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Self-supported NiFe-LDH nanosheets on NiMo-based nanorods as high-performance bifunctional electrocatalysts for overall water splitting at industrial-level current densities

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Nano Research 2024年第5期17卷 3769-3776页

作者： Yan Zhang Biao Feng MingLei Yan Zhen Shen Yiqun Chen Jingyi Tian Fengfei Xu Guanghai Chen Xizhang Wang Lijun Yang Qiang Wu Zheng Hu Key lab.ratory of Mesoscopic chemistry of Ministry of Education(MOE)and Jiangsu Provincial lab.for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China College of Water Conservancy and Hydropower Engineering Sichuan Agricultural UniversityYa’an 625014China

Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis ***,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 *** outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D ***,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both *** study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.

关键词： alkaline water splitting bifunctional electrocatalysts layered double hydroxides high durability industrial current densities

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Metal-metal bonds in Zintl clusters:Synthesis,structure and bonding in[Fe_(2)Sn_(4)Bi_(8)]^(3-)and[Cr_(2)Sb_(12)]^(3-)

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Chinese Chemical Letters 2024年第8期35卷 558-566页

作者： Ya-Nan Yang Zi-Sheng Li Sourav Mondal Lei Qiao Cui-Cui Wang Wen-Juan Tian Zhong-Ming Sun John E.McGrady State Key lab.ratory of Element-Organic chemistry Tianjin Key Lab for Rare Earth Materials and ApplicationsSchool of Materials Science and EngineeringNankai UniversityTianjin 300350China Department of chemistry University of OxfordInorganic Chemistry LaboratoryOxfordOX13QRUnited Kingdom

We report here the synthesis and characterization of two new members of the M2 E 12 family of endohe-dral Zintl clusters,[Fe_(2)Sn_(4)Bi_(8)]^(3-)and[Cr_(2)Sb_(12)]^(3-),both of which contain open-shell metal dimers encap-sulated inside a triple-decker cluster of main-group *** 75-electron[Fe_(2)Sn_(4)Bi_(8)]^(3-)cluster has a D4h-symmetric structure,while[Cr_(2)Sb_(12)]^(3-),despite having the same 75-electron count,is strongly dis-torted to a geometry that resembles a CrSb_(8)crown capped by a CrSb_(4)*** structural differences between the two are driven by the increasing availab.lity of 3d electron density in the earlier transi-tion metal,which leads,ultimately,to different electronic configurations in the two *** trends precisely mirror those observed in the ME_(10)and ME_(12)families containing a single transition metal ion.

关键词： Zintl anions Endohedral clusters Metal-metal bond Second-order Jahn-Teller effect DFT calculation

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The Current Progress and Challenges of Carbonized Polymer Dot-Based Room-Temperature Phosphorescent Materials

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CCS chemistry 2024年第3期6卷 604-622页

作者： Chengyu Zheng Songyuan Tao Bai Yang State Key lab.of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012

Carbonized polymer dots(CPDs)as one type of carbon dots have attracted widespread attention in recent *** proposal of the“shell–core”structure of CPDs leads to further thinking about the association between their special structures and luminescent *** recent years,great progress has been made in the field of CPD-based room-temperature phosphorescent *** review pays particular attention to how the special“core–shell”structure of CPDs influences the activation of roomtemperature phosphorescence(RTP).The strategies and vital factors to activate RTP for CPD-based materials in both solid state and water were reviewed in detail to elab.rate on the effect of the special structure on RTP ***,some perspectives on the current challenges were also provided to guide the further development of CPD-based room-temperature phosphorescent materials.

关键词： room-temperature phosphorescent materials carbon dots carbonized polymer dots “core-shell”structure photoluminescent mechanism

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Injection molding of highly filled microcrystalline cellulose/polycaprolactone composites with the aid of reversible Diels-Alder reaction

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Journal of Materials Science & Technology 2024年第3期170卷 246-254页

作者： Ze Pu Wang WenHong Ruan MinZhi Rong MingQiu Zhang Key lab.ratory for Polymeric Composite and Functional Materials of MOE GD HPPC LabIGCMESchool of ChemistrySun Yat-Sen UniversityGuangzhou 510275China

To tackle the challenge of producing highly filled polymer composites using the traditional injection molding technique,which is characterized by the fairly high melt viscosity that makes mold filling difficult,the authors propose a solution based on dynamic covalent *** demonstrated by the proof-of-concept experiments,the 4-arm starshaped polycaprolactone(PCL)oligomers and microcrystalline cel-lulose(MCC)are crosslinked by the reversible Diels-Alder(DA)*** flowability of the compounds greatly decreases due to the dissociation of the intercomponent DA bonds at the retro-reaction tempera-ture,and the networked architecture is reconstructed during cooling as a result of the forward DA ***,the high-loading MCC fillers are well distributed in the matrix and covalently bonded to the nearby PCL,forming a striking contrast to the control in which linear PCL acts as the *** DA bonds crosslinked biodegradable PCL composites exhibit decent mechanical strength(20.7 MPa)even at the MCC fraction of 65 wt%,which is superior to those(5-12.2 MPa)of the highly filled PCL composites(with filler contents of 50-63.8 wt%)reported so *** proposed approach has sufficient expansibility for the fabrication of the highly filled polymer composites constructed by other types of matrix and fillers.

关键词： Polymer composites Microcrystalline cellulose Polycaprolactone Injection molding Dynamic reversible chemistry

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Thermally Conductive,Healab.e Glass Fiber Cloth Reinforced Polymer Composite based onβ-Hydroxyester Bonds Crosslinked Epoxy with Improved Heat Resistance

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Chinese Journal of Polymer Science 2024年第5期42卷 643-654,I0009页

作者： Fang Chen Xiao-Yan Pang Ze-Ping Zhang Min-Zhi Rong Ming-Qiu Zhang Key lab.ratory for Polymeric Composite and Functional Materials of Ministry of Education GD HPPC LabIGCMESchool of ChemistrySun Yat-sen UniversityGuangzhou510275China Guangdong Provincial lab.ratory of chemistry and Fine Chemical Engineering Jieyang Center Jieyang515200China

To simultaneously endow thermal conductivity,high glass transition temperature(Tg)and healing capability to glass fiber/epoxy(GFREP)composite,dynamic crosslinked epoxy resin bearing reversibleβ-hydroxyl ester bonds was reinforced with boron nitride nanosheets modified glass fiber cloth(GFC@BNNSs).The in-plane heat conduction paths were constructed by electrostatic self-assembly of polyacrylic acid treated GFC and polyethyleneimine decorated ***,the GFC@BNNSs were impregnated with the mixture of lower concentration(3-glycidyloxypropyl)trimethoxysilane grafted BN micron sheets,3,4-epoxycyclohexylmethyl 3,4-epoxycyclohexanecarboxylate and hexahydro-4-methylphthalic anhydride,which accounted for establishing the through-plane heat transport pathways and avoiding serious deterioration of mechanical *** resultant GFREP composite containing less boron nitride particles(17.6 wt%)exhibited superior in-plane(3.29 W·m^(-1)·K^(-1))and through-plane(1.16 W·m^(-1)·K^(-1))thermal conductivities,as well as high Tg of 204℃(Tg of the unfilled epoxy=177℃).The reversible transesterification reaction enabled closure of interlaminar cracks within the composite,achieving decent healing efficiencies estimated by means of tensile strength(71.2%),electrical breakdown strength(83.6%)and thermal conductivity(69.1%).The present work overcame the disadvantages of conventional thermally conductive composites,and provided an efficient approach to prolong the life span of thermally conductive GFREP laminate for high-temperature resistant integrated circuit application.

关键词： Thermally conductive composites Boron nitride High-temperature resistance β-Hydroxyl ester bond Healing

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Synthesis,Characterization of Polyethylene Ionomers and Their Antibacterial Properties

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Chinese Journal of Polymer Science 2024年第8期42卷 1077-1084页

作者： Jia-Jia Wu Fei Wang Peng-Qi Wan Li Pan Chun-Sheng Xiao Zhe Ma Yue-Sheng Li Tianjin Key lab.Composite&Functional Materials School of Materials Science and EngineeringTianjin UniversityTianjin 300350China Key lab.Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Owing to its high production volume and wide range of application s,polyethylene has gained a great deal of attention,but its low surface energy and non-polar nature have limited its application in some important *** this study,ethylene/11-iodo-1-undecene copolymers were prepared and used as the intermediates to afford a series of imidazolium-based ionomers bearing methanesulfonate(CH_(3)SO_(3)^(-)),trifluoromethanesulfonate(CF_(3)SO_(3)^(-)),or bis(trifluoromethane)sulfonimide(Tf_(2)N^(-))*** tensile test results showed that the stress-at-break(7.8-25.6 MPa)and the elongation-at-break(445%-847%)of the ionomers could be adjusted by changing the counterion species and the ionic group *** importantly,the ionomers exhibited marvelous antibacterial activities against Staphylococcus aureus(***)and Escherichia coli(***).The ionomers bearing Tf_(2)N^(-)exhibited antibacterial activities>99%against both *** and *** when ionic content reached 9.1%.The imidazolium-based ionomers prepared in this work demonstrated excellent comprehensive properties,especially highefficient and broad-spectrum antibacterial ability,exhibiting the potential fo r the application as the antibacterial materials in packaging,medical,and other fields.

关键词： Polyethylene Ionomer Polymerization catalysis Imidazolium Antibacterial material

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Recent progress of in situ/operando characterization techniques for electrocatalytic energy conversion reaction

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Chinese Chemical Letters 2024年第9期35卷 92-101页

作者： Zhao Li Huimin Yang Wenjing Cheng Lin Tian School of Materials and Chemical Engineering Xuzhou University of TechnologyXuzhou 221018China University and College Key lab.of Natural Product chemistry and Application in Xinjiang School of Chemistry and Environmental ScienceYili Normal UniversityYining 835000China

Catalysts can significantly promote the reaction dynamics and are therefore considered crucial components for achieving high electrochemical energy conversion ***,the active sites of the catalysts,particularly for nano-level and atomic-level catalysts commonly undergo reconstruction under practical ***,obtaining an in-depth and systematic understanding on the real active sites through in situ/operando characterization techniques is a prerequisite for establishing the structureperformance relationship and guiding the future design of more efficient ***,we summarize the recent progress of in situ/operando characterization techniques for identifying the nature of active sites of electrocatalysts when used in electrocatalytic energy conversion ***,our focus lies in the fundamental principles of various in situ/operando characterization techniques,with particular emphasis on their applications for electrocatalytic *** that,the challenges and perspective insights are also added in the final section to highlight the future direction of this important field.

关键词： In situ techniques Electrocatalysis Active sites Energy conversion

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Ir single atoms on NiFeZn-LDH matrix for exceptional oxygen evolution reaction

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Nano Research 2024年第8期17卷 7039-7044页

作者： Muhammad Israr Muhammad Humayun Jiaqi Zhang Khadim Shah Xin Tan Chen Chen Yadong Li Department of chemistry Tsinghua UniversityBeijing 100084China Energy Water and Environment LabCollege of Humanities and SciencePrince Sultan UniversityRiyadh11586Saudi Arabia

To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabilize single-atom active centers with optimal geometric and electronic structures is crucial for enhancing catalytic ***,we report the design and fabrication of Ir single atoms on NiFeZn layered double hydroxide(Ir-SAC/NiFeZn-LDH)electrocatalyst for highly efficient and stable *** is investigated that the NiFeZn support exhibits abundant defect sites and unsaturated coordination *** sites function to anchor and stabilize single Ir single atoms on the *** strong synergetic electronic interaction between the Ir single atoms and the NiFeZn matrix resulted in remarkable OER performance of the as-fabricated Ir-SAC/NiFeZn *** a loading Ir content of 1.09 wt.%,this catalyst demonstrates a highly stable OER activity,with an overpotential of 196 mV at 10 mA·cm^(−2) and a small Tafel slope of 35 mV·dec^(−1) for the OER in a 1 M KOH *** results significantly surpass the performance of the commercially availab.e IrO_(2) catalyst.

关键词： Ir single atoms layered double hydroxides rational design geometric optimization oxygen evolution reaction

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From charge storage mechanism to performance:A strategy toward boosted lithium/sodium storage through heterostructure optimization

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Journal of Energy chemistry 2024年第1期88卷 112-124,I0003页

作者： Xiaoke Zhang Guangfa Deng Mianying Huang Zhaohui Xu Jianlin Huang Xuan Xu Zhiguang Xu Maochan Li Lei Hu Xiaoming Lin Key lab.ratory of Theoretical chemistry of Environment Ministry of EducationSchool of ChemistrySouth China Normal UniversityGuangzhou 510006GuangdongChina Anhui lab.ratory of Functional Coordinated Complexes for Materials chemistry and Application School of Chemical and Environmental EngineeringAnhui Polytechnic UniversityWuhu 241000AnhuiChina National Engineering Research Center for Carbohydrate Synthesis Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of EducationJiangxi Normal UniversityNanchang 330022JiangxiChina

Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent *** this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and *** optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active ***_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in *** functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical *** heterostructure building technique may pave the way for the development of high-performance LIBs and ***,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.

关键词： Metal-organic framework Heterostructure Lithium-ion batteries Sodium-ion batteries DFT calculation

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Real-time identification of multiple nanoclusters with a protein nanopore in single-cluster level

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Nano Research 2024年第1期17卷 262-269页

作者： Ling Zhang Peilei He Huang Chen Qingda Liu Libo Li Xun Wang Jinghong Li Department of chemistry Center for BioAnalytical ChemistryKey Laboratory of Bioorganic Phosphorus Chemistry&Chemical BiologyTsinghua UniversityBeijing 100084China School of chemistry and Chemical Engineering Guangdong Prov Key Lab Green Chem Prod TechnolSouth China University of TechnologyGuangzhou 510640China New Cornerstone Science lab.ratory Shenzhen 518054China Beijing Institute of Life Science and Technology Beijing 102206China Center for BioAnalytical chemistry Hefei National Laboratory of Physical Science at MicroscaleUniversity of Science and Technology of ChinaHefei 230026China

It is important and challenging to analyze nanocluster structure with atomic ***,α-hemolysin nanopore was used to identify nanoclusters at the single molecule level by providing two-dimensional(2D)dwell time–current blockage spectra and translocation event frequency which sensitively depended on their *** such as Anderson,Keggin,Dawson,and a few lacunary Dawson polyoxometalates with very similar structures,even with only a two-atom difference,could be *** nanopore device could simultaneously measure multiple nanoclusters in a mixture qualitatively and ***,molecular dynamics(MD)simulations provided microscopic understandings of the nanocluster translocation dynamics and yielded 2D dwell time–current blockage spectra in close agreement with *** nanopore platform provides a novel powerful tool for nanocluster characterization.

关键词： nanopore single-molecule nanocluster polyoxometalates real-time detection

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