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Structural transformation from Waugh-type to Keggin-type polyoxomolybdate-based crystalline material for photo/electrocatalysis

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Rare Metals 2024年第5期43卷 2241-2250页

作者： Pei-Sen Wang Zi-Tong Wang Ya-Ya Tan Peng Chen Xue-Cheng Zhang Lu-Nan Zhang Yong-Ge Wei Lu-Bin Ni School of chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China key Lab of Organic Optoelectronics and molecular Engineering of ministry of education Department of ChemistryTsinghua UniversityBeijing 100084China State key laboratory of natural and Biomimetic Drugs Peking UniversityBeijing100191China

An inorganicDorganic hybrid crystalline material(SiMo_(12)O_(40))[Cu(2,2'-bipy)_(2)]_(2)·2H_(2)O(Complex 1,2,2'-bipy=2,2'-bipyridine)was synthesized for the first time by using 2,2'-bipy and transition metal copper to convert Waugh-type polyoxometalate[MnMo_(9)O_(3)_(2)]_(6-)into a Keggin polyoxometalate structure[SiMo_(12)O_(40)]^(4-)under hydrothermal conditions in glass *** crystal tests and a series of characterizations were carried out on Complex *** structure of Complex 1 is composed of[SiMo_(12)O_(40)]^(4-)and[Cu^(Ⅱ)(2,2'-bipy)_(2)]^(2+).The five-coordinated Cu is connected to two 2,2'-bipy through CuDN bonds,forming an approximately square ***,Complex 1 exhibited good photocatalytic performance for methylene blue degradation and electrocatalytic nitrite reduction properties simultaneously.

关键词： Polyoxometalates Inorganic-organic hybrid materials Photocatalytic Electrocatalytic

Synthesis of poly(thiourethane-alt-thioester)by alternating ring-opening copolymerization of N-thiocarboxyanhydrides and episulfides

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Science China chemistry 2024年第9期67卷 3091-3097页

作者： Wei Xiong Tianjun Yue Haiwang Lai Chunyan Lyu Weimin Ren Hua Lu Beijing National laboratory for molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China State key laboratory of Fine Chemicals Dalian University of TechnologyDalian 116081China

Polythiourethanes(PTU)and polythioesters(PTE)derived from renewable sources are emerging sustainable polymers for their excellent degradability and ***,P(TU-alt-TE)copolymers have been rare and challenging to ***,we report the efficient synthesis of novel P(TU-alt-TE)copolymers via the alternating copolymerization of N-thiocarboxyanhydrides(NTA)/episufides(ES)and provide mechanistic insight into the alternating chain propagation process via density functional theory(DFT)*** incorporation of ESs into traditional peptide backbone is capable of adjusting the glass transition temperature below thermal decomposition temperature,which confers better thermal processability by regulating the rigidity of the backbone and the hydrogen bond interaction among the polymer *** PTUs with tailored properties are accessible by altering the feeding ratio of NTAs and(bifunctional)***,the thiourethane in the backbone can endow interesting underwater adhesion properties to the *** the broad scope of NTA and ES monomers,this method is expected to provide a promising and general route to a wide range of P(TU-alt-TE)copolymers with diverse properties.

关键词： poly(thiourethane-alt-thioester) alternating ring-opening copolymerization N-thiocarboxyanhydrides episulfides

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Phenylhydrazone anions excitation for the photochemical carbonylation of aryl iodides with aldehydes

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Chinese Chemical Letters 2024年第4期35卷 346-351页

作者： Lei Shen Yang Zhang Linlin Zhang Chuanwang Liu Zhixian Ma Kangjiang Liang Chengfeng Xia key laboratory of Medicinal chemistry for natural Resource Ministry of EducationYunnan Provincial Center for Research&Development of Natural ProductsSchool of PharmacyYunnan UniversityKunming 650500China

Spectroscopic investigations discovered that the in-situ generated phenylhydrazone anion was significantly bathochromically shifted to visible light region for photoactivation under irradiation. The photoexcited phenylhydrazone anion was potential to reduce aryl iodides via single electron transfer process for the subsequent radical chain reaction. A redox-neutral photochemical carbonylation of aryl iodides was developed on basis of the special spectroscopic features of phenylhydrazone anion. This protocol provided a convenient and efficient synthetic tool for accessing carbonylation products under redox neutral conditions without the need of transition-metals.

关键词： Organic anion Hydrazone Carbonylation Visible light Single electron transfer

Thermally Conductive and UV-EMI Shielding Electronic Textiles for Unrestricted and Multifaceted Health Monitoring

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Nano-Micro Letters 2024年第10期16卷 149-162页

作者： Yidong Peng Jiancheng Dong Jiayan Long Yuxi Zhang Xinwei Tang Xi Lin Haoran Liu Tuoqi Liu Wei Fan Tianxi Liu Yunpeng Huang key laboratory of synthetic and Biological Colloids Ministry of EducationSchool of Chemical and Material EngineeringJiangnan UniversityWuxi 214122People's Republic of China

Skin-attachable electronics have garnered considerable research attention in health monitoring and artificial intelligence domains,whereas susceptibility to elec-tromagnetic interference(EMI),heat accumulation issues,and ultraviolet(UV)-induced aging problems pose significant constraints on their potential ***,an ultra-elas-tic,highly breathable,and thermal-comfortable epidermal sensor with exceptional UV-EMI shielding performance and remarkable thermal conductivity is developed for high-fidelity monitoring of multiple human electrophysiological *** filling the elastomeric microfibers with thermally conductive boron nitride nanoparticles and bridging the insulating fiber interfaces by plating Ag nanoparticles(NPs),an interwoven thermal con-ducting fiber network(0.72 W m^(-1) K^(-1))is constructed benefiting from the seamless thermal interfaces,facilitating unimpeded heat dissipation for comfort skin *** excitingly,the elastomeric fiber substrates simultaneously achieve outstanding UV protection(UPF=143.1)and EMI shielding(SET>65,X-band)capabilities owing to the high electrical conductivity and surface plasmon resonance of Ag ***,an electronic textile prepared by printing liquid metal on the UV-EMI shielding and thermally conductive nonwoven textile is finally utilized as an advanced epidermal sensor,which succeeds in monitoring different electrophysiological signals under vigorous electromagnetic *** research paves the way for developing protective and environmentally adaptive epidermal electronics for next-generation health regulation.

关键词： Skin electronics Thermal regulating textiles Electromagnetic interference shielding Ultraviolet proof Health monitoring

Rare earth inorganic-organic hybrid compounds based on Keggin-type polyoxometalate {SiW_(12)} with fast-responsive photochromism and switchable luminescence properties

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Journal of Rare Earths 2024年第2期42卷 286-292,I0003页

作者： Hong Cui Yanli Yang Xue Bai Xu Han Wensha Zhang Ying Lu Shuxia Liu key laboratory of Polyoxometalate and Reticular Material chemistry of the ministry of education College of ChemistryNortheast Normal UniversityChangchun 130024China

Four rare earth inorganic-organic hybrid compounds based on Keggin-type polyoxometalate {SiW_(12)}with general formula [{RE(DMF)_(4)(H_(2)O)_4RE(DMF)_(6)}_(2){SiW_(12)O_(40)}_(3)](RE = La(1),Pr(2),Sm(3),Eu(4),DMF=N,N-dimethylformamide) were synthesized by the conventional solution *** analyses indicate that four compounds are isostructural and are all built from three [SiW_(12)O_(40)]^(4-) polyoxoanions and DMF ligands linked by RE^(3+).Compounds 1-4 are extremely sensitive to UV light and present excellent photochromic properties,in which the coloring and fading time of samples are both no more than 2 min,and the reversible coloring-fading process can be repeated for at least 10 cycles with little fatigue,suggesting that compounds 1-4 can be a series of fast-responsive and durable photochromic ***,the solid-state photoluminescence spectra of compounds 3(Sm) and 4(Eu)display strong characteristic emissions of rare earth ions based on f-f ***,compound4(Eu) has a longer fluorescence lifetime up to 566.74 μ***,co mpounds 3(Sm) and 4(Eu) exhibit the switchable luminescence behavior induced by photochromism,which allows them to be used as potential molecular switches.

关键词： Inorganic-organic hybrid Keggin-type polyoxometalates Rare earths Photochromism Photoluminescence

Polyoxometalates-Modulated Hydrophilic-Hydrophobic Composite Interfacial Material for Efficient Solar Water Evaporation and Salt Harvesting in High-Salinity Brine

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Energy & Environmental Materials 2024年第3期7卷 219-227页

作者： Sihang Cheng Cuimei Liu Yingqi Li Huaqiao Tan Yonghui Wang Yangguang Li key laboratory of Polyoxometalate and Reticular Material chemistry of ministry of education Faculty of ChemistryNortheast Normal UniversityChangchun 130024China

Solar vapor generation(SVC)represents a promising technique for seawater desalination to alleviate the global water crisis and energy *** of its main bottleneck problems is that the evaporation efficiency and stability are limited by salt crystallization under high-salinity ***,we demonstrate that the 3D porous melamine-foam(MF)wrapped by a type of self-assembling composite materials based on reduced polyoxometalates(*** blue,HPB),oleic acid(OA),and polypyrrole(PPy)(labeled with MF@HPB-PPy_(n)-OA)can serve as efficient and stable SVC material at high *** characterizations of MF@HPB-PPy_(n)-OA indicate that both hydrophilic region of HPBs and hydrophobic region of OA co-exist on the surface of composite materials,optimizing the hydrophilic and hydrophobic interfaces of the SVC materials,and fully exerting its functionality for ultrahigh water-evaporation and anti-salt *** optimal MF@HPB-PPy_(10)-OA operates continuously and stably for over 100 h in 10wt%***,MF@HPB-PPy_(10)-OA accomplishes complete salt-water separation of 10wt%brine with 3.3kgm^(-2)h^(-1)under 1-sun irradiation,yielding salt harvesting efficiency of 96.5%,which belongs to the record high of high-salinity systems reported so far and is close to achieving zero liquid ***,the low cost of MF@HPB-PPy_(10)-OA(2.56$m^(-2))suggests its potential application in the practical SVC technique.

关键词： heteropoly blue(HPB) hydrophilic-hydrophobic interface polyoxometalates(POM) salt-water separation solar vapor generation(SVG)

Recent advances in post-chiroptical manipulation of supramolecular aggregates assembled with molecular modules

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Science China chemistry 2024年第9期67卷 2842-2863页

作者： Yanling Shen Wanhua Wu Zhipeng Yu Cheng Yang key laboratory of Green chemistry&Technology of ministry of education College of Chemistry InstitutionSichuan UniversityChengdu 610064China

Recently,various supramolecular assembly systems have been identified where the pre-existing chiral supramolecular structure can be manipulated through environmental adjustments,such as temperature,solvent,and *** changes result in diverse microscopic morphologies during the assembly process and induce chiroptical variations,particularly in circular dichroism(CD)and circularly polarized luminescence(CPL)*** chiroptical properties serve as direct indicators of the chiral supramolecular structure and hold promise for applications in sensing,molecular recognition,asymmetric synthesis,and material *** review focuses on research published in the last five years,highlighting instances where assembled structures aggregated by small organic molecular modules demonstrate in-situ chiroptical changes through external condition *** categorizes and discusses different modes of regulation,aiming to offer insights and guidelines for exploring dynamic changes in assembly processes and designing in-situ adjustable structures of assembly modules.

关键词： supramolecular assemblies post-chiroptical manipulation in-situ structural changes

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Plasmon Bi in-situ anchored on BiOCl nanosheets assembled microspheres towards optimized photothermal-photocatalytic performance

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Chinese Chemical Letters 2024年第2期35卷 469-476页

作者： Dongxue Song Mingxia Li Fan Yang Menghan Yu Zhenzi Li Jie Chen Xiaoshuang Zhang Wei Zhou School of chemistry and Materials Science Key Laboratory of Functional Inorganic Material ChemistryMinistry of Education of the People's Republic of ChinaHeilongjiang UniversityHarbin 150080China Shandong Provincial key laboratory of molecular Engineering School of Chemistry and Chemical EngineeringQilu University of Technology (Shandong Academy of Sciences)Ji'nan 250353China

Interface engineering is of great importance to improve the photocatalytic ***,in-situ formation plasmon Bi/BiOCl nanosheets assembled heterojunction microspheres are fabricated via facile reductive solvothermal *** aldehyde group in the DMF structure is used to exert the weak reducing property of the solvent and thus strip out the metal Bi in *** metal Bi is anchored on surface of BiOCl firmly due to in-situ formation engineered interface,which could realize efficient charge transfer *** resultant Bi/BiOCl heterojunctions assemblies with narrow bandgap of 3.05 eV and mesoporous structure extend the photoresponse to visible light region and could provide sufficient surface active *** visible-light-driven photocatalytic degradation of high-toxic norfloxacin for Bi/BiOCl heterojunctions is up to 95.5%within 20 min,representing several times that of pristine BiOCl nanosheets and the physical *** is attributed to the in-situ formation of Bi/BiOCl heterojunctions and surface plasmon resonance(SPR)effect of plasmon Bi promoting charge transfer,and the obvious photothermal effect promoting the photocatalytic reaction,which are verified by experimental and density functional theory(DFT)*** strategy provides ideal perspectives for fabricating metal/semiconductor heterojunctions photocatalysts with high-performance.

关键词： Photocatalysis BiOCl Heterojunction Plasmon Bi Mesoporous structure

Polyoxometalate-based flexible conductive materials with superionic conductivity

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Science China chemistry 2024年第10期67卷 3299-3309页

作者： Yuxin Wang Shuping Xue Jun Geng Ying Lu Teng Li Xiaozheng Duan Xue Bai Yanli Yang Jingqi Yang Shuxia Liu key laboratory of Polyoxometalate and Reticular Material chemistry of ministry of education College of ChemistryNortheast Normal University State key laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences

Flexible ion-conductive materials exhibit intriguing advantages for applications in flexible electronic ***,the further enhancement of their conductivity within environmental limitations is an urgent demand for the development of flexible electronic devices,yet remains as a great ***,we report a“dual-acid”strategy,via the encapsulation of two acids,H3PW12O40（HPW） and NH2SO3H（SA）,with synergistic interaction into poly（vinyl alcohol）-glycerol（PVA-Gly） hydrogel,to achieve polyoxometalate（POM）-based flexible materials with superionic conductivity under various environmental *** a representative example,the prepared PVA-Gly/HPW-SA-20% hydrogel presents an ultrahigh proton conductivity ranging from -30℃(3.33×10-2S cm-1) to room temperature(2.78×10-1S cm-1) under ambient ***,the PVA-Gly/HPW-SA-20% hydrogel exhibits remarkable advantages in anti-freezing,mechanical flexibility and self-adhesiveness,making it a promising multifunctional electrolyte for flexible electronic *** experimental results and molecular dynamics（MD） simulations jointly demonstrate that SA bridges HPW clusters to form a dense proton transport pathway induced by multiple electrostatic and hydrogen bonding interactions between SA and HPW counterparts,which contributes to the high-level proton conductivity of the PVA-Gly/HPW-SA-20% *** work provides new insights into the design of POM-based flexible materials with superionic conductivity.

关键词： polyoxometalates proton conduction dual-acid effect hydrogel molecular dynamics simulation