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Lowering the kinetic barrier via enhancing electrophilicity of surface oxygen to boost acidic oxygen evolution reaction

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Chinese Journal of Structural Chemistry 2024年第11期43卷 4-5页

作者： Ling Tang Yan Wan Yangming Lin CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen361021China

Oxygen evolution reaction(OER)is of significance in anodic reaction in the field of electrochemical energy conversion and storage,such as water splitting,metal-air battery,etc.[1,2].Being a thermodynamically downhill reaction comprising multiple-step proton coupled electron transfer within a narrow potential range(equations(1)-(5)),the reaction pathways involved in OER highly depend on the pH value of electrolyte[3,4].

关键词： narrow electrolyte anodic

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Modulator-directed assembly of hybrid composites based on metalorganic frameworks and upconversion nanoparticles

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Nano Research 2023年第1期16卷 1482-1490页

作者： Yanhui Feng Xingjun Li Shan Lu Renfu Li Zhongliang Gong Xiaoying Shang Yifan Pei Wei Zheng Datao Tu Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of chemistry Fuzhou universityFuzhou 350108China Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117China

Hybrid composites made of metal-organic frameworks(MOFs)and lanthanide-doped upconversion nanoparticles(UCNPs)have attracted considerable interest for their synergistically enhanced functions in various applications such as chemical sensing,photocatalysis,anticounterfeiting and ***,precise assembly of MOF/UCNP hybrid composites with tunable morphologies remains a challenge due to the lack of effective synthetic methods and fundamental understanding of the growth ***,we propose a modulator-directed assembly strategy to synthesize a series of ZIF-8@UCNP composites(ZIF-8=zeolitic imidazolate framework-8).The UCNPs densely paved on the surface of ZIF-8 microcrystals and endowed the composites with intense upconversion blue emission,which were verified by steady-state/transient photoluminescence(PL)spectroscopy and single-particle ***(EDA)was firstly used as a modulator to fine-tune the predominant MOF facets and realized distinct morphologies of the *** adjusting the concentration of EDA from 0 to 25 mmol/L,the morphology of the ZIF-8@UCNP composites was tuned from rhombic dodecahedron(RD)to truncated rhombic dodecahedron(TRD),cube with truncated edges(CTE),cube,and finally a unique form of interpenetration twins(IT).The nucleation and growth process of the ZIF-8@UCNP composites was monitored by time-dependent scanning electron microscopy(SEM)images and the formation mechanism was thoroughly ***,we demonstrated that the strategy for assembly of morphology-controllable ZIF-8@UCNP composites was generally applicable to various UCNPs with different sizes and *** proposed strategy is expected to open up new avenues for the controllable synthesis of MOF/UCNP composites toward diverse applications.

关键词： metal-organic frameworks upconversion nanoparticles hybrid composites ethylenediamine modulator

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Organic polystyrene and inorganic silica double shell protected lead halide perovskite nanocrystals with high emission efficiency and superior stability

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Nano Research 2023年第7期16卷 10507-10514页

作者： Shujian Wang Dejian Chen Kunyuan Xu Jie Hu Decai Huang Maochun Hong Haomiao Zhu University of Science and Technology of China Hefei 230026China Ganjiang Innovation Academy Chinese Academy of SciencesGanzhou 341000China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of Nanomaterials Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Research Center of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen 361021China

The practical application of all-inorganic semiconductor lead halide perovskite nanocrystals(LHP NCs)has been limited by their poor ***,a lot of research on core-shell structure has been done to improve the stability of perovskite NCs,but the effect was far from the application ***,we,for the first time,report a convenient approach to synthesize organic-inorganic double shell CsPbBr_(3)@SiO_(2)@polystyrene(PS)NCs with an inter-core of CsPbBr_(3),the intermediate layer of SiO_(2)shell,and outmost PS ***,the CsPbBr_(3)@SiO_(2)@PS NCs maintained more than 90%of their initial photoluminescence(PL)intensity under one month's ultraviolet lamp irradiation or in 85℃ and 85%relative humidity(RH)*** white-light-emitting-diodes(WLEDs)were fabricated by encapsulating commercial InGaN chip with CsPbBr_(3)@SiO_(2)@PS NCs and K2SiF6:Mn^(4+)(KSF:Mn^(4+))phosphor with a luminous efficacy of~100 lm/W at 20 mA current and a color gamut of 128%of the National Television Standards Committee(NTSC)*** addition,these WLEDs still maintain 91%of the initial luminous efficacy after 1200 h of continuous *** results demonstrated that double shell-protected CsPbBr_(3)perovskite NCs have great potential in the field of WLEDs.

关键词： core-shell structure organic polystyrene(PS)inorganic SiO_(2)double shell CsPbBr_(3)@SiO_(2)@PS nanocrystals(NCs) high stability

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ZnMn_(3)O_(7):A New Layered Cathode Material for Fast-Charging Zinc-Ion Batteries

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Chinese Journal of Structural Chemistry 2022年第5期41卷 85-92页

作者： Ruitao Sun Qin Liu Wenzhuo Deng CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsState Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China University of Chinese Academy of Sciences Beijing 100039China

Low-cost and high-energy-density manganese-based compounds are promising cathode materials for rechargeable aqueous zinc-ion batteries(AZIBs),however,they often experience cycling instability issues and inferior rate ***,we report a new layered manganese-based cathode material,ZnMn_(3)O_(7)(ZMO),which possesses a large interlayer spacing of 4.8Åand allows the intercalation of~1.23 Zn-ions per formula unit(corresponding to a capacity of~170 mAh/g).Importantly,ZMO exhibits good cycling stability(72.9%capacity retention over 400 cycles),ultrafast-charging capability(73%state of charge in 1.5 min),and an ultrahigh power density(3510 W/kg at 88 Wh/kg).Through kinetic characterization,the favorable diffusion of ions and the dominant capacitor contribution are found to be conducive to the achievement of superior fast charging ***,the charge storage mechanism is revealed by ex-situ XRD and ex-situ *** work may shed light on the design of high-performance electrode materials for AZIBs.

关键词： layered structure zinc-manganese oxide cathode zinc-ion battery

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Protective layer for stable lithium-metal anodes at 60 mA·h/cm^(2) and 60 mA/cm^(2) with ion channel and inductive effect

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Journal of Materiomics 2024年第6期10卷 1252-1260页

作者： Xiao Zhang Zhiwei Chen Jiaojiao Han Qiang Wang Jinshan Wang Juhua Luo Jianguang Xu Chi Chen Wei Yao School of Materials Science and Engineering Jiangsu Provincial Key Laboratory of Eco-Environmental MaterialsYancheng Institute of TechnologyYancheng 224051China School of Materials and Energy Shanghai Key Laboratory of Engineering Materials Application and EvaluationShanghai Polytechnic UniversityShanghai 201209China CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials and Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021China

Contradiction between ultrafast nucleation and deposition rates of lithium(Li)crystals at high rate and heterogeneity of Li^(+)flux resulting from concentration polarization has compromised the performance of Li metal anodes especially at high areal capacity and current ***,multifunctional protective layer consisting of MoO_(3) nanobelt films(MoO_(3)-NF)is introduced on the surface of Li by a simple rolling *** strong binding energy between Li and MoO_(3) guides the homogeneous nucleation and deposition of Li,while the nanobelt networks provide effective ion channels for uniform distribution of the Li+*** of the novel multifunctional protective layer,the MoO_(3)-NF@Li anodes demonstrate a remarkable stability for 800 h with ultralow overpotential of 159 mV at extreme harsh conditions of 60 mA·h/cm^(2) and 60 mA/cm^(2).MoO_(3)-NF@Li||LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2) full-cells can run 100 cycles with a superior capacity retention of 84.2%under practical test conditions,demonstrating great potential for high output and energy-density metal batteries.

关键词： Multifunctional protective layer Ion channel Inductive effect High areal capacity Li metal anodes

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Synergic catalysis of W and Ni originating from substitution of trivacant phosphotungstate for the selective oxidation of aniline to azoxybenzene

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Chinese Chemical Letters 2024年第2期35卷 558-563页

作者： Sheng Cai Xiao-Yuan Wu Weiming Wu Sa-Sa Wang Can-Zhong Lu CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Provincial Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry and Materials Science Fujian Normal UniversityFuzhou 350117China Xiamen Institute of Rare Earth Materials Chinese Academy of SciencesXiamen 361021China University of Chinese Academy of Sciences Beijing 100049China

Partial substitution of polyoxometalate(POM)is an efficient route to modulate the catalytic property of maternal *** this work,a new Keggin type POM involving{Ni 6}cluster,{[Ni(H_(2)O)_(2)(Dach)_(2)][Ni(Dach)_(2)]_(2)}{[Ni_(6)Cl(μ-OH)_(3)(H_(2)O)(Dach)_(3)(WO_(4))(PW9 O_(3)_(4))][Ni_(6)(μ-OH)_(3)(H_(2)O)_(2)(Dach)_(3)(WO_(4))(PW9 O_(3)_(4))]}Cl·27H_(2)O,(1,Dach=1,2-diaminocyclohexane)was *** 1 shows excellent catalytic performance in the selective oxidation of aniline to azoxybenzene(AOB)in *** apparently different results from that with the matrix{PW_(9)O_(34)}({PW9})suggest the successful regulation of the catalytic property of{PW9}by the introduction of the{Ni6}cluster into the *** experimental results indicate that the highlighted performance of 1 is contributed by the synergy of W and Ni sites,which are respectively responsible for the oxidation and condensation steps in the production of *** good selectivity to AOB is essentially attributed to the effective modulation of the reaction rates of oxidation and condensation steps by W and Ni sites,respectively.

关键词： Polyoxometalate {Ni_(6)}cluster Modulated catalytic property Aniline oxidation Azoxybenzene

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Unlimited near-infrared photoswitching in inorganic photon avalanching nanocrystals

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Science China Materials 2023年第8期66卷 3379-3380页

作者： Jin Xu Guoqin Ma Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of NanomaterialsState Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China Fujian College University of Chinese Academy of SciencesFuzhou 350116China

Luminescent materials capable of photoswitching driven by optical stimulation have been the robust tools of diverse advanced technologies,including superresolution imaging,nanophotonics,data storage,and optogenetics[1].Up to date,various kinds of photoswitchable materials have been developed,most of which(e.g.,organic fluorophores and proteins)are prone to photodegradation and usually operate in the ultraviolet or visible spectral regions[2].Near-infrared(NIR)light excitable inorganic upconversion nanocrystals(NCs)can offer significantly improved photostability and penetration depth.

关键词： inorganic ultraviolet visible

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Recent Advances in Mechanistic Understanding of Metal-Free Carbon Thermocatalysis and Electrocatalysis with Model Molecules

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Nano-Micro Letters 2024年第7期16卷 74-97页

作者： Wei Guo Linhui Yu Ling Tang Yan Wan Yangming Lin CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstituteChinese Academy of SciencesXiamen 361021People’s Republic of China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002People’s Republic of China Institute of Urban Environment Chinese Academy of SciencesXiamen 361021People’s Republic of China

Metal-free carbon,as the most representative heterogeneous metal-free catalysts,have received considerable interests in electro-and thermo-catalytic reac-tions due to their impressive performance and *** the past decade,well-designed carbon catalysts with tunable structures and heteroatom groups coupled with various characterization techniques have proposed numerous reaction ***,active sites,key intermediate species,precise structure-activity relationships and dynamic evolution processes of carbon catalysts are still rife with controversies due to the monotony and limitation of used experimental *** this Review,we sum-marize the extensive efforts on model catalysts since the 2000s,particularly in the past decade,to overcome the influences of material and structure limitations in metal-free carbon *** both nanomolecule model and bulk model,the real contribution of each alien species,defect and edge configuration to a series of fundamentally important reactions,such as thermocatalytic reactions,electrocatalytic reactions,were systematically *** with in situ techniques,isotope labeling and size control,the detailed reaction mechanisms,the precise 2D structure-activity relationships and the rate-determining steps were revealed at a molecular ***,the outlook of model carbon catalysis has also been proposed in this work.

关键词： Metal-free carbon catalysts Model catalyst Electrocatalysis Active site Reaction mechanisms

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Recent progress, challenges and prospects of electrolytes for fluoride-ion batteries

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Energy Reviews 2024年第3期3卷 102-128页

作者： Ming Zhang Xiaocao Cao Yaowei Hao Haodong Wang Jian Pu Bo Chi Zhongrong Shen CAS Key Laboratory of Design and Assembly of Functional Nanostructures and Fujian Key Laboratory of NanomaterialsFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou350002China Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials Xiamen Institute of Rare Earth MaterialsHaixi InstitutesChinese Academy of SciencesXiamen361021China College of Chemical Engineering Fuzhou UniversityFuzhouFujian350116China School of Materials Science and Engineering State Key Laboratory of Material Processing and Die&Mould TechnologyHuazhong University of Science and TechnologyWuhan430074China

In the development of new electrochemical concepts for the fabrication of high-energy-density batteries,fluorideion batteries(FIBs)have emerged as one of the valid candidates for the next generation electrochemical energy storage technologies,showing the potential to match or even surpass the current lithium-ion batteries(LIBs)in terms of energy density,safety without dendritic grains,and elimination of dependence on scarce lithium and cobalt ***,the development of FIBs is still in its infancy and their performance is far from satisfactory,with issues such as the lower fluoride-ion conductivity of the electrolytes and the reversibility of the electrodes hindering their *** reviews have mainly focused on inorganic solid electrolytes with a brief emphasis on the development of various fluoride-ion conductors and their ion-conducting ***,this review summarizes the current developments in various electrolytes,a systematic overview of the current progress for various fluoride-ion electrolytes is presented by beginning with the history,structure and classification of FIBs,ion-transport mechanisms are briefly *** advances in different classes of fluoride-ion electrolytes are *** methods for optimizing the ionic conductivity characteristics of the fluoride-ion electrolytes are ***,an outlook on the future research direction of FIBs is given by highlighting some critical issues,challenges and prospects of fluoride-ion electrolytes.

关键词： Solid electrolyte Liquid electrolyte Composited electrolyte Fluoride-ion Conductivity

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Unraveling the triplet excited-state dynamics of Bi^(3+)in vacancyordered double perovskite Cs_(2)SnCl_(6) nanocrystals

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Nano Research 2022年第7期15卷 6422-6429页

作者： Mengyao Jin Wei Zheng Zhongliang Gong Ping Huang Renfu Li Jin Xu Xingwen Cheng Wei Zhang Xueyuan Chen CAS Key Laboratory of Design and Assembly of Functional Nanostructures Fujian Key Laboratory of Nanomaterialsand State Key Laboratory of Structural ChemistryFujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China College of Chemistry Fuzhou UniversityFuzhou 350116China Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China

Luminescent metal halides doped with ns^(2-)metal ions such as 6s^(2-)metal Bi^(3+)have aroused reviving interest owing to their outstanding optical properties;however,the origin of the photoluminescence(PL)remains controversial and ***,we report a strategy for the controlled synthesis of Bi^(3+)-doped vacancy-ordered double perovskite Cs_(2)SnCl_(6)nanocrystals(NCs)and unravel the triplet excited-state dynamics of Bi^(3+)through temperature-dependent PL and ultrafast femtosecond transient absorption *** to the aliovalent Bi^(3+)doping in the spatially confined zero-dimensional(0D)structure of Cs2SnCl6,Bi^(3+)ions experience an enhancive Jahn-Teller distortion in the excited state,which results in intense broadband blue PL originating from the inter-configurational 3P0,1→1S0 transitions of Bi^(3+)at 450 nm,with a large Stokes shift and a quantum yield of 35.2%.Specifically,an unusual thermal-enhanced Jahn-Teller splitting of the excitation band and a remarkable transition of the PL lifetime from ms at 10 K toμs at 300 K were observed,as solid evidence for the isolated Bi^(3+)*** findings clarify the controversy about the PL origin in ns^(2-)metal ion-doped lead-free luminescent metal halides,thereby paving the way for exploring their optoelectronic applications.

关键词： bismuth luminescent nanocrystals metal halide excited-state dynamics electron-phonon coupling

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