Ion recognition enables fast Mg–Cl bond dissociation kinetics and better Mg plating/stripping reversibility  

作　　者：Jiacheng Yang Jinlei Zhang Kun Zhang Jing Liu Zhenfang Zhou Zhenjiang Li Guicun Li Guanglei Cui Zhonghua Zhang 

机构地区：[1]College of Materials Science and Engineering,Qingdao University of Science and Technology,Qingdao 266042,PR China [2]Department of Pharmacy,Jining Medical University,Rizhao 276826,PR China [3]Qingdao Industrial Energy Storage Research Institute,Qingdao Institute of Bioenergy and Bioprocess Technology,Chinese Academy of Sciences,Qingdao 266101,PR China [4]Zibo Institute for Product Quality Inspection,Zibo 255063,PR China

出　　处：《Journal of Magnesium and Alloys》2024年第12期5205-5215,共11页镁合金学报(英文)

基　　金：supported by the Natural Science Foundation of Shandong Province(ZR2021QE166);the National Natural Science Foundation of China(51972187,22279068);the Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09);the National Natural Science Foundation for Distinguished Young Scholars of China(51625204);We also thank the Introduction and Cultivation Plan of Young Innovative Talents in Colleges and Universities of Shandong Province(2019).

摘　　要：Rechargeable Mg-metal batteries hold considerable promise for renewable energy storage and utilization.However,the Mg stripping/plating processes suffer from sluggish ion pairs dissociation kinetics,resulting in poor rate and cycle properties.In this work,an efficient skeleton host containing dissimilar coupling elements with varied electronegativity has been designed to promote interfacial reaction kinetics by accelerating the Mg–Cl bond dissociation process.As a proof-of-concept prototype,the N/O-doped cobalt nanoparticles embedded in carbonaceous polyhedrons has been synthesized via facile high temperature annealing of zeolitic imidazolate framework-67(ZIF-67).The exposed electron-rich N/O sites and electron-deficient Co sites can regulate the adsorbing structure configuration of[Mg-Cl]^(+)complex ions by selectively bonding with the Mg^(2+)and Cl^(–)through chemical coordination linkage,respectively.The elongated bond length from 2.596A to 2.679A and the weakened bond strength are beneficial for the complex ions dissociation,leading to better charge transfer kinetics.In addition,the better magnesiophilic property accompanied by the conductive and porous permeable three-dimensional architecture realizes the homogeneous electrodeposition of Mg and improved electrode kinetics.The decreased overpotential has been verified in both magnesium organohaloaluminates electrolyte(from 290 mV to 189 mV)and conventional Mg(TFSI)2-based electrolyte(from 600 mV to 200 mV).The designed skeleton host also exhibits excellent long cycle lifespan above 2300 h and extra-high average Coulombic efficiency of 99.65%within 700 cycles.The accelerated bond splitting strategy enables improved metal-anode reversibility,which is also insightful to high concentrated or other electrolyte systems that contain abundant ion pairs or aggregates.

关 键 词：KINETICS DISSOCIATION KINETICS 

分 类 号：TM912[电气工程—电力电子与电力传动]