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Advances in materials Physics and Chemistry 2024年第3期14卷 47-53页

作者： Fupeng Zhi Juanhui Wang Xiaomin Zhang Jun Zhang Yellow River Basin Ecotope Integration of Industry and Education research Institute Lanzhou Resources and Environment Voc-Tech University Lanzhou China national nickel and cobalt advanced materials engineering research center Lanzhou China

The high compacted density LiNi0.5-xCo0.2Mn0.3MgxO2 cathode material for lithium-ion batteries was synthesized by high temperature solid-state method, taking the Mg element as a doping element and the spherical Ni0.5Co0.2Mn0.3 (OH)2, Li2CO3 as raw materials. The effects of calcination temperature on the structure and properties of the products were investigated. The structure and morphology of cathode materials powder were analyzed by X-ray diffraction spectroscopy (XRD) and scanning electronmicroscopy (SEM). The electrochemical properties of the cathode materials were studied by charge-discharge test and cyclic properties test. The results show that LiNi0.4985Co0.2Mn0.3 Mg0.0015O2 cathode material prepared at calcination temperature 930°C has a good layered structure, and the compacted density of the electrode sheet is above 3.68 g/cm3. The discharge capacity retention rate is more than 97.5% after 100 cycles at a charge-discharge rate of 1C, displaying a good cyclic performance.

关键词： High Compacted Density Ternary Cathode materials Electrochemical Performance

Exciting lattice oxygen of nickel–iron bi-metal alkoxide for efficient electrochemical oxygen evolution reaction

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Journal of Energy Chemistry 2024年第1期88卷 194-201,I0005页

作者： Saihang Zhang Senchuan Huang Fengzhan Sun Yinghui Li Li Ren Hao Xu Zhao Li Yifei Liu Wei Li Lina Chong Jianxin Zou national engineering research center of Light Alloy Net Forming&State Key Laboratory of Metal Matrix Composites Center of Hydrogen ScienceSchool of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Department of Chemistry Laboratory of Advanced MaterialsShanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsiChEM and State Key Laboratory of Molecular Engineering of PolymersCollege of Chemistry and MaterialsFudan UniversityShanghai 200433China

High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.

关键词： Oxygen evolution reaction nickel-iron bi-metal alkoxide Lattice oxygen-mediated reaction mechanism Alkaline electrolysis Electrocatalysts

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nickel-Catalyzed Regiodivergent Acylzincation of Styrenes with Organozincs and CO

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Chinese Journal of Chemistry 2024年第6期42卷 599-604页

作者： Chenglong Wang Ning Liu Xianqing Wu Jingping Qu Yifeng Chen Key Laboratory for advanced materials and Joint International research Laboratory of Precision Chemistry and Molecular engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistrySchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai200237 China Dedicated to the Special Issue of C1 Chemistry.

Transition metal-catalyzed carbometallation of unsaturated hydrocarbons constitutes one of the most efficient synthetic methodologies for the construction of C—C bond.Recently,the incorporation of organometallic reagent with the CO gas as a nucleophilic acyl synthon could enable the acylmetallation reaction,which greatly increases the horizon of carbometallation chemistry.Herein,we report a nickel-catalyzed regiodivergent acylzincation of o-cyano cinnamate ester and o-cyano styrene,in which the cyano moiety intramolecularly captures zinc intermediates to trigger the tandem cyclization process.This protocol features mild conditions,broad substrate scope and excellent functional group tolerance,thus affording a diverse array of highly functionalized carbocyclic compounds.

关键词： Carbonylation Carbometallation Styrene nickel Cyclization

Residual alkali-evoked cross-linked polymer layer for anti-air-sensitivity LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)cathode

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Journal of Energy Chemistry 2024年第5期92卷 450-458页

作者： Chao Zhao Xuebao Li Yun Zhao Jingjing He Yuanpeng Cao Wei Luo Ding Wang Jianguo Duan Xianshu Wang Baohua Li national and Local Joint engineering research center of Lithium-ion Batteries and materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093YunnanChina School of materials Science and engineering Central South UniversityChangsha 410083HunanChina Institute of materials research Tsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen 518055Guangdong China City College Kunming University of Science and TechnologyKunming 650051YunnanChina

High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.

关键词： Lithium-ion batteries nickel-rich layered cathode Residual alkalis Cross-linked polyme rmodification Airsensitivity

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Homogenous coating of Li+ conductive Li5AlO4 on single-crystalline nonstoichiometric Li1.04Ni0.92Al0.04O2 for rechargeable lithium-ion batteries

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Journal of Energy Chemistry 2024年第8期95卷 651-659页

作者： Guoyu Ding Shizhou Wang Jinhan Li Ziyan Wu Jiayu Chen Jiayong Du Xinhui Huang Kuiming Liu Yudong Zhang Zhonghan Wu Yiyang Peng Qiancheng Zhao Meng Yu Fangyi Cheng Key Laboratory of advanced Energy materials Chemistry(Ministry of Education) Engineering Research Center of High-efficiency Energy Storage(Ministry of Education) College of Chemistry Nankai University State Key Laboratory of advanced Chemical Power Sources Nankai University Haihe Laboratory of Sustainable Chemical Transformations

cobalt-free,nickel-rich LiNi1-xAlxO2（x ≤ 0.1） is an attractive cathode material because of high energy density and low cost but suffers from severe structural degradation and poor rate performance.In this study,we propose a molten salt-assisted synthesis in combination with a Li-refeeding induced aluminum segregation strategy to prepare Li5AlO4-coated single-crystalline slightly Li-rich Li1.04Ni0.92Al0.04O2.The symbiotic formation of Li5AlO4from reaction between molten lithium hydroxide and doped aluminum in the bulk ensures a high lattice matching between the Ni-rich oxide and the homogenous conductive Li5AlO4that permits high Li+conductivity.Benefiting from mitigated undesirable side reactions and phase evolution,the Li5AlO4-coated single-crystalline Li1.04Ni0.92Al0.04O2delivers a high specific capacity of220.2 mA h g-1at 0.1 C and considerable rate capability(182.5 mA h g-1at 10 C).Besides,superior capacity retention of 90.8% is obtained at 1/3 C after 100 cycles in a 498.1 mA h pouch full cell.Furthermore,the particulate morphology of Li1.04Ni0.92Al0.04O2remains intact after cycling at a cutoff voltage of 4.3 V,whereas slightly Li-deficient Li0.98Ni0.97Al0.05O2features intragranular cracks and irreversible lattice distortion.The results highlight the value of molten salt-assisted synthesis and Li-refeeding induced elemental segregation strategy to upgrade Ni-based layered oxide cathode materials for advanced Li-ion batteries.

关键词： Aluminum segregation Cathode materials Molten synthesis Nonstoichiometric oxides Surface coating

Optimal geometrical configuration and oxidation state of cobalt cations in spinel oxides to promote the performance of Li-O_(2) battery

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Nano research 2024年第1期17卷 221-227页

作者： Yu Zhang Shuting Zhang Mengwei Yuan Yufeng Li Rong Liu Caiyun Nan Chen Chen engineering research center of advanced Rare Earth materials Department of ChemistryTsinghua UniversityBeijing 100084China Beijing Key Laboratory of Energy Conversion and Storage materials Institution College of ChemistryBeijing Normal UniversityBeijing 100875China X-ray diffraction Lab Analytical and Testing CenterBeijing Normal UniversityBeijing 100875China

Co_(3)O_(4) is considered as one of promising cathode catalysts for lithium oxygen(Li-O_(2))batteries,which contains both tetrahedral Co^(2+)sites(Co^(2+)Td)and octahedral Co^(3+)sites(Co^(3+)Oh).It is important to reveal the effect of optimal geometric configuration and oxidation state of cobalt ion in Co_(3)O_(4) to improve the performance of Li-O_(2) batteries.Herein,through regulating the synthesis process,Co^(2+)and Co^(3+)sites in Co_(3)O_(4) were replaced with Zn and Al atoms to form materials with a unique Co site.The Li-O_(2) batteries based on ZnCo_(2)O_(4) showed longer cycle life than that of CoAl_(2)O_(4),suggesting that in Co_(3)O_(4),the Co^(3+)Oh site is a relatively better geometric configuration than Co^(2+)Td site for Li-O_(2) batteries.Theoretical calculations revealed that Co^(3+)Oh sites provide higher catalysis activity,regulating the adsorption energy of the intermediate LiO_(2) and accelerating the kinetics of the reaction in batteries,which further leads to the change of the morphology of the discharge product and ultimately improves the electrochemical performance of the batteries.

关键词： lithium oxygen(Li-O_(2))batteries geometrical configuration oxidation state lithium peroxide

Heterointerface engineering of assembled CoP_(2) on N-modified carbon as efficient trifunctional electrocatalysts for Zn-Air batteries and overall water splitting

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Nano research 2024年第5期17卷 3801-3809页

作者： Yan Chen Zhenrui Yang Juan Wang Yun Yang Xuedong He Yang Wang Jiadong Chen Yaqing Guo Xin Wang Shun Wang Huile Jin Wenzhou Key Lab of advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Zhejiang engineering research center for Electrochemical Energy materials and Devices Institute of New Materials and Industrial TechnologiesWenzhou UniversityWenzhou 325035China School of Chemical and Biomedical engineering Nanyang Technological UniversitySingapore 637459Singapore

Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.

关键词： two-dimensional(2D)carbon metal-organic framework cobalt phosphide zinc air battery water splitting

Development of anti-corrosive coating on AZ31 Mg alloy modified by MOF/LDH/PEO hybrids

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Journal of Magnesium and Alloys 2024年第2期12卷 586-607页

作者： Muhammad Ali Khan Ananda Repycha Safira Mohammad Aadil Mosab Kaseem Corrosion and Electrochemistry Laboratory Department of Nanotechnology and Advanced Materials EngineeringSejong UniversitySeoul 05006Republic of Korea

The self-assembly of hybrid inorganic-organic materials on stationary platforms plays a critical role in improving their structural stability and wide usability.In this work,a novel two-step hydrothermal approach is proposed for synthesizing stable and advanced hybrid coatings on metal-oxide platforms through the surface modification of layered double hydroxide(LDH)films using novel metal-organic frameworks(MOFs).Initially,Mg-Al LDH nanocontainers,grown on a magnesium oxide layer produced through plasma electrolytic oxidation(PEO)of AZ31 Mg alloy substrate,were intercalated with cobalt via an oxidation route,providing the metallic coordination center for the MOF formation.In the subsequent step,a pioneering technique is introduced,utilizing tryptophan as the organic linker for the first time at a pH of 10.The self-assembly of cobalt-tryptophan complex,driven by the strong bonding between electrophilic sites of monomers and nucleophilic sites,facilitated the formation of a MOF network having a cloud-like structure on the surface of MgAl LDH's film.The resulting MOF-LDH encapsulation containers demonstrate exceptional electrochemical stability when exposed to a 3.5 wt.%NaCl solution,surpassing the performance of PEO and pure LDH coatings.This enhanced stability is attributed to the development of a dense top layer and a stable composition within the self-assembled MOF,effectively sealing flaws and preventing the infiltration of corrosive ions into the underlying metallic substrate.The formation mechanism of MOFs on LDH galleries is investigated using density functional theory calculations.

关键词： Mg alloy Layered double hydroxide Metal-organic frameworks Corrosion DFT

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Tribological properties and tribomechanism of nickel nanoparticles in-situ synthesized in rapeseed oil

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Friction 2024年第3期12卷 474-489页

作者： Wenya XU Guangbin YANG Shengmao ZHANG Jun XU Yujuan ZHANG Tianhua SUN Ningning SONG Laigui YU Pingyu ZHANG engineering research center for Nanomaterials Henan UniversityKaifeng 475004China State Key Laboratory of Tribology in advanced Equipment Tsinghua UniversityBeijing 100084China

nickel(Ni)nanoparticles can be enriched on the surface of iron-based frictional pairs,which provides the possibility to get rid of the competitive adsorption between the polar species of vegetable oil and the surface-active nano-additives thereon.In this paper,nickel acetylacetonate was used as a precursor to in-situ synthesize nickel nanoparticles with an average diameter of about 12 nm in rapeseed oil(RO)as the reducing agent,surface modifier,and solvent as well.The tribological properties of the as-synthesized Ni nanoparticles were evaluated with a four-ball tribometer,and their tribomechanism was investigated based on the characterizations of the tribofilm on rubbed steel surfaces by the scanning electron microscopy(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).It was found that the Ni nanoparticles in-situ prepared in the RO with a mass fraction of 0.3%can reduce the wear scar diameter(WSD)of the steel ball by 36%.This is because,on the one hand,the Ni nanoparticles are adsorbed on the rubbed steel surfaces to repair or fill up the micro-pits and grooves thereon.On the other hand,Ni nanoparticles participate in tribochemical reactions with atmospheric O and steel substrate to form the tribochemical reaction film on the rubbed steel surfaces with the assistance of friction-induced heat and applied normal load.In addition,an amorphous carbon film is formed on the rubbed surface via the carbonization of base oil under the catalysis of Ni nanoparticles.The adsorbed Ni layer,the tribochemical reaction film,and the carbon layer comprise a composite tribofilm composed of amorphous carbon,polar fatty acid,metallic nickel,iron oxides,and nickel oxides on the rubbed steel surfaces,which contributes to significantly improving the antiwear ability and load-carrying capacity of the RO for the steel-steel sliding pair.

关键词： nickel(Ni)nanoparticles rapeseed oil(RO) in-situ synthesis tribological properties tribomechanism

A general and facile calcination method to synthesize single-site catalysts for highly efficient electrochemical CO_(2) reduction

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Nano research 2024年第5期17卷 3895-3901页

作者： Rui Sui Bingyan Wang Yongsheng Wang Jiajing Pei Wei Zhu Wenxing Chen Chunhui Li Ailing Sun Zhongbin Zhuang engineering research center of advanced Rare Earth materials Department of ChemistryTsinghua UniversityBeijing 100084China College of Chemistry and Green Catalysis center Zhengzhou UniversityZhengzhou 450001China State Key Lab of Organic-Inorganic Composites and Beijing advanced Innovation center for Soft Matter Science and engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Energy&Catalysis center School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

The electrochemical CO_(2) reduction reaction(CO_(2)RR)has received widespread attention as a promising method for producing sustainable chemicals and mitigating the global warming.Here,we demonstrate a general and facile synthetic route for the metal-nitrogen-carbon(M-N-C)type catalyst by simply calcinating metal acetate and urea with commercial carbon black,which have potential application in CO_(2)RR.The synthesized Ni-NC-600 catalyst has the structure of single Ni atom coordinated with one N atom and three C atoms(Ni-N_(1)C_(3)),which is suggested by X-ray absorption spectroscopy.The Ni-NC-600 catalyst exhibits high CO_(2)RR catalytic performance and a high CO Faraday efficiency above 98%in a wide potential range from-0.7 to-1.3 V(vs.reversible hydrogen electrode(RHE)),superior to most of the reported Ni-N-C catalysts.This work has developed a facile strategy to synthesize high performance CO_(2)RR catalyst.

关键词： nickel single atom catalyst CO_(2)reduction reaction CO production electrocatalyst