A High Conductivity 1D pi-d Conjugated Metal-Organic Framework with Efficient Polysulfide Trapping-Diffusion-Catalysis in Lithium-Sulfur Batteries

Yang, Dawei1,2; Liang, Zhifu1,3,4; Tang, Pengyi5,6,7; Zhang, Chaoqi1,2; Tang, Mingxue8; Li, Qizhen9; Biendicho, Jordi Jacas1; Li, Junshan10; Heggen, Marc5,6; Dunin-Borkowski, Rafal E.5,6; Xu, Ming11; Llorca, Jordi12,13; Arbiol, Jordi3,4,14; Morante, Joan Ramon1,2; Chou, Shu-Lei15; Cabot, Andreu1,14

2022

10.1002/adma.202108835

ADVANCED MATERIALS   影响因子和分区

0935-9648

1521-4095

The shuttling behavior and sluggish conversion kinetics of the intermediate lithium polysulfides (LiPS) represent the main obstructions to the practical application of lithium-sulfur batteries (LSBs). Herein, a 1D pi-d conjugated metal-organic framework (MOF), Ni-MOF-1D, is presented as an efficient sulfur host to overcome these limitations. Experimental results and density functional theory calculations demonstrate that Ni-MOF-1D is characterized by a remarkable binding strength for trapping soluble LiPS species. Ni-MOF-1D also acts as an effective catalyst for S reduction during the discharge process and Li2S oxidation during the charging process. In addition, the delocalization of electrons in the pi-d system of Ni-MOF-1D provides a superior electrical conductivity to improve electron transfer. Thus, cathodes based on Ni-MOF-1D enable LSBs with excellent performance, for example, impressive cycling stability with over 82% capacity retention over 1000 cycles at 3 C, superior rate performance of 575 mAh g(-1) at 8 C, and a high areal capacity of 6.63 mAh cm(-2) under raised sulfur loading of 6.7 mg cm(-2). The strategies and advantages here demonstrated can be extended to a broader range of pi-d conjugated MOFs materials, which the authors believe have a high potential as sulfur hosts in LSBs.

lithium polysulfide lithium-sulfur batteries metal organic frameworks pi-d conjugation

SCI ; EI

英语

NI论文 ; ESI高被引

其他

Spanish Ministerio de Economia y Competitividad["ENE2016-77798-C4-3-R","PID2020-116093RB-C43"] ; National Natural Science Foundation of China[21974007,"U1930401"] ; MINECO SO FPI Ph.D. Grant[SEV-2013-0295-17-1] ; Generalitat de Catalunya["2017 SGR 327","2017 SGR 1246"] ; Severo Ochoa Programme (MINECO)[SEV-2017-0706] ; Fundamental Research Funds for the Central Universities[buctrc202112] ; European Union's Horizon 2020 Research and Innovation Programme[823717 - ESTEEM3]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Multidisciplinary ; Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Applied ; Physics, Condensed Matter

WOS:000747786300001

WILEY-V C H VERLAG GMBH

20220511571195

Density functional theory ; Lithium compounds ; Lithium sulfur batteries ; Sulfur

Secondary Batteries:702.1.2 ; Chemical Products Generally:804 ; Organic Polymers:815.1.1 ; Synthetic Rubber:818.2.1 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

MATERIALS SCIENCE

Web of Science

1.Catalonia Inst Energy Res IREC, Barcelona 08930, Spain
2.Univ Barcelona, Dept Elect & Biomed Engn, Barcelona 08028, Spain
3.CSIC, Catalan Inst Nanosci & Nanotechnol ICN2, Campus UAB, Barcelona 08193, Spain
4.BIST, Campus UAB, Barcelona 08193, Spain
5.Forschungszentrum Julich, Ernst Ruska Ctr Microscopy & Spect Electrons, D-52425 Julich, Germany
6.Forschungszentrum Julich, Peter Grunberg Inst, D-52425 Julich, Germany
7.Chinese Acad Sci, ShangHai Inst Microsyst & Informat Technol, State Key Lab Informat Funct Mat, 2020 X Lab, Shanghai, Peoples R China
8.Ctr High Pressure Sci & Technol Adv Res, Beijing 100094, Peoples R China
9.Southern Univ Sci & Technol SUSTech, Dept Biomed Engn, Shenzhen 518055, Guangdong, Peoples R China
10.Chengdu Univ, Inst Adv Study, Chengdu 610106, Peoples R China
11.Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
12.Univ Politecn Cataluna, Dept Chem Engn, Inst Energy Technol, Barcelona 08019, Spain
13.Univ Politecn Cataluna, Barcelona Res Ctr Multiscale Sci & Engn, EEBE, Barcelona 08019, Spain
14.ICREA, Pg Lluis Co 23, Barcelona 08010, Spain
15.Wenzhou Univ, Coll Chem & Mat Engn, Inst Carbon Neutralizat, Wenzhou 325035, Zhejiang, Peoples R China

Yang, Dawei,Liang, Zhifu,Tang, Pengyi,et al. A High Conductivity 1D pi-d Conjugated Metal-Organic Framework with Efficient Polysulfide Trapping-Diffusion-Catalysis in Lithium-Sulfur Batteries[J]. ADVANCED MATERIALS,2022,34.

Yang, Dawei.,Liang, Zhifu.,Tang, Pengyi.,Zhang, Chaoqi.,Tang, Mingxue.,...&Cabot, Andreu.(2022).A High Conductivity 1D pi-d Conjugated Metal-Organic Framework with Efficient Polysulfide Trapping-Diffusion-Catalysis in Lithium-Sulfur Batteries.ADVANCED MATERIALS,34.

Yang, Dawei,et al."A High Conductivity 1D pi-d Conjugated Metal-Organic Framework with Efficient Polysulfide Trapping-Diffusion-Catalysis in Lithium-Sulfur Batteries".ADVANCED MATERIALS 34(2022).