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Reversible Magnesium Metal Anode Enabled by Cooperative Solvation/Surface Engineering in Carbonate Electrolytes

Nano-Micro Letters 2021年第12期13卷 109-119页

作者： Caiyun Wang Yao Huang Yunhao Lu Hongge Pan Ben Bin Xu Wenping Sun Mi Yan yinzhu jiang School of Materials Science and Engineering State Key Laboratory of Clean Energy UtilizationZhejiang UniversityHangzhou 310027ZhejiangPeople’s Republic of China ZJU‑Hangzhou Global Scientific and Technological Innovation Centre Zhejiang UniversityHangzhou 311200People’s Republic of China Institute of Science and Technology for New Energy Xi’an Technological UniversityXi’an 710021People’s Republic of China Mechanical and Construction Engineering Faculty of Engineering and EnvironmentNorthumbria UniversityNewcastle upon Tyne NE18STUK

Magnesium metal anode holds great potentials toward future high energy and safe rechargeable magnesium battery technology due to its divalent redox and dendrite-free nature. Electrolytes based on Lewis acid chemistry enable the reversible Mg plating/stripping,while they fail to match most cathode materials toward highvoltage magnesium batteries. Herein,reversible Mg plating/stripping is achieved in conventional carbonate electrolytes enabled by the cooperative solvation/surface engineering. Strongly electronegative Cl from the MgCl_(2) additive of electrolyte impairs the Mg…O = C interaction to reduce the Mg^(2+) desolvation barrier for accelerated redox kinetics,while the Mg^(2+)-conducting polymer coating on the Mg surface ensures the facile Mg^(2+) migration and the e ective isolation of electrolytes. As a result,reversible plating and stripping of Mg is demonstrated with a low overpotential of 0.7 V up to 2000 cycles. Moreover,benefitting from the wide electrochemical window of carbonate electrolytes,high-voltage(> 2.0 V) rechargeable magnesium batteries are achieved through assembling the electrode couple of Mg metal anode and Prussian blue-based cathodes. The present work provides a cooperative engineering strategy to promote the application of magnesium anode in carbonate electrolytes toward high energy rechargeable batteries.

关键词： Rechargeable magnesium batteries Metal anode Solvation effect Passivation Carbonate electrolytes

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Multiscale simulations of surface adsorption characteristics of amino acids on zinc metal anode

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Journal of Energy Chemistry 2023年第12期87卷 153-161,I0006页

作者： Yufan Xia Zijian Hong Linming Zhou Shuang Chen Zhen Luo Shoutong Jin Yuhui Huang yinzhu jiang Yongjun Wu School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina ZJU-Hangzhou Global Scientific and Technological Innovation Center Zhejiang UniversityHangzhou 311215ZhejiangChina State Key Laboratory of Silicon and Advanced Semiconductor Materials Zhejiang UniversityHangzhou 310027ZhejiangChina Research Institute of Zhejiang University-Taizhou Zhejiang UniversityTaizhou 318000ZhejiangChina

Aqueous zinc-ion batteries(ZIBs) are considered promising power sources for grid storage,but they face several issues,including dendrite growth,corrosion,hydrogen evolution,etc.,which are related to the Zn metal/liquid electrolyte *** address these challenges,many researchers have focused on modifying the Zn anode with surface ***,the underlying mechanism between the Zn surface and adsorbed/protective molecules has not been thoroughly *** this study,we built a multiscale simulation platform that integrates state-of-art simulation methods to comprehensively investigate the adsorption process of amino acids on the Zn metal *** major finding is that adsorption sites,adsorbate–surface angle,and average distance are critical parameters for the stability and strength of surface ***,ab initio molecular dynamics reveal the kinetics of the surface adsorption and molecule reorientation ***,it can be discovered that the amino acids prefer to align parallel to the Zn metal surface,leading to better surface protection against corrosion and preventing dendrite *** findings pave the way for an in-depth understanding of the surface adsorption process,as well as providing concrete design principles for stable Zn metal anodes.

关键词： Zn-ion battery First-principles calculations Surface adsorption Ab initio molecular dynamics

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Revitalizing sodium-ion batteries via controllable microstructures and advanced electrolytes for hard carbon

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eScience 2024年第3期4卷 65-103页

作者： Feng Wang Zhenming jiang Yanyan Zhang Yanlei Zhang Jidao Li Huibo Wang yinzhu jiang Guichuan Xing Hongchao Liu Yuxin Tang College of Chemical Engineering Fuzhou UniversityFuzhou 350116PR China Institute of Applied Physics and Materials Engineering University of MacaoMacao999078PR China School of Materials Science and Engineering ZJU-Hangzhou Global Scientific and Technological Innovation CentreZhejiang UniversityHangzhou 310027China Qingyuan Innovation Laboratory 1 Xueyuan RoadQuanzhou 362801PR China

Sodium-ion batteries(SIBs)with low cost and high safety are considered as an electrochemical energy storage technology suitable for large-scale energy *** carbon,which is inexpensive and has both high capacity and low sodium storage potential,is regarded as the most promising anode for commercial ***,the commercialization of hard carbon still faces technical issues of low initial Coulombic efficiency,poor rate performance,and insufficient cycling stability,due to the intrinsically irregular microstructure of hard *** address these challenges,the rational design of the hard carbon microstructure is crucial for achieving high-performance SIBs,via gaining an in-depth understanding of its structure-performance *** this context,our review firstly describes the sodium storage mechanism from the perspective of the hard carbon microstructure's *** then summarize the state-of-art development of hard carbon,providing a critical overview of emergence of hard carbon in terms of precursor selection,microstructure design,and electrolyte regulation to optimize strategies for addressing practical ***,we highlight directions for the future development of hard carbon to achieve the commercialization of high-performance *** believe this review will serve as basic guidance for the rational design of hard carbon and stimulate more exciting research into other types of energy storage devices.

关键词： Hard carbon Coulombic efficiency Controllable microstructure Electrolyte regulation Sodium storage mechanism Sodium-ion batteries

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Multiple unpinned Dirac points in group-Va single-layers with phosphorene structure

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npj Computational Materials 2016年第1期2卷 142-148页

作者： Yunhao Lu Di Zhou Guoqing Chang Shan Guan Weiguang Chen yinzhu jiang Jianzhong jiang Xue-sen Wang Shengyuan A Yang Yuan Ping Feng Yoshiyuki Kawazoe Hsin Lin School of Materials Science and Engineering Zhejiang UniversityHangzhouChina State Key Laboratory of Silicon Materials Zhejiang UniversityHangzhouChina Centre for Advanced 2D Materials and Graphene Research Centre National University of SingaporeSingaporeSingapore Department of Physics National University of SingaporeSingaporeSingapore Research Laboratory for Quantum Materials Singapore University of Technology and DesignSingaporeSingapore College of Physics and Electronic Engineering Zhengzhou Normal UniversityZhengzhouChina New Industry Creation Hatchery Center Tohuku UniversitySendaiJapan Institute of Thermophysics Siberian Branch of Russian Academy of SciencesNovosibirskRussia

Emergent Dirac fermion states underlie many intriguing properties of graphene,and the search for them constitutes one strong motivation to explore two-dimensional(2D)allotropes of other ***,the ultrathin layers of black phosphorous,has been a subject of intense investigations recently,and it was found that other group-Va elements could also form 2D layers with similar puckered lattice ***,by a close examination of their electronic band structure evolution,we discover two types of Dirac fermion states emerging in the low-energy *** pair of(type-I)Dirac points is sitting on high-symmetry lines,while two pairs of(type-II)Dirac points are located at generic k-points,with different anisotropic dispersions determined by the reduced symmetries at their *** fully-unpinned(type-II)2D Dirac points are discovered for the first *** the absence of spin-orbit coupling(SOC),we find that each Dirac node is protected by the sublattice symmetry from gap opening,which is in turn ensured by any one of three point group *** SOC generally gaps the Dirac nodes,and for the type-I case,this drives the system into a quantum spin Hall insulator *** suggest possible ways to realise the unpinned Dirac points in strained phosphorene.

关键词： structure spectrum Dirac

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Tuning coordination environment of iron ions to ensure ultra-high pseudocapacitive capability in iron oxide

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Nano Research 2023年第5期16卷 6914-6921页

作者： Wubin Du Chenhui Yan Mingxi Gao Jian Chen Panyu Gao Xuebin Yu yinzhu jiang Wenping Sun Yongfeng Liu Mingxia Gao Shibo Xi Hongge Pan State Key Laboratory of Silicon Materials and School of Materials Science and Engineering Zhejiang UniversityHangzhou 310027China Institute of Science and Technology for New Energy Xi'an Technological UniversityXi'an 710021China Department of Materials Science Fudan UniversityShanghai 200433China Institute of Chemical and Engineering Sciences Agency for ScienceTechnology and ResearchSingapore 138632Singapore

The mechanism governing the pseudocapacitive lithium storage behavior is one of the most critical unsolved issues in conversion-type anodes for lithium-ion *** this work,we,for the first time,demonstrate that the pseudocapacitive capability of iron oxide-based anodes is closely associated with the electronic structures of iron *** proof of concept,the introduction of amorphization,nitrogen doping,oxygen vacancies reduces the coordination of iron ions and contributes significantly to the pseudocapacitive lithium storage capability of iron oxide,reaching up to 96%of the specific capacity at 1 mV·s^(−1).Due to the significantly modulated coordination environment,the 3d electrons of Fe(II)are delocalized with increased spin state and the energy band gap is narrowed,accompanied by an upshift of Fermi *** redox activity and carrier mobility of iron oxides are substantially increased,which substantially enhance the exchange current density and thereby improve the pseudocapacitive capability of iron oxide.

关键词： coordination environment electronic structure exchange current density pseudocapacitive capability lithium-ion batteries

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Prussian Blue-Based Cathodes for Sodium Ion Batteries

Prussian Blue-Based Cathodes for Sodium Ion Batteries

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中国化学会2019能源材料和缺陷化学研讨会

作者： Baoqi Wang Shenglan Yu yinzhu jiang State Key Laboratory of Silicon Materials School of Material Science and Engineering Zhejiang University

Rechargeable sodium ion batteries（SIBs） are emerging as one of the promising candidates for applications in large-scale energy-storage systems. Prussian blue analogues（PBAs） have been considered as potential cathodes because of their rigid open framework and low-cost synthesis. However, the less activated low spin Fe in FeC6 octahedron lowers the average potential and the overall capacity, while the lattice vacancies and side reactions between low spin Fe and the electrolyte shortens PB’s cycling life. Herein, PB with a controllable gradient nickel substitution, which features a high-Ni-content outer layer and low-Ni-content inner layer in a single grain, is demonstrated for high performance sodium storage. The high-Ni-content outer layer efficiently prevents side reactions, ensuring excellent cycling stability, while a small amount of nickel ions in the inner layer efficiently activates the low spin Fe for achieving high capacity. Taking the above synergistic advantages, our gradient-PB exhibits a high reversible capacity of 114 mAh g-1 at 100 m Ah g-1 and 84 mAh g-1 at 1 A g-1 with very stable cycling for up to 1000 cycles. Gradient substitution in PB analogues provides a novel strategy for exploring high performance PB-based cathodes for SIBs. On the other hand, PBAs also suffer from inferior rate capability and poor cycling stability resulting from the low electronic conductivity and deficiencies in the framework. In the light of understanding on vacancy-impacted sodium storage and Na-inserted reaction kinetics, we report in-situ synthesized PB@C composite as a high-performance SIB cathode. Perfect and nanosized PB cubes were grown directly on carbon chains, assuring fast charge transfer and Na-ion diffusion. The existence of [Fe（CN）6] vacancy in the PB crystal is found to greatly degrade the electrochemical activity of the FeLS（C） redox couple via the first principles computation. The superior reaction kinetics is demonstrated for the redox reactions of the FeH

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Interface engineering of heterostructured electrocatalysts towards efficient alkaline hydrogen electrocatalysis

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Science Bulletin 2021年第1期66卷 85-96,M0004页

作者： Guoqiang Zhao yinzhu jiang Shi-Xue Dou Wenping Sun Hongge Pan School of Materials Science and Engineering State Key Laboratory of Silicon MaterialsZhejiang UniversityHangzhou 310027China Institute for Superconducting and Electronic Materials Australian Institute for Innovative MaterialsUniversity of WollongongWollongongNSW 2522Australia

Boosting the alkaline hydrogen evolution and oxidation reaction(HER/HOR)kinetics is vital to practicing the renewable hydrogen cycle in alkaline ***,intensive research has demonstrated that interface engineering is of critical significance for improving the performance of heterostructured electrocatalysts particularly toward the electrochemical reactions involving multiple reaction intermediates like alkaline hydrogen electrocatalysis,and the research advances also bring substantial non-trivial fundamental insights ***,we review the current status of interface engineering with respect to developing efficient heterostructured electrocatalysts for alkaline HER and *** major subjects—how interface engineering promotes the reaction kinetics and what fundamental insights interface engineering has brought into alkaline HER and HOR—are ***,heterostructured electrocatalysts with abundant interfaces have shown substantially accelerated alkaline hydrogen electrocatalysis kinetics owing to the synergistic effect from different components,which could balance the adsorption/desorption behaviors of the intermediates at the ***,interface engineering can effectively tune the electronic structures of the active sites via electronic interaction,interfacial bonding,and lattice strain,which would appropriately optimize the binding energy of targeted intermediates like ***,the confinement effect is critical for delivering high durability by sustaining high density of active *** last,our own perspectives on the challenges and opportunities toward developing efficient heterostructured electrocatalysts for alkaline hydrogen electrocatalysis are provided.

关键词： Interface engineering Heterostructure Hydrogen evolution reaction Hydrogen oxidation reaction Electrocatalysis

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A robust,highly reversible,mixed conducting sodium metal anode

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Science Bulletin 2021年第2期66卷 179-186,M0004页

作者： Keshuang Cao Qianli Ma Frank Tietz Ben Bin Xu Mi Yan yinzhu jiang School of Materials Science and Engineering State Key Laboratory of Clean Energy UltilizationZhejiang UniversityHangzhou 310027China Forschungszentrum Jülich GmbH Institute of Energy and Climate ResearchMaterials Synthesis and Processing(IEK-1)52425 JülichGermany Smart Materials and Surfaces Lab Mechanical EngineeringFaculty of Engineering and EnvironmentNorthumbria UniversityNewcastle upon Tyne NE18STUK

Sodium metal anode holds great promise in pursuing high-energy and sustainable rechargeable batteries,but severely suffers from fatal dendrite growth accompanied with huge volume ***,a robust mixed conducting sodium metal anode is designed through incorporating Na SICON-type solid Na-ion conductor into bulk Na.A fast and continuous pathway for simultaneous transportation of electrons and Na+is established throughout the composite *** intimate contact between Na-ion conducting phase and Na metallic phase constructs abundant two-phase boundaries for fast redox ***,the compact configuration of the composite anode substantially protects Na metal from being corroded by liquid organic electrolyte for the minimization of side *** from the unique configuration,the composite anode shows highly reversible and durable Na plating/stripping *** symmetric cells exhibit ultralong lifespan for over 700 h at 1 mA cm^(-2)with a high capacity of 5 m Ah cm^(-2)and outstanding rate capability up to 8 m A cm^(-2)in the carbonate *** cells with Na_(3)V_(2)(PO_(4))_(3)/C cathode demonstrate impressive cycling stability(capacity decay of 0.012%per cycle)and low charge/discharge polarization as *** work provides new insights into rational design and development of robust sodium metal anode through an architecture engineering strategy for advanced rechargeable sodium batteries.

关键词： Sodium metal battery Sodium metal anode Solid Na-ion conductor Dendrite Cycling stability

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FeCuNbSiB纳米晶软磁粉芯的制备和磁性能

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稀有金属材料与工程 2014年第8期43卷 1951-1954页

作者：熊亚东林坤严密姜银珠浙江大学浙江杭州310027

采用熔体快淬法制备了Fe73.5Cu1Nb3Si13.5B9（FINEMET,at%）非晶薄带,通过高能球磨制成磁粉,筛分后的磁粉在0.2%~1.0%（质量分数）的磷酸溶液中钝化,并与0.4%的环氧树脂混合,于1.64~1.96 GPa下压制成磁环。磁环经过500℃去应力退火处理... 详细信息

采用熔体快淬法制备了Fe73.5Cu1Nb3Si13.5B9（FINEMET,at%）非晶薄带,通过高能球磨制成磁粉,筛分后的磁粉在0.2%~1.0%（质量分数）的磷酸溶液中钝化,并与0.4%的环氧树脂混合,于1.64~1.96 GPa下压制成磁环。磁环经过500℃去应力退火处理,在非晶基体表面析出晶粒大小为14.3 nm的纳米晶α-Fe（Si）相。通过去应力过程和双相结构的协同作用,纳米晶软磁粉芯表现出优良的磁性能,在100 kHz和0.1 T下的损耗仅为583 mW/cm3。

关键词：损耗磁粉芯钝化处理 FINEMET合金

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聚阴离子型钠离子电池正极材料的研究进展

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物理化学学报 2020年第5期36卷 63-74页

作者：潘雯丽关文浩姜银珠浙江大学材料科学与工程学院硅材料国家重点实验室杭州310027

作为钠离子电池正极材料的体系之一,聚阴离子型化合物具有成本低廉和安全性高的优点,适合于大规模固定式储能系统。实时平衡电网电力供需水平对正极材料的倍率性能提出了更高的要求,而聚阴离子材料虽然存在离子扩散通道,但缺乏电子传输... 详细信息

作为钠离子电池正极材料的体系之一,聚阴离子型化合物具有成本低廉和安全性高的优点,适合于大规模固定式储能系统。实时平衡电网电力供需水平对正极材料的倍率性能提出了更高的要求,而聚阴离子材料虽然存在离子扩散通道,但缺乏电子传输路径,导致其动力学性能不佳。为了挖掘影响聚阴离子型正极动力学性能的因素,本文以结构为基础,对影响聚阴离子正极离子扩散行为的本征原因作了阐述,再从表面修饰和形态设计入手,对目前研究较多的改善电极表面及界面处离子和电子扩散的策略作了总结与点评,然后从材料的分级结构回归到鲜见报导的元素掺杂和取代,从本质上提出优化动力学性能的方案,并展望了进一步提高正极材料倍率性能的方向。本文可为高倍率的聚阴离子型正极材料及其他材料的开发提供基本理论和实践依据。

关键词：钠离子电池聚阴离子型正极高倍率性能离子扩散电子传输

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