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Chiral thermally activated delayed fluorescence materials for circularly polarized organic light-emitting diodes

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science China {1. 2024年第4期67卷 1097-1116页

作者： Li Yuan Yi-Pin Zhang You-Xuan Zheng state {1. laboratory of Coordination chemistry Collaborative Innovation Center of Advanced MicrostructuresJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chirality is an important natural characteristic of organic molecules,and chiral organic molecules have shown extensive application in areas such as pharmaceutical development and material *** from the ability to achieve circularly polarized luminescence(CPL),chiral luminescent materials have shown potential applications in anti-glare display,optical communication and,3D display,*** to the ability to harvest both singlet and triplet excitons by a fast reverse intersystem crossing process without involving noble metals,chiral thermally activated delayed fluorescence(TADF)materials with point chirality,axial chirality,planar chirality and helical chirality are regarded as the state-of-the-art materials for circularly polarized organic light-emitting diodes(CP-OLEDs).In recent years,the chiral TADF materials and CP-OLEDs have rapidly developed,but unfortunately,the dissymmetry factors(g)are far from the requirement of practical *** ideal emitters and devices should have both high efficiency and a g factor,or at least a balance between these two *** review gives an overview of recent progress in chiral TADF materials,with a particular focus on the chiral skeleton,CPL property and device ***,the molecular design concept,device structure and methods to improve the g factors of chiral materials and CP-OLEDs are also discussed.

关键词： chiral thermally activated delayed fluorescence material chiral skeleton circularly polarized luminescence circularly polarized organic light-emitting diodes dissymmetry factor

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 {1. 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 *** electro-oxidation of water to oxygen plays a crucial role in such energy conversion ***,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 1. mA cm^(-2)at an overpotential of 21. mV in 0.1.M KOH *** catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in *** spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline ***-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 *** mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and *** 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

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

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science China {1. 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 {1.s 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 {1. 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

Palladium-catalyzed multi components oxy-aminofluorination and aminofluorination of gem-difluoroalkenes

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Chinese Chemical Letters 2024年第2期35卷 420-425页

作者： Fen Wu Xin Li Junbiao Chang Dachang Bai state {1. laboratory of Antiviral Drugs NMPA Key Laboratory for Research and Evaluation of Innovative DrugKey Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringPingyuan LaboratoryHenan Normal UniversityXinxiang 453007China state {1. laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Organofluorine compounds are widely used in the realm of drug discovery and material ***,we developed palladium catalyzed intermolecular aminofluorination and oxy-aminofluorination of gem‑difluoroalkenes with N-fluorobenzenesulfonimide(NFSI),in which NFSI was used as the nitrogen source and *** reaction provides an efficient and straightforward synthesis route of a series ofα-trifluoromethyl benzylic ***,three/four components oxy-aminofluorination processes were realized to giveα-trifluoromethyl benzylic ether with a terminal amino group,which proceed through C(sp^(3))-O bond cleavage of easily available ether and simultaneous introduced a fluorine,an amino and an oxy substituent in one pot with excellent *** divergent reactivity not only included the incorporation of one ether molecular,but also much more challenged two ether insertion with excellent selectivity through succession C(sp^(3))-O bonds *** protocol allows for concise synthesis of high value amines with fluoroalkyl-substituents and selectively transformation of easily available ethers by high-valent palladium catalysis.

关键词： Palladium Multi components Aminofluorination Oxy-aminofluorination C(sp^(3))-O bond cleavage

Recent advances in the synthesis and application of N-heterocyclic carbene-based molecular cages

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science China {1. 2024年第5期67卷 1510-1523页

作者： Qiongjie Chai Lixin Duan Yanzhe Ma Tianheng Hou Tao Tu Shanghai key {1. of Molecular Catalysis and Innovative Materials Department of ChemistryFudan UniversityShanghai 200438China state {1. laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

N-Heterocyclic carbene(NHC)-based cages have emerged as a prominent and dynamic research area within the research field of chemistry. Leveraging the distinctive electronic and steric properties of NHC ligands, the design, synthesis, and application of these corresponding cages have garnered substantial scholarly interest. In recent years, we have witnessed the successful fabrication of diverse NHC-based cages through a range of synthetic methodologies, which hold significant potential for applications in molecular recognition and catalysis. In this review, we delve into the foundational synthetic strategies that underlie the creation of NHC-based cages, employing approaches encompassing metal–NHC chelation, coordination assembly,and covalent bonding. Additionally, we compile the diverse applications of these cages within catalytic processes and molecular recognition. Lastly, we shed light on the current limitations of synthesis and outline future trends in the development of NHCbased cages.

关键词： N-heterocyclic carbene molecular cages supramolecular chemistry synthetic strategies applications

Photoswitchable Spiropyridine Enabled Photoactuation of Polymeric Hydrogels under Physiological pH Conditions

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Chinese Journal of Polymer science 2024年第10期42卷 1602-1609,I0015页

作者： Cong Liao Meng-Qi Du Chuang Li key {1. of Precision and Intelligent chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaAnhui230026China

The incorporation of molecular switches into polymer networks has been a powerful approach for the development of functional polymer materials that display macroscopic actuation and function enabled directly by molecular ***,such materials sometimes require harsh conditions to perform their functions,and the design of new molecular photoswitches that can function under physiological conditions is highly ***,we report the design and synthesis of a spiropyridine-based photoswitchable hydrogel that exhibits light-driven actuation at physiological *** to its high p Ka,spiropyridine maintains its ring-open protonated form at neutral pH,and the resulting hydrogel remains in a swollen *** irradiation with visible light,the ring closure of spiropyridine leads to a decrease in the charge and a reduction in the volume of the *** contracted gel could spontaneously recover to its expanding state in the dark,and this process is highly dynamic and reversible when the light is switched on and ***,the hydrogel shows switchable fluorescence in response to visible *** deformation is observed in the hydrogel thin films upon irradiation from one ***,the independence of this spiropyridine hydrogel from the acidic environment makes it biotolerant and shows excellent *** biocompatible spiropyridine hydrogel might have important biorelated applications in the future.

关键词： Spiropyridine photowitch Polymer hydrogel Photoactuation Physiological pH Biocompatibility

Stabilizing perovskite precursors with the reductive natural amino acid for printable mesoscopic perovskite solar cells

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Journal of Energy chemistry 2024年第3期90卷 32-39,I0003页

作者： Wenjing Hu Jian Yang Chuang Yang Xufeng Xiao Chaoyang Wang Zhaozhen Cui Qiaojiao Gao Jianhang Qi Minghao Xia Yaqiong Su Anyi Mei Hongwei Han Michael Gratzel Center for Mesoscopic Solar Cells Wuhan National Laboratory for OptoelectronicsKey Laboratory of Materials Chemistry for Energy Conversion and Storage of Ministry of Education Huazhong University of Science and TechnologyWuhan 430074HubeiChina School of chemistry Xi'an Key Laboratory of Sustainable Energy Materials ChemistryState Key Laboratory of Electrical Insulation and Power EquipmentXi'an Jiaotong UniversityXi'an 710049ShaanxiChina

Solution processability significantly advances the development of highly-efficient perovskite solar ***,the precursor solution tends to undergo irreversible degradation reactions,impairing the device performance and ***,we utilize a reductive natural amino acid,Nacetylcysteine(NALC),to stabilize the precursor solution for printable carbon-based hole-conductorfree mesoscopic perovskite solar *** find that I_(2) can be generated in the aged solution containing methylammonium iodide(MI) in an inert atmosphere and speed up the MA-FA^(+)(formamidinium) reaction which produces large-size cations and hinders the formation of perovskite *** effectively stabilizes the precursor via its sulfhydryl group which reduces I_(2) back to I^(-)and provides H^(+).The NALC-stabilized precursor which is aged for 1.40 h leads to devices with a power conversion efficiency equivalent to 98% of that for devices prepared with the fresh ***,NALC improves the device power conversion efficiency from 1..1.% to 1..41. along with enhanced stability under atmospheric conditions by modifying grain boundaries in perovskite films and reducing associated defects.

关键词： Perovskite solar cells Perovskite precursor Degradation Stabilization Reductive natural amino acid

Photocatalytic dicarboxylation of strained C-C bonds with CO_(2) via consecutive visible-light-induced electron transfer

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Chinese Chemical Letters 2024年第6期35卷 268-273页

作者： Yi Liu Zhe-Hao Wang Guan-Hua Xue Lin Chen Li-Hua Yuan Yi-Wen Li Da-Gang Yu Jian-Heng Ye key {1. of Green chemistry&Technology of Ministry of Education College of ChemistrySichuan UniversityChengdu 610064China College of Polymer science and Engineering State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610065China state {1. laboratory of Elemento-Organic chemistry Nankai UniversityTianjin 300071China

Dicarboxylic acids have a wide range of applications in the polymer industry to construct valuable *** has recently emerged as an efficient and sustainable strategy to generate dicarboxylic ***,photocatalytic dicarboxylation with CO_(2) is mainly limited to unsaturated bonds,and the dicarboxylation of C-C single bonds still remains a ***,we report a photocatalytic dicarboxylation of C-C single bonds in strained rings with CO_(2) units via consecutive photo-induced electron transfer(ConPET).It is also the first photocatalytic reductive ring-opening reaction of ***,this transition-metal-free protocol exhibits good functional group tolerance,broad substrate scope,facile scalability,and easy product ***,diacids can easily be derivatized to mainchain liquid crystalline polyesters.

关键词： Consecutive photo-induced electron transfer Visible-light catalysis Dicarboxylation Carbon dioxide Cyclopropanes

Polyoxometalate-based flexible conductive materials with superionic conductivity

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science China {1. 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 {1. of Polyoxometalate and Reticular Material chemistry of Ministry of Education College of ChemistryNortheast Normal UniversityChangchun 130024China state {1. laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

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,H_(3)PW_(1.)O_(40)(HPW) and NH_(2)SO_(3)H(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℃(3.33×1.^(-2)S cm^(-1.) to room temperature(2.78×1.^(-1.S 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