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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 University State key laboratory of Natural and Biomimetic Drugs Peking University key lab of organic optoelectronics and molecular engineering of ministry of education Department of Chemistry Tsinghua University

An inorganicDorganic hybrid crystalline material (Si Mo12O40)[Cu（2,2'-bipy）2]2·2H2O （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[Mn Mo9O32]6-into a Keggin polyoxometalate structure[Si Mo12O40]4-under hydrothermal conditions in glass vials.Single crystal tests and a series of characterizations were carried out on Complex 1.The structure of Complex 1 is composed of[Si Mo12O40]4-and[CuII（2,2'-bipy）2]2+.The five-coordinated Cu is connected to two 2,2'-bipy through CuDN bonds,forming an approximately square structure.Astonishingly,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

Moisture‑Electric–Moisture‑Sensitive Heterostructure Triggered Proton Hopping for Quality‑Enhancing Moist‑Electric Generator

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Nano-Micro Letters 2024年第3期16卷 351-366页

作者： Ya’nan Yang Jiaqi Wang Zhe Wang Changxiang Shao Yuyang Han Ying Wang Xiaoting Liu Xiaotong Sun Liru Wang Yuanyuan Li Qiang Guo Wenpeng Wu Nan Chen Liangti Qu key laboratory of Cluster Science Ministry of Education of ChinaKey Laboratory of Photoelectronic/Electrophotonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Yangtze Delta Region Academy of Beijing Institute of Technology Jiaxing 314019People’s Republic of China Department of Chemistry Key Laboratory of Organic Optoelectronics&Molecular EngineeringMinistry of EducationTsinghua UniversityBeijing 100084People’s Republic of China

Moisture-enabled electricity(ME)is a method of converting the potential energy of water in the external environment into electrical energy through the interaction of functional materials with water molecules and can be directly applied to energy harvesting and signal expression.However,ME can be unreliable in numerous applications due to its sluggish response to moisture,thus sacrificing the value of fast energy harvesting and highly accurate information representation.Here,by constructing a moisture-electric-moisture-sensitive(ME-MS)heterostructure,we develop an efficient ME generator with ultra-fast electric response to moisture achieved by triggering Grotthuss protons hopping in the sensitized ZnO,which modulates the heterostructure built-in interfacial potential,enables quick response(0.435 s),an unprecedented ultra-fast response rate of 972.4 mV s^(−1),and a durable electrical signal output for 8 h without any attenuation.Our research provides an efficient way to generate electricity and important insight for a deeper understanding of the mechanisms of moisture-generated carrier migration in ME generator,which has a more comprehensive working scene and can serve as a typical model for human health monitoring and smart medical electronics design.

关键词： Moist-electric generators Grotthuss proton hopping Fast response Durable electrical output Personal health monitoring

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Promising thermal photonic management materials for sustainable human habitat

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Nano Research 2024年第1期17卷 112-131页

作者： Houze Yao Qihua Liao Huhu Cheng Liangti Qu key laboratory of organic optoelectronics&molecular engineering Ministry of EducationDepartment of ChemistryLaboratory of Flexible Electronics TechnologyTsinghua UniversityBeijing 100084China State key laboratory of Tribology in Advanced Equipment(SKLT) Department of Mechanical EngineeringTsinghua UniversityBeijing 100084China

The spectral characteristics of outdoor structures,such as automobiles,buildings,and clothing,determine their energy interaction with the environment,from broad-spectrum absorption of light energy to high-efficiency thermal emission.Recently developed spectrally selective absorption(SSA)materials permit the reduction of energy loss from human habitat eco-system in the sustainable way and further reduce the utilization of fossil energy to achieve carbon neutrality.Here we review recent advances in SSA materials that enable rational and efficient management of thermal energy and provide new solutions for the resource base that supports human life like comfortable heat management,electricity production,and water supply.The basic principles of thermal photonic management,the regulation of SSA materials,and functional properties are summarized.An outlook discussing challenges and opportunities in SSA material energy management for comfortable living environments is finally presented,which expects the enormous potential of this interdisciplinary research in solving growing resource-shortage of human society.

关键词： spectrally selective absorption passive cooling solar power eco-system

Polymer: Non-fullerene acceptor heterojunction-based phototransistor for short-wave infrared photodetection

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Nano Research 2024年第4期17卷 3087-3095页

作者： Jing Li Weigang Zhu Yang Han Yanhou Geng Wenping Hu key laboratory of organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Science&Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin 300072China key laboratory of organic Integrated Circuits of ministry of education&key laboratory of molecular Optoelectronic Sciences School of Materials Science and EngineeringTianjin UniversityTianjin 300072China

It remains full of challenge for extending short-wave infrared(SWIR)spectral response and weak-light detection in the context of broad spectral responses for phototransistor.In this work,a novel poly(2,5-bis(4-hexyldodecyl)-2,5-dihydro-3,6-di-2-thienyl-pyrrolo[3,4-c]pyrrole-1,4-dione-alt-thiophene)(PDPPT3-HDO):COTIC-4F organic bulk-heterojunction is prepared as active layer for bulk heterojunction phototransistors.PDPPT3-HDO serves as a hole transport material,while COTIC-4F enhances the absorption of SWIR light to 1020 nm.As a result,smooth and connected PDPPT3-HDO film is fabricated by blade coating method and exhibits high hole mobility up to 2.34 cm^(2)·V^(-1)·s^(-1) with a current on/off ratio of 4.72×10^(5) in organic thin film transistors.PDPPT3-HDO:COTIC-4F heterojunction phototransistors exhibit high responsivity of 2680 A·W^(-1) to 900 nm and 815 A·W^(-1) to 1020 nm,with fast response time(rise time~20 ms and fall time~100 ms).The photosensitivity of the heterojunction phototransistor improves as the mass ratio of non-fullerene acceptors increases,resulting in an approximately two orders of magnitude enhancement compared to the bare polymer phototransistor.Importantly,the phototransistor exhibits decent responsivity even under ultra-weak light power of 43μW·cm^(-2) to 1020 nm.This work represents a highly effective and general strategy for fabricating efficient and sensitive SWIR light photodetectors.

关键词： photodetection phototransistor organic semiconductor heterojunction non-fullerene acceptor

Versatile Organogels of Aluminum Oxide Subnanosheets for Locking Solvents and Adhesion

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Precision Chemistry

Precision Chemistry 2024年第1期2卷 21-27页

作者： Wanyue Ouyang Xun Wang key lab of organic optoelectronics and molecular engineering Department of ChemistryTsinghua UniversityBeijing 100084China

Herein,we present a facile strategy to prepare versatile aluminum oxide subnanometer nanosheets with oleic acid and stearic acid ligands(OA-Al SNSs and SA-Al SNSs,respectively).The size effect endows subnanosheets with abundant acting sites,remarkable intermolecular interactions,and unique polymer-like properties,including flexibility,viscoelasticity,and sol-gel transitions,which is quite different from traditional inorganic materials.Consequently,subnanosheets could form freestanding organogels and OA-Al SNSs exhibit satisfying semisolidification of various solvents,making it an intriguing candidate for the safe storage and transportation of solvents.Furthermore,SA-Al SNSs exhibit excellent adhesive properties of high strength on diverse substrates,and it is easy to erase it without any damage,demonstrating the promising prospects in practical applications.

关键词： subnanometer nanomaterials self-assembly polymer-analogue organogel adhesive

Thiazoloisoindigo-based Polymer Semiconductors: Synthesis,Structure-Property Relationship, Charge Carrier Polarity, and Field-Effect Transistor Performance

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Chinese Journal of Polymer Science 2024年第1期42卷 24-31,I0006页

作者： Bo-Wen Li Miao Xiong Mei-Hua Liu Zhi-Gao Li Long Sang Zi-Han Xiong Biao Xiao Jian Pei Xiao-Bo Wan key laboratory of Optoelectronic Chemical Materials and Devices Ministry of EducationSchoolofOptoelectronic Materials&TechnologyJianghan UniversityWuhan430056China Bejing National laboratoryfor molecular Sciences the Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China

Developing new polymeric semiconductors with excellent device performance is essential for organic electronics. Herein, we synthesized two new thiazoloisoindigo(Tz II)-based polymers, namely, P(Tz II-d Th-d Th) and P(Tz II-d Th-d Tz), by copolymerizing thiophene-flanked Tz II with bithiophene and bithiazole, respectively. Owing to the more electron-deficient nature of bithiazole than bithiophene, P(Tz II-d Th-d Tz)possesses deeper LUMO/HOMO levels of-3.45/-5.47 e V than P(Tz II-d Th-d Th)(-3.34/-5.32 e V). The organic field-effect transistor(OFET) devices based on P(Tz II-d Th-d Th) exhibited p-type behaviors with an average hole mobility value as high as 1.43 cm^(2)·V^(-1)·s^(-1), while P(Tz II-d Th-d Tz)showed typical ambipolar characteristics with average hole and electron mobilities of 0.38 and 0.56 cm^(2)·V^(-1)·s^(-1). In addition, we compared the performances of both polymers with other Tz II-based polymers reported in our previous work, and showed that the charge carrier polarity can be manipulated by adjusting the number of the thiophene units between the acceptor unit. As the increase of the number of thiophene rings,charge carrier polarity shifts from electron-dominated ambipolar transport to hole-dominated ambipolar transport and then to unipolar hole transport in OFETs, which provides an effective molecular design strategy for further optimization of polymer OFET performance.

关键词： Field-effect transistor Charge carrier polarity Thiazoloisoindigo

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Asymmetric Two-Component Alkenyl Catellani Reaction for the Construction of C—N Axial Chirality

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Chinese Journal of Chemistry 2024年第7期42卷 699-704页

作者： Chenggui Wu Ze-Shui Liu Yong Shang Chang Liu Shuang Deng Hong-Gang Cheng Hengjiang Cong Yinchun Jiao Qianghui Zhou Sauvage Center for molecular Sciences Engineering Research Center of Organosilicon Compounds&Materials(Ministry of Education)Hubei Key Lab on Organic and Polymeric OptoElectronic MaterialsCollege of Chemistry and Molecular SciencesThe Institute for Advanced Studiesand TaiKang Center for Life and Medical SciencesWuhan UniversityWuhanHubei 430072China key laboratory of Xin'an Medicine Ministry of EducationAnhui University of Chinese MedicineHefeiAnhui 230038China School of Chemistry and Chemical engineering Hunan University of Science and TechnologyXiangtanHunan 411201China

Herein,we report an asymmetric two-component alkenyl Catellani reaction for the construction of C—N axial chirality through a palladium/chiral norbornene cooperative catalysis and an axial-to-axial chirality transfer process.Various partially aromatic iodinated 2-pyridones,quinolones,coumarin and uracil substrates react with 2,6-disubstituted aryl bromides with a tethered amide group,to afford a wide variety of polycyclic C—N atropisomers(38 examples,up to 97%e.e.).The obtained C—N axial chirality originates from the preformed transient C—C axial chirality with high fidelity.The synthetic utility of this chemistry is demonstrated by facile prepa-ration of complex quinoline and pyridine based C—N atropisomers through a N-deprotection and aromatization sequence.In addi-tion,a remote axial-to-central diastereoinduction process dictated by C—N axial chirality is observed with excellent diastereocontrol.

关键词： Alkenyl Catellani reaction Asymmetric catalysis Atropisomerism Axial-to-axial chirality transfer Heterocycles

Synthesis and Modulation of Low-Dimensional Transition Metal Chalcogenide Materials via Atomic Substitution

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Nano-Micro Letters 2024年第9期16卷 49-94页

作者： Xuan Wang Akang Chen XinLei Wu Jiatao Zhang Jichen Dong Leining Zhang key laboratory of Cluster Science Ministry of Education of ChinaBeijing Key Laboratory of Photoelectronic and Electrophonic Conversion MaterialsSchool of Chemistry and Chemical EngineeringBeijing Institute of TechnologyBeijing 100081People’s Republic of China Beijing National laboratory for molecular Sciences Key Laboratory of Organic SolidsInstitute of Chemistry Chinese Academy of SciencesBeijing 100190People’s Republic of China

In recent years,low-dimensional transition metal chalcogenide(TMC)materials have garnered growing research attention due to their superior electronic,optical,and catalytic properties compared to their bulk counterparts.The controllable synthesis and manipulation of these materials are crucial for tailoring their properties and unlocking their full potential in various applications.In this context,the atomic substitution method has emerged as a favorable approach.It involves the replacement of specific atoms within TMC structures with other elements and possesses the capability to regulate the compositions finely,crystal structures,and inherent properties of the resulting materials.In this review,we present a comprehensive overview on various strategies of atomic substitution employed in the synthesis of zero-dimensional,one-dimensional and two-dimensional TMC materials.The effects of substituting elements,substitution ratios,and substitution positions on the structures and morphologies of resulting material are discussed.The enhanced electrocatalytic performance and photovoltaic properties of the obtained materials are also provided,emphasizing the role of atomic substitution in achieving these advancements.Finally,challenges and future prospects in the field of atomic substitution for fabricating low-dimensional TMC materials are summarized.

关键词： Transition metal chalcogenides Atomic substitution Ion exchange Low-dimensional materials Controllable synthesis

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Copper Catalyzed Enantioconvergent Nucleophilic Substitutions

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Chinese Journal of Chemistry 2024年第10期42卷 1161-1174页

作者： Chunxi Huang Zilong Wan Aoping Zhu Caiyou Chen College of Chemistry and molecular Sciences Wuhan UniversityWuhanHubei 430072China ministry of education key laboratory for the Synthesis and Application of organic Functional Molecules and College of Chemistry and Chemical engineering Hubei UniversityWuhanHubei 430062China

As a versatile earth-abundant transition metal,Cu has long been widely applied in the C—C and C—X bond forming reactions.As for now,low-valent Cu(Ⅰ)is known to reduce the redox active electrophiles via an SET pathway to give the corresponding radical and Cu(Ⅱ)species.The resulting Cu(Ⅱ)species can interact with the radical via the out-sphere pathway,affording the coupling product.Alternatively,Cu(Ⅱ)can trap the radical through the inner-sphere process to generate Cu(Ⅲ)species and then realize challenging bond formations due to the facile reductive elimination of Cu(Ⅲ)intermediate.Although copper catalysis has been widely applied in arylations of various nucleophiles,copper-catalyzed enantioconvergent nucleophilic substitutions of racemic alkyl electrophiles have been less explored,likely due to the difficulties in overcoming the reduction potential of alkyl electrophiles,elimination of side reactions,and enantiomeric control.In order to overcome the high reduction potential of alkyl electrophiles,the photo-induced strategy has been developed under mild conditions.An alternative strategy with new anionic tridentate ligands has also been reported in this regard.This review summarizes recent developments in copper-catalyzed enantioconvergent nucleophilic substitutions of alkyl electrophiles by various nucleophiles to realize C—N,C—C,C—B,C—P and C—O bond formations and their brief mechanistic studies.

关键词： Enantioconvergent Nucleophilic substitution Copper Radical reactions Photocatalysis Asymmetric catalysis