Defects Engineering of Lightweight Metal-Organic Frameworks-Based Electrocatalytic Membrane for High-Loading Lithium-Sulfur Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 34379405.
- Also identified by DOI 10.1021/acsnano.1c05585.
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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-NH<sub>2</sub>-4/graphene electrocatalytic membrane (D-UiO-66-NH<sub>2</sub>-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-NH<sub>2</sub>) can be directionally chemical engraved to form concave octahedra with abundant defects. According to electrocatalytic kinetics and DFT calculations studies, the D-UiO-66-NH<sub>2</sub>-4 architecture effectively provides ample sites to capture polysulfides <i>via</i> 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<sup>-2</sup> (1013 mAh g<sup>-1</sup>) at a sulfur loading up to 12.2 mg·<sub>S</sub> cm<sup>-2</sup> under a lean electrolyte condition (E/S = 5 μL mg<sup>-1</sup>-sulfur) at 2.1 mA cm<sup>-2</sup> (0.1 C). Moreover, a prototype soft package battery also exhibits excellent cycling stability with a maintained capacity of 996 mAh g<sup>-1</sup> upon 100 cycles.