Defects Engineering of Lightweight Metal-Organic Frameworks-Based Electrocatalytic Membrane for High-Loading Lithium-Sulfur Batteries

Sha Li; Jiande Lin; Yu Ding; Pan Xu; Xiangyang Guo; Weiming Xiong; De-Yin Wu; Quanfeng Dong; Jiajia Chen; Li Zhang

doi:10.1021/acsnano.1c05585

Defects Engineering of Lightweight Metal-Organic Frameworks-Based Electrocatalytic Membrane for High-Loading Lithium-Sulfur Batteries

ACS Nano. 2021 Aug 24;15(8):13803-13813. doi: 10.1021/acsnano.1c05585. Epub 2021 Aug 11.

Authors

Sha Li¹, Jiande Lin¹, Yu Ding¹, Pan Xu¹, Xiangyang Guo², Weiming Xiong¹, De-Yin Wu¹, Quanfeng Dong¹, Jiajia Chen¹, Li Zhang¹

Affiliations

¹ State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Tan Kah Kee Innovation Laboratory, Xiamen University, Xiamen 361005, Fujian, China.
² State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China.

PMID: 34379405
DOI: 10.1021/acsnano.1c05585

Abstract

The sluggish kinetics and shuttle effect of lithium polysulfide intermediates are the major issues that retard the practical applications of lithium-sulfur (Li-S) batteries. Herein, we introduce a defect engineering strategy to construct a defected-UiO-66-NH₂-4/graphene electrocatalytic membrane (D-UiO-66-NH₂-4/G EM) which could accelerate the conversion of lithium polysulfides in high sulfur loadings and low electrolyte/sulfur (E/S) ratio Li-S batteries. Metal-organic frameworks (UiO-66-NH₂) can be directionally chemical engraved to form concave octahedra with abundant defects. According to electrocatalytic kinetics and DFT calculations studies, the D-UiO-66-NH₂-4 architecture effectively provides ample sites to capture polysulfides via strong chemical affinity and effectively delivers electrocatalytic activity of polysulfide conversion. As a result, a Li-S battery with such an electrocatalytic membrane delivers a high capacity of 12.3 mAh cm^-2 (1013 mAh g^-1) at a sulfur loading up to 12.2 mg·_S cm^-2 under a lean electrolyte condition (E/S = 5 μL mg^-1-sulfur) at 2.1 mA cm^-2 (0.1 C). Moreover, a prototype soft package battery also exhibits excellent cycling stability with a maintained capacity of 996 mAh g^-1 upon 100 cycles.

Keywords: defects engineering; electrocatalytic membrane; high sulfur loadings; lean electrolyte conditions; lithium−sulfur batteries; metal−organic frameworks.