{"title":"作为先进锂硫电池阴极和阳极主材料的多功能氧化还原活性金属有机框架","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":"{\"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}","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
摘要
多功能金属有机框架(MOFs)通过提供可定制的客体-宿主相互作用,在应对能量存储设备的挑战方面具有巨大潜力。在这里,我们将路易斯酸性金属簇(M = Zr4+、Hf4+ 和 Th4+)和具有氧化还原活性的镍-双(二硫代二苯)单元(NiS4)整合到一系列双功能 MOF 中,作为锂-硫(Li-S)电池的阴极和阳极宿主材料。通过系统控制实验和密度泛函理论模拟,我们阐明了金属团簇和 NiS4 单元在阴极实现多硫化物高效吸附和快速电催化转化以及在阳极促进锂均匀成核以增强循环稳定性方面的关键作用。通过优化 MOF 设计,先进的锂-S 电池在 800 次循环后表现出显著的容量保持率(81.5%)和超高的库仑效率(99.5%)。这项研究凸显了多功能 MOFs 在同时克服 S 阴极和 Li 阳极所面临的瓶颈方面的潜力。
All-purpose redox-active metal-organic frameworks as both cathodic and anodic host materials for advanced lithium-sulfur batteries
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.