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Ni/Co bimetallic organic frameworks nanospheres for highperformance electrochemical energy storage

Nano Research 2024年第6期17卷 5122-5130页

作者： Jianru Guan Minlu Liu Limin Zhu Jiamei Wang Qing Han Xiaoxia Yang weibo hua Lingling Xie Xiaoyu Cao School of Chemistry and Chemical Engineering Key Laboratory of High Specific Energy Materials for Electrochemical Power Sources of Zhengzhou CityHenan University of TechnologyZhengzhou 450001China School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’an 710049China School of Environmental Engineering Henan University of TechnologyZhengzhou 450001China

In addition to their many well-known advantages(e.g.,ultra-high porosity,good pore size distribution,easy functionalization,and structural tolerability),metal-organic frameworks(MOFs)are a new class of advanced functional ***,their backbones are highly susceptible to deformation after exposure to acidic or alkaline *** a result of lithium-ion batteries embedding or detaching directly from MOFs,they irreversibly *** a result,they fail to maintain their electrochemical *** factors have hindered the development of MOFs as direct electrode materials,making the design of MOF materials with controlled morphology and stable dimensions a new *** this study,we adopted a versatile and effective method to synthesize a novel MOF material(NiCo-BP(BP=BTC/phen and BTC=1,3,5-benzenetricarboxylic acid))using the rigid ligands 1,10-phenanthroline and homobenzotrizoic acid,and the emergence of the Ni-O/N and Co-O/N coordination layers was observed by extended X-ray absorption fine structure(EXAFS)tests,indicating that Ni and Co were coordinated with heterocyclic N-given atoms to form a stable p-πconjugated ***,the metal-ion is attached to the carboxylic acid ligand on the other side,making the metal-organic skeleton complete and *** nanosphere structure of NiCo-BP(~400 nm)allows for full exposure and utilisation of the active sites,especially the Ni,Co,and phenanthroline units,and exhibit impressively high specific capacity and cycling *** a high current density of 1.0 A·g^(−1),a high discharge specific capacity of 631.6 mAh·g^(−1)was obtained after 1000 *** co-participation of two organic ligands in the coordination is in accordance with the theory of soft and hard acids and bases,which contributes to the ability of the material to maintain a high capacity in cycling as well as its cyclic stability.

关键词： lithium-ion batteries metal organic frame electrochemical energy storage dual ligand hard-soft-acid-base

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Preparation and Electrochemical Performance of Li[Ni1/3Co1/3Mn1/3]O2 Synthesized Using LizCO3 as Template

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Chinese Journal of Chemistry 2015年第11期33卷 1303-1309页

作者： Jibin Zhang Yanjun Zhong Xiaxing Shi Zhuo Zheng weibo hua Yanxiao Chen Wenyuan Liu Benhe Zhong College of Chemical Engineering Sichuan University Chengdu Sichuan 610065 China

Porous structure Li[Ni1/3Co1/3Mn1/3]O2 has been synthesized via a facile carbonate co-precipitation method using Li2CO3 as template and lithium-source. The physical and electrochemical properties of the materials were examined by many characterizations including TGA, XRD, SEM, EDS, TEM, BET, CV, EIS and galvanostatic charge-discharge cycling. The results indicate that the as-synthesized materials by this novel method own a well-ordered layered structure a-NaFeO2 [space group： R-3m（166）], porous morphology, and an average primary particle size of about 150 nm. The porous material exhibits larger specific surface area and delivers a high initial capacity of 169.9 mAh·g^-1 at 0.1 C （1 C=180 mA·g ^-1） between 2.7 and 4.3 V, and 126.4, 115.7 mAh.g 1 are still respectively reached at high rate of 10 C and 20 C. After 100 charge-discharge cycles at 1 C, the capacity retention is 93.3%, indicating the excellent cycling stability.

关键词： porous structure Li[Ni1/3Co1/3Mn1/3]O2 cathode material lithium-ion batteries rate performance

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An Approach towards Synthesis of Nanoarchitectured LiNi1/3Co1/3Mn1/3O2 Cathode Material for Lithium Ion Batteries

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Chinese Journal of Chemistry 2015年第2期33卷 261-267页

作者： weibo hua Yanjie Wang Yanjun Zhong Guoping Wang Benhe Zhong Baizeng Fang Xiaodong Guo Shixuan Liao Haijiang Wang College of Chemical Engineering Sichuan UniversityChengduSichuan 610065China Department of Chemical and Biological Engineering University of British Columbia2360 East MallVancouverBCCanadaV6T 1Z3 Institute for Fuel Cell Innovation National Research Council of Canada4250 Wesbrook MallVancouverBC V6T 1W5Canada College of Chemical Engineering University of South ChinaHengyangHunan 421001China

To explore advanced cathode materials for lithium ion batteries(LIBs),a nanoarchitectured LiNi_(1/3)Co_(1/3)Mn_(1/3)O_(2)(LNCM)material is developed using a modified carbonate coprecipitation method in combination with a vacuum distillation-crystallisation *** with the LNCM materials produced by a traditional carbonate copre-cipitation method,the prepared LNCM material synthesized through this modified method reveals a better hexago-nal layered structure,smaller particle sizes(ca.110.5 nm),and higher specific surface *** of its unique structural characteristics,the as-prepared LNCM material demonstrates excellent electrochemical properties in-cluding high rate capability and good cycleability when it is utilized as a cathode in the lithium ion battery(LIB).

关键词： cathode materials nanoarchitectured coprecipitation electrochemical properties lithium ion battery

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Metal-free two-dimensional phosphorene-based electrocatalyst with covalent P-N heterointerfacial reconstruction for electrolyte-lean lithium-sulfur batteries

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Carbon Energy 2024年第5期6卷 175-185页

作者： Jiangqi Zhou Chengyong Shu Jiawu Cui Chengxin Peng Yong Liu weibo hua Laura Simonelli Yuping Wu Shi Xue Dou Wei Tang School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anChina School of Materials Science and Engineering University of Shanghai for Science and TechnologyShanghaiChina State Key Laboratory of Space Power-Sources Technology Shanghai Institute of Space Power-SourcesShanghaiChina CELLS-ALBA Synchrotron BarcelonaSpain School of Energy and Environment Southeast UniversityNanjingChina

The use of lithium-sulfur batteries under high sulfur loading and low electrolyte concentrations is severely restricted by the detrimental shuttling behavior of polysulfides and the sluggish kinetics in redox ***-dimensional(2D)few layered black phosphorus with fully exposed atoms and high sulfur affinity can be potential lithium-sulfur battery electrocatalysts,which,however,have limitations of restricted catalytic activity and poor electrochemical/chemical *** resolve these issues,we developed a multifunctional metal-free catalyst by covalently bonding few layered black phosphorus nanosheets with nitrogen-doped carbon-coated multiwalled carbon nanotubes(denoted c-FBP-NC).The experimental characterizations and theoretical calculations show that the formed polarized P-N covalent bonds in c-FBP-NC can efficiently regulate electron transfer from NC to FBP and significantly promote the capture and catalysis of lithium polysulfides,thus alleviating the shuttle ***,the robust 1D-2D interwoven structure with large surface area and high porosity allows strong physical confinement and fast mass ***,with c-FBP-NC as the sulfur host,the battery shows a high areal capacity of 7.69 mAh cm^(−2) under high sulfur loading of 8.74 mg cm^(−2) and a low electrolyte/sulfur ratio of 5.7μL mg^(−1).Moreover,the assembled pouch cell with sulfur loading of 4 mg cm^(−2) and an electrolyte/sulfur ratio of 3.5μL mg^(−1) shows good rate capability and outstanding *** work proposes an interfacial and electronic structure engineering strategy for fast and durable sulfur electrochemistry,demonstrating great potential in lithium-sulfur batteries.

关键词： black phosphorus electronic structure high sulfur loading interfacial covalent bonds lean electrolyte

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Quasi-Solid-State Ion-Conducting Arrays Composite Electrolytes with Fast Ion Transport Vertical-Aligned Interfaces for All-Weather Practical Lithium-Metal Batteries

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Nano-Micro Letters 2022年第12期14卷 401-414页

作者： Xinyang Li Yong Wang Kai Xi Wei Yu Jie Feng Guoxin Gao Hu Wu Qiu Jiang Amr Abdelkader weibo hua Guiming Zhong Shujiang Ding School of Chemistry Xi’an Key Laboratory of Sustainable Energy Materials ChemistryState Key Laboratory of Electrical Insulation and Power EquipmentXi’an Jiaotong UniversityXi’an 710049People’s Republic of China State Key Laboratory for Mechanical Behaviour of Materials Xi’an Jiaotong UniversityXi’an 710049People’s Republic of China Yangtze Delta Region Institute(Huzhou) University of Electronic Science and Technology of ChinaHuzhouZhejiang 313001People’s Republic of China School of Materials and Energy University of Electronic Science and Technology of ChinaChengdu 610054People’s Republic of China Faculty of Science and Technology Bournemouth UniversityTalbot CampusFern BarrowPoole BH125BBUK Institute for Applied Materials-Energy Storage Systems(IAM-ESS) Karlsruhe Institute of Technology(KIT)76344 Eggenstein-LeopoldshafenGermany School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’anShaanxi 710049People’s Republic of China Laboratory of Advanced Spectroelectrochemsitry and Li-ion Batteries Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023People’s Republic of China State Key Laboratory of Organic-inorganic Composites Beijing University of Chemical TechnologyBeijing 100029People’s Republic of China

The rapid improvement in the gel polymer electrolytes(GPEs)with high ionic conductivity brought it closer to practical applications in solid-state Li-metal *** combination of solvent and polymer enables quasi-liquid fast ion transport in the ***,different ion transport capacity between solvent and polymer will cause local nonuniform Li+distribution,leading to severe dendrite *** addition,the poor thermal stability of the solvent also limits the operating-temperature window of the *** the ion transport environment and enhancing the thermal stability are two major challenges that hinder the application of ***,a strategy by introducing ion-conducting arrays(ICA)is created by vertical-aligned montmorillonite into *** ion transport on the ICA was demonstrated by 6Li solid-state nuclear magnetic resonance and synchrotron X-ray diffraction,combined with computer simulations to visualize the transport *** with conventional randomly dispersed fillers,ICA provides continuous interfaces to regulate the ion transport environment and enhances the tolerance of GPEs to extreme ***,GPE/ICA exhibits high room-temperature ionic conductivity(1.08 mS cm^(−1))and long-term stable Li deposition/stripping cycles(>1000 h).As a final proof,Li||GPE/ICA||LiFePO_(4) cells exhibit excellent cycle performance at wide temperature range(from 0 to 60°C),which shows a promising path toward all-weather practical solid-state batteries.

关键词： Solid-state batteries Composite electrolytes Vertical-aligned ion-conducting arrays Interfacial ion-conduction mechanism All-weather practical electrolyte design

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Probing thermally-induced structural evolution during the synthesis of layered Li-, Na-, or K-containing 3d transition-metal oxides

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eScience 2022年第2期2卷 183-191页

作者： weibo hua Xiaoxia Yang Nicola PMCasati Laijun Liu Suning Wang Volodymyr Baran Michael Knapp Helmut Ehrenberg Sylvio Indris School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anShaanxi710049China Institute for Applied Materials(IAM) Karlsruhe Institute of Technology(KIT)Hermann-von-Helmholtz-Platz 1D-76344Eggenstein-LeopoldshafenGermany College of Materials Science and Engineering Guilin University of TechnologyGuilin541004China Paul Scherrer Institut(PSI) WLGA/2295232Villigen PSISwitzerland Deutsches Elektronen-Synchrotron(DESY) Notkestr.85Hamburg22607Germany

Layered alkali-containing 3d transition-metal oxides are of the utmost importance in the use of electrode materials for advanced energy storage applications such as Li-,Na-,or K-ion batteries.A significant challenge in the field of materials chemistry is understanding the dynamics of the chemical reactions between alkali-free precursors and alkali species during the synthesis of these *** this study,in situ high-resolution synchrotron-based X-ray diffraction was applied to reveal the Li/Na/K-ion insertion-induced structural transformation mechanism during high-temperature solid-state *** in situ diffraction results demonstrate that the chemical reaction pathway strongly depends on the alkali-free precursor type,which is a structural matrix enabling phase *** phase analysis identifies for the first time the decomposition of lithium sources as the most critical factor for the formation of metastable intermediates or impurities during the entire process of Li-rich layered Li[Li_(0.2)Ni_(0.2)Mn_(0.6)]O_(2) *** the alkali ions have different ionic radii,Na/K ions tend to be located on prismatic sites in the defective layered structure(Na_(2/3-x)[Ni_(0.25)Mn_(0.75)]O_(2) or K_(2/3-x)[Ni_(0.25)Mn_(0.75)]O_(2))during calcination,whereas the Li ions prefer to be localized on the tetrahedral and/or octahedral sites,forming O-type structures.

关键词： In situ sXRD Structural evolution 3d transition-metal oxides Layered structure High-temperature solid-state reaction

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Unveiling the correlation between structural alterations and enhanced high-voltage cyclability in Na-deficient P3-type layered cathode materials via Li incorporation

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Electron 2024年第1期2卷 164-176页

作者： Xiaoxia Yang Suning Wang Hang Li Jochi Tseng Zhonghua Wu Sylvio Indris Helmut Ehrenberg Xiaodong Guo weibo hua School of Chemical Engineering and Technology Xi'an Jiaotong UniversityXi'anChina School of Chemical Engineering Sichuan UniversityChengduChina Institute for Applied Materials(IAM) Karlsruhe Institute of Technology(KIT)Eggenstein‐LeopoldshafenGermany Diffraction and Scattering Division Japan Synchrotron Radiation Research Institute(JASRI)KoutoSayo‐choSayo‐gunHyogoJapan Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijingChina

With exceptional capacity during high-voltage cycling,P3-type Nadeficient layered oxide cathodes have captured substantial ***,they are plagued by severe capacity degradation over *** this study,tuning and optimizing the phase composition in layered oxides through Li incorporation are proposed to enhance the high-voltage *** structural dependence of layered Na_(2/3)LixNi_(0.25)Mn_(0.75)O_(2)þδoxides on the lithium content(0.0≤x≤1.0)offered during synthesis is investigated systematically on an atomic ***,increasing the Li content triggers the formation of mixed P2/O3-type or P3/P2/O3-type layered *** the voltage window is 1.5-4.5 V,P3-type Na2/3Ni_(0.25)Mn_(0.75)O_(2)(NL0.0NMO,R3m)material exhibits a sequence of phase transformations throughout the process of(de)sodiation,that is,O3⇌P3⇌O30⇌O3″.Such complicated phase transitions can be effectively suppressed in the Na2/3Li_(0.7)Ni_(0.25)Mn_(0.75)O_(2.4)(NL_(0.7)NMO)oxide with P2/P3/O3-type mixed ***,cathodes made of NL0.7NMO exhibit a substantially enhanced cyclic performance at high voltages compared to that of the P3-type layered NL0.0NMO ***,NL0.7NMO demonstrates an outstanding capacity retention of 98%after 10 cycles at 1 C within 1.5-4.5 V,much higher than that of NL0.0NMO(83%).This work delves into the intricate realm of bolstering the high-voltage durability of layered oxide cathodes,paving the way for advanced sodium-ion battery technologies.

关键词： high-voltage cycling Li incorporation phase transition sodium ion batteries triphasic composites

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Na^+掺杂锂离子电池正极材料LiNi_(0.6)Co_(0.2)Mn_(0.2)O_2的制备及电化学性能

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高等学校化学学报 2017年第8期38卷 1458-1464页

作者：郑卓吴振国向伟滑纬博郭孝东四川大学高分子研究所成都610065 四川大学化学工程学院成都610065 成都理工大学材料与化学化工学院成都610059 伍伦贡大学超导与电子材料研究所

采用草酸盐共沉淀法制备了钠掺杂改性的Li_(0.98)Na_(0.02)Ni_(0.6)Co_(0.2)Mn_(0.2)O_2正极材料,借助X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、能量分散谱(EDS)、感应耦合等离子体原子发射光谱(ICP-AES)、电化学阻... 详细信息

采用草酸盐共沉淀法制备了钠掺杂改性的Li_(0.98)Na_(0.02)Ni_(0.6)Co_(0.2)Mn_(0.2)O_2正极材料,借助X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、能量分散谱(EDS)、感应耦合等离子体原子发射光谱(ICP-AES)、电化学阻抗谱(EIS)和恒电流充放电测试等手段对材料的颗粒形貌、晶体结构和电化学性能进行了研究.结果表明,掺钠后的材料具有更完善的α-NaFeO_2结构(空间群为R3m)、更低的Li^+/Ni^(2+)阳离子混排和更大的Li层间距,易于Li^+在晶格中的快速脱嵌迁移.电化学性能测试结果证实掺钠样品具有优异的循环稳定性和高倍率性能,在2.7~4.3 V,1C下循环100次后,放电比容量仍为146 mA·h/g(容量保持率为95.4%),在0.1C,0.2C,0.5C,1C,3C,5C,10C和20C时的放电比容量分别为181,168,162,155,143,136,126和113 mA·h/g.

关键词：钠掺杂正极材料锂离子扩散通道电化学性能锂离子电池

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O_(3)-NaNi_(0.4)Fe_(0.2)Mn_(0.4)O_(2)正极Na^(+)传输动力学及相变机制

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储能科学与技术 2023年第4期12卷 1011-1017页

作者：周亚男滑纬博周德重西安交通大学陕西西安710049

钠离子电池因其成本低廉、环境友好且与锂离子电池工作原理相似,在大规模储能领域极具应用潜力。作为决定电池能量密度的关键组成部分,O3型钠基层状过渡金属氧化物因高容量、合成简单等优势在众多正极材料中脱颖而出。然而,Na^(+)在O3... 详细信息

钠离子电池因其成本低廉、环境友好且与锂离子电池工作原理相似,在大规模储能领域极具应用潜力。作为决定电池能量密度的关键组成部分,O3型钠基层状过渡金属氧化物因高容量、合成简单等优势在众多正极材料中脱颖而出。然而,Na^(+)在O3结构中八面体位点间的迁移需克服较大的能垒,最终导致复杂反应相变的发生和容量快速衰减。因此,探究O3型正极材料电化学反应过程中Na^(+)脱嵌行为与结构演变的构效关系对开发高性能正极材料至关重要。本工作以O_(3)-NaNi_(0.4)Fe_(0.2)Mn_(0.4)O_(2)(O3-NFM)正极为研究对象,对其电化学性能、Na^(+)传输动力学性质及相变机制展开了系统研究。电化学测试结果表明,O3-NFM在充电至高压(4.3 V)时可脱出0.84 mol Na^(+),发挥约201.9 mAh/g的比容量,但可逆性欠佳。当截止电压为4.0 V时,该正极材料循环性能优异,原位XRD结果进一步证明了电化学反应过程中O3-P3/O3-P3-P3/O3-O3的可逆结构转变。循环伏安(CV)曲线和恒电流间歇滴定技术(GITT)结果表明其具有快速的钠离子扩散速率,从而表现出较好的倍率性能。本研究为探索以O3-NFM为基础的正极材料结构设计及性能调控提供了理论基础。

关键词：钠离子电池过渡金属氧化物 O_(3)-NaNi_(0.4)Fe_(0.2)Mn_(0.4)O_(2) 原位XRD

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Enhancing bifunctionality of CoN nanowires by Mn doping for long-lasting Zn-air batteries

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Science China Chemistry 2020年第7期63卷 890-896页

作者： Yongqi Zhang Bo Ouyang Guankui Long hua Tan Zhe Wang Zheng Zhang weibo Gao Rajdeep Singh Rawat Hong Jin Fan School of Physical and Mathematical Sciences Nanyang Technological University21 Nanyang Link637371Singapore Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731China Department of Applied Physics and Institution of Energy and Microstructure Nanjing University of Science and TechnologyNanjing 210094China Institute of Materials Research and Engineering A*STAR(Agency fo r ScienceTechnology and Research)Innovis 138634Singapore Natural Sciences and Science Education National Institute of EducationNanyang Technological UniversitySingapore 637616Singapore

Tailoring the nanostructure and composition of transition metal nitrides is highly important for their use as potent low-cost electrocatalysts. Cobalt nitride(CoN) exhibits strong catalytic activity for oxygen evolution reaction(OER). However, its poor catalytic efficiency for oxygen reduction reaction(ORR) hinders its application in rechargeable zinc-air batteries(ZABs) as the air cathode. In this work, we deploy the effective strategy of Mn doping to improve both OER and ORR activity of CoN nanowires as the cathode material for ZAB. Theoretical calculation predicts that moderate Mn doping in cobalt nitride results in a downshift of the d-band center and reduces the adsorption energy of reaction intermediates. With ~10 at% Mn dopants, stronger catalysis activities for both OER and ORR are achieved compared to pure CoN nanowires. Subsequently, both aqueous and flexible quasi-solid-state ZABs are constructed using the Mn-doped CoN nanowires array as additive-free air cathode. Both types of devices present large open circuit potential, high power density and long-cycle stability. This work pushes forward the progress in developing cost-effective ZABs.

关键词： bifunctional electrocatalyst Zn-air battery oxygen reduction reaction flexible battery plasma processing

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