{"title":"All-purpose redox-active metal-organic frameworks as both cathodic and anodic host materials for advanced lithium-sulfur batteries","authors":"","doi":"10.1016/j.matt.2024.04.039","DOIUrl":null,"url":null,"abstract":"<div><p>Multifunctional metal-organic frameworks (MOFs) hold great potential in addressing challenges in energy storage devices by offering customizable guest-host interactions. Herein, we integrated Lewis acidic metal clusters (M = Zr<sup>4+</sup>, Hf<sup>4+</sup>, and Th<sup>4+</sup>) and redox-active Ni-bis(dithiolene) units (NiS<sub>4</sub><span>) into a series of bifunctional MOFs, which serve as both cathodic and anodic host materials for lithium-sulfur (Li-S) batteries. Through systematic control experiments and density functional theory simulations, we elucidate the crucial roles of metal clusters and NiS</span><sub>4</sub><span> units in achieving efficient adsorption and rapid electrocatalytic conversion of polysulfides on the cathode and promoting uniform Li nucleation for enhanced cycling stability on the anode. Optimizing the MOF design resulted in advanced Li-S batteries, exhibiting remarkable capacity retention (81.5%) and an ultrahigh Coulombic efficiency (99.5%) after 800 cycles. This study highlights the potential of multifunctional MOFs in simultaneously overcoming the bottlenecks faced by the S cathode and Li anode.</span></p></div>","PeriodicalId":388,"journal":{"name":"Matter","volume":null,"pages":null},"PeriodicalIF":17.3000,"publicationDate":"2024-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Matter","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2590238524002121","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MATERIALS SCIENCE, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
Multifunctional metal-organic frameworks (MOFs) hold great potential in addressing challenges in energy storage devices by offering customizable guest-host interactions. Herein, we integrated Lewis acidic metal clusters (M = Zr4+, Hf4+, and Th4+) and redox-active Ni-bis(dithiolene) units (NiS4) into a series of bifunctional MOFs, which serve as both cathodic and anodic host materials for lithium-sulfur (Li-S) batteries. Through systematic control experiments and density functional theory simulations, we elucidate the crucial roles of metal clusters and NiS4 units in achieving efficient adsorption and rapid electrocatalytic conversion of polysulfides on the cathode and promoting uniform Li nucleation for enhanced cycling stability on the anode. Optimizing the MOF design resulted in advanced Li-S batteries, exhibiting remarkable capacity retention (81.5%) and an ultrahigh Coulombic efficiency (99.5%) after 800 cycles. This study highlights the potential of multifunctional MOFs in simultaneously overcoming the bottlenecks faced by the S cathode and Li anode.
期刊介绍:
Matter, a monthly journal affiliated with Cell, spans the broad field of materials science from nano to macro levels,covering fundamentals to applications. Embracing groundbreaking technologies,it includes full-length research articles,reviews, perspectives,previews, opinions, personnel stories, and general editorial content.
Matter aims to be the primary resource for researchers in academia and industry, inspiring the next generation of materials scientists.