositorio:UPCommons. Portal del coneixement obert de la UPC
Idioma:inglés
OAI Identifier:oai:upcommons.upc.edu:2117/382969
Acceso en línea:https://hdl.handle.net/2117/382969
https://dx.doi.org/10.1021/acsnano.2c03788
Access Level:acceso abierto
Palabra clave:Copper selenide
Phase engineering
Copper vacancies
Lithium-sulfur battery
Lithium polysulfide
Àrees temàtiques de la UPC::Enginyeria química
Descripción
Sumario:The shuttling of soluble lithium polysulfides (LiPS) and the sluggish Li–S conversion kinetics are two main barriers toward the practical application of lithium–sulfur batteries (LSBs). Herein, we propose the addition of copper selenide nanoparticles at the cathode to trap LiPS and accelerate the Li–S reaction kinetics. Using both computational and experimental results, we demonstrate the crystal phase and concentration of copper vacancies to control the electronic structure of the copper selenide, its affinity toward LiPS chemisorption, and its electrical conductivity. The adjustment of the defect density also allows for tuning the electrochemically active sites for the catalytic conversion of polysulfide. The optimized S/Cu1.8Se cathode efficiently promotes and stabilizes the sulfur electrochemistry, thus improving significantly the LSB performance, including an outstanding cyclability over 1000 cycles at 3 C with a capacity fading rate of just 0.029% per cycle, a superb rate capability up to 5 C, and a high areal capacity of 6.07 mAh cm–2 under high sulfur loading. Overall, the present work proposes a crystal phase and defect engineering strategy toward fast and durable sulfur electrochemistry, demonstrating great potential in developing practical LSBs.