A High conductivity 1D π-d conjugated metal-organic framework with efficient polysulfide trapping-diffusion-catalysis in lithium-sulfur batteries

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 π-d conjugated metal-organic framework (MOF), Ni-MOF-1D, is presented as an efficient...

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Bibliographic Details
Authors: Yang, Dawei|||0000-0002-3842-8286, Liang, Zhifu, Tang, PengYi|||0000-0002-2306-095X, Zhang, Chaoqi|||0000-0002-0357-235X, Tang, Mingxue|||0000-0002-7282-4100, Li, Qizhen, Jacas Biendicho, Jordi|||0000-0001-5981-6168, Li, Junshan|||0000-0002-1482-1972, Heggen, Marc|||0000-0002-2646-0078, Dunin-Borkowski, Rafal E.|||0000-0001-8082-0647, Xu, Ming, Llorca, Jordi|||0000-0002-7447-9582, Arbiol i Cobos, Jordi|||0000-0002-0695-1726, Morante, Joan Ramon|||0000-0002-4981-4633, Chou, Shulei|||0000-0003-1155-6082, Cabot i Codina, Andreu|||0000-0002-7533-3251
Format: article
Publication Date:2022
Country:España
Institution:Universitat Autònoma de Barcelona
Repository:Dipòsit Digital de Documents de la UAB
Language:English
OAI Identifier:oai:ddd.uab.cat:271941
Online Access:https://ddd.uab.cat/record/271941
https://dx.doi.org/urn:doi:10.1002/adma.202108835
Access Level:Open access
Keyword:Lithium polysulfide
Lithium-sulfur batteries
Metal organic frameworks
π-d conjugation
Description
Summary: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 π-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 LiS oxidation during the charging process. In addition, the delocalization of electrons in the π-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 at 8 C, and a high areal capacity of 6.63 mAh cm under raised sulfur loading of 6.7 mg cm. The strategies and advantages here demonstrated can be extended to a broader range of π-d conjugated MOFs materials, which the authors believe have a high potential as sulfur hosts in LSBs.

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