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Polaron interfacial entropy as a route to high thermoelectric performance in DAE-doped PEDOT:PSS films

National Science Review 2024年第3期11卷 259-270页

作者： Jiajia Zhang Caichao Ye Genwang Wei Liang Guo Yuhang Cai Zhi Li Xinzhi Wu Fangyi Sun Qikai Li Yupeng Wang Huan Li Yuchen Li Shuaihua Wang Wei Xu Xuefeng Guo Wenqing Zhang Weishu Liu Department of materials Science and Engineering Southern University of Science and Technology Academy for Advanced Interdisciplinary Studies and guangdong provincial key laboratory of Computational Science and Material Design Southern University of Science and Technology Department of Mechanical and Energy Engineering Southern University of Science and Technology Beijing National laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences College of Chemistry and Molecular Engineering National Biomedical Imaging Centre Peking University guangdong provincial key laboratory of Functional Oxide materials and Devices Southern University of Science and Technology

Enhancing the thermoelectric transport properties of conductive polymer materials has been a long-term challenge, in spite of the success seen with molecular doping strategies. However, the strong coupling between the thermopower and the electrical conductivity limits thermoelectric performance. Here, we use polaron interfacial occupied entropy engineering to break through this intercoupling for a PEDOT:PSS(poly（3,4-ethylenedioxythiophene）-poly（4-styrenesulfonate）) thin film by using photochromic diarylethene（DAE） dopants coupled with UV-light modulation. With a 10-fold enhancement of the thermopower from 13.5 μV K-1to 135.4 μV K-1and almost unchanged electrical conductivity, the DAE-doped PEDOT:PSS thin film achieved an extremely high power factor of 521.28 μW m-1K-2from an original value of 6.78 μW m-1K-2. The thermopower was positively correlated with the UV-light intensity but decreased with increasing temperature, indicating resonant coupling between the planar closed DAE molecule and PEDOT. Both the experiments and theoretical calculations consistently confirmed the formation of an interface state due to this resonant coupling. Interfacial entropy engineering of polarons could play a critical role in enhancing the thermoelectric performance of the organic film.

关键词： thermoelectric PEDOT: PSS interfacial occupied entropy resonant coupling UV-light modulation

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Polarization engineering in porous organic polymers for charge separation efficiency and its applications in photocatalytic aerobic oxidations

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Science China Chemistry 2024年第3期67卷 1000-1007页

作者： Kun Wu Pei-Wen Cheng Xin-Yi Liu Ji Zheng Xiao-Wei Zhu Mo Xie Puxin Weng Weigang Lu Dan Li College of Chemistry and materials Science Guangdong Provincial Key Laboratory of Functional Supramolecular Coordination Materials and ApplicationsJinan UniversityGuangzhou 510632China guangdong Rare Earth Photofunctional materials Engineering Technology Research Center School of Chemistry and EnvironmentJiaying UniversityMeizhou 514015China

Photocatalytic aerobic oxidation reactions are largely governed by the efficiency of charge separation and subsequent reactive oxygen species(ROS) generation. Herein, we report a polarization engineering strategy to promote the charge separation and ROS generation efficiency by substituting the benzene unit with furan/thiophene in porous organic polymers(POPs). Benefiting from the extent of local polarization, the thiophene-containing POP(JNU-218) exhibits the best photocatalytic performance in aerobic oxidation reactions, with a yield much higher than those for the furan-containing POP(JNU-217) and the benzenecontaining POP(JNU-216). Experimental studies and theoretical calculations reveal that the increase of local polarization can indeed reduce the exciton binding energy, and therefore facilitate the separation of electron-hole pairs. This work demonstrates a viable strategy to tune charge separation and ROS generation efficiency by modulating the dipole moments of the building blocks in porous polymeric organic semiconductors.

关键词： porous organic polymer local polarization photocatalytic aerobic oxidation charge separation reactive oxygen species exciton binding energy

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Highly elastic energy storage device based on intrinsically super-stretchable polymer lithium-ion conductor with high conductivity

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Fundamental Research 2024年第1期4卷 140-146页

作者： Shi Wang Jixin He Qiange Li Yu Wang Chongyang Liu Tao Cheng Wen-Yong Lai State key laboratory of organic electronics and Information Displays(SKLOEID) Institute of Advanced Materials(IAM)School of Chemistry and Life SciencesNanjing University of Posts&Telecommunications9 Wenyuan RoadNanjing 210023China Frontiers Science Center for Flexible electronics(FSCFE) MIIT Key Laboratory of Flexible Electronics(KLoFE)Northwestern Polytechnical UniversityXi'an 710072China

Stretchable power sources,especially stretchable lithium-ion batteries(LIBs),have attracted increasing attention due to their enormous prospects for powering flexible/wearable electronics.Despite recent advances,it is still challenging to develop ultra-stretchable LIBs that can withstand large deformation.In particular,stretchable LIBs require an elastic electrolyte as a basic component,while the conductivity of most elastic electrolytes drops sharply during deformation,especially during large deformations.This is why highly stretchable LIBs have not yet been realized until now.As a proof of concept,a super-stretchable LIB with strain up to 1200%is created based on an intrinsically super-stretchable polymer electrolyte as the lithium-ion conductor.The super-stretchable conductive system is constructed by an effective diblock copolymerization strategy via photocuring of vinyl functionalized 2-ureido-4-pyrimidone(VFUpy),an acrylic monomer containing succinonitrile and a lithium salt,achieving high ionic conductivity(3.5×10^(-4)mS cm^(-1)at room temperature(RT))and large deformation(the strain can reach 4560%).The acrylic elastomer containing Li-ion conductive domains can strongly increase the compatibility between the neighboring elastic networks,resulting in high ionic conductivity under ultra-large deformation,while VFUpy increases elasticity modulus(over three times)and electrochemical stability(voltage window reaches 5.3 V)of the prepared polymer conductor.At a strain of up to 1200%,the resulting stretchable LIBs are still sufficient to power LEDs.This study sheds light on the design and development of high-performance intrinsically super-stretchable materials for the advancement of highly elastic energy storage devices for powering flexible/wearable electronics that can endure large deformation.

关键词： Stretchable electronics Flexible electronics Flexible energy storage devices Stretchable lithium-ion conductors Flexible lithium-ion batteries

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Solution-processed D-A-π-A-D radicals for highly efficient photothermal conversion

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Aggregate 2024年第1期5卷 398-408页

作者： Jiaxing Huang Zejun Wang Weiya Zhu Yuan Li Institute of polymer Optoelectronic materials and Devices State Key Laboratory of Luminescent Materials and DevicesSouth China University of TechnologyGuangzhouP.R.China

organic donor-acceptor semiconductors exhibit great potential in photothermal conversion.However,it is still challenging to achieve pure organic materials with broad absorption comparable with inorganic materials such as graphene.Herein,two D-AD type DPA-BT-O4 and NDI-TPA-O4 and three D-A-π-A-D type Th-O4,Th2-O4,and IDT-O4 were readily prepared via two high-yield steps and simple air oxidization.The stability can be attributed to their multiple resonance structures based on the aromatic nitric acid radical mechanism.Compared with the D-A-D radicals,the conjugation extension of the D-A-π-A-D radicals endows them with a narrowed band gap and broad absorption in powder.Interestingly,the IDT-O4 powder with aggregation-induced radical effect exhibits broad absorption between 300 and 2500 nm,which is comparable with graphene and other inorganic materials.Under irradiation of 0.9 W/cm^(2)(808 nm),the temperature of IDT-O4 powder rises to 250℃within 60 s.The water evaporation conversion efficiency of 94.38%and an evaporation rate of 1.365 kg/m^(2)h^(−1)under one sun illumination were achieved.IDT-O4 stands as one of the most efficient photothermal conversion materials among pure organic materials via a rational design strategy.

关键词： donor-acceptor near-infrared absorption open-shell radicals photothermal conversion seawater desalination

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Highly efficient through-space charge transfer TADF molecule employed in TADF-and TADF-sensitized organic light-emitting diodes

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Science China Chemistry 2024年第4期67卷 1270-1276页

作者： Jiasen Zhang Deli Li Wei Li Yujie Wu Xilin Mu Chunyu Liu Kaibo Fang Ziyi Ge Zhejiang provincial Engineering Research Center of Energy Optoelectronic materials and Devices Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China Center of materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China State key laboratory of Luminescent materials and Devices and Institute of polymer Optoelectronic materials and Devices South China University of TechnologyGuangzhou 510640China

The inception and harnessing of excitons are paramount for the electroluminescence performance of organic light-emitting devices(OLEDs).Through-space charge transfer(TSCT)via intramolecular interaction has proved to be one of the most potent techniques employed to achieve 100% internal quantum efficiency.However,molecular strategies utilized to comprehensively enhance the electroluminescent performance of TSCT emitters regarding improving the photoluminescence quantum yield(PLQY)and elevating the light out-coupling efficiency remain arduous.To surmount this challenge,we deliberately designed and synthesized a proof-of-concept TSCT emitter called CzO-TRZ by incorporating an extra carbazole donor into spiroheterocyclic architecture.The introduction of rigid spiral fragments can immensely boost the horizontal orientation dipole ratio and establish an extra through-bond charge transfer(TBCT)radiative decay channel.As a result,a very high PLQY of 98.7%,fast kRISCof 2.2×10^(5)s^(-1)and high k_(r)^(s) of 2.2×10^(7)s^(-1),and an ultrahigh horizontal dipolar ratio of 90%were concurrently achieved for Cz O-TRZ blended films.Furthermore,corresponding thermally activated delayed fluorescence(TADF)-and TADF-sensitized fluorescence(TSF)-OLEDs based on CzO-TRZ demonstrated external quantum efficiencies(EQEs)of 33.4% and 30.3%,respectively,highlighting its versatile applications as both an emitter and sensitized host.

关键词： organic electronics organic light-emitting diodes polycyclic aromatic hydrocarbons multiple-resonance

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High-Performance Recyclable Furan-based Epoxy Resin and Its Carbon Fiber Composites with Dense Hydrogen Bonding

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Chinese Journal of polymer Science 2024年第1期42卷 73-86,I0008页

作者： Chang-Bo Zhao Lu-Kun Feng Hui Xie Ming-Liang Wang Bing Guo Zhi-Yong Xue Cai-Zhen Zhu Jian Xu Advanced materials Research Institute North China Electric Power UniversityBejing 102206China Institute of Low-Dimensional materials Genome Initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China Chengdu Institute of organic Chemistry Chinese Academy of SciencesChengdu 610041China School of Science and Shenzhen key laboratory of Flexible Printed electronics Technology and Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive ApplicationHarbin Institute of TechnologyShenzhen 518055China

The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of society.Since the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine solution.This study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.

关键词： Furan Hydrogen bond network Dynamic Schiff base Carbon fiber composites Recycling

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用于紫外线成像和无线报警的水凝胶基可伸缩、高稳定性和高性能的光电传感器

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Science China materials 2024年第6期67卷 1926-1937页

作者：洪杰钊姚帝杰王浩丁琼玲罗艺冰于家豪张鹤曾令兴杨柏儒王冰陶凯吴进 State key laboratory of Optoelectronic materials and Technologies and guangdong Province key laboratory of Display Material and Technology School of Electronics and Information TechnologySun Yat-sen UniversityGuangzhou 510275China Ministry of Education key laboratory of Micro and Nano Systems for Aerospace Northwestern Polytechnical UniversityXi’an 710072China Research&Development Institute of Northwestern Polytechnical University in Shenzhen Northwestern Polytechnical UniversityShenzhen 518063China State key laboratory of Transducer Technology Shanghai 200050China guangdong provincial key laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing National Engineering Research Center of Novel Equipment for Polymer ProcessingKey Laboratory of Polymer Processing Engineering(SCUT)Ministry of EducationSouth China University of TechnologyGuangzhou 510641China Engineering Research Center of polymer Green Recycling of Ministry of Education College of Environment and ResourcesFujian Normal UniversityFuzhou 350007China State key laboratory of polymer materials Engineering Sichuan UniversityChengdu 610065China

柔性可穿戴的紫外线探测器在个体紫外线暴露监测、智能仿生眼和军事领域受到广泛关注.然而,传统不可拉伸的材料和器件结构设计限制了设备在可动态变形的人体皮肤和非平面表面上的精确监测应用和稳定附着.在本研究中,我们提出了基于氧化... 详细信息

柔性可穿戴的紫外线探测器在个体紫外线暴露监测、智能仿生眼和军事领域受到广泛关注.然而,传统不可拉伸的材料和器件结构设计限制了设备在可动态变形的人体皮肤和非平面表面上的精确监测应用和稳定附着.在本研究中,我们提出了基于氧化铜/碳-水凝胶-氧化锌/碳的新型应变隔离异质结构的本征可拉伸(拉伸应变或弯曲高达150%)紫外线探测器,该探测器具有高灵敏度(开/关比为2100%)、高稳定性(大于4000次循环),以及快速响应和恢复时间(分别为1.5和4 s).值得注意的是,该探测器通过水凝胶桥在氧化铜/碳和氧化锌/碳电极之间引入的p-n结能带结构,以及离子导电水凝胶中I^(-)/I_(3)^(-)的电化学反应机制,显著提高了其载流子效率和紫外线响应强度.本文通过集成传感器与所设计的电路板,进一步开发了一种无线紫外线报警系统,用于紫外线强度超标警报.此外,本文还设计了一种光电传感器阵列,并将其用作视网膜假体,以实现对环境紫外线强度的实时监测和成像.本文基于水凝胶基异质结构为开发可穿戴、可拉伸的光电紫外线传感器单元和成像阵列提供了一种新的可行方法.

关键词： flexible hydrogel sensors stretchable UV sensors UV imaging array optoelectronic sensors wireless alarm

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Enhancing efficiency and stability of organic solar cells through a simplified four-step synthesis of fully non-fused ring electron acceptor

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Journal of Energy Chemistry 2024年第6期93卷 601-608,I0015页

作者： Chenyang Han Huanhuan Gao Yanna Sun Yuanyuan Kan Zhaozhao Bi Wei Ma Yani Zhang Juan Antonio Zapien Yingguo Yang Ke Gao College of New Energy Xi’an Shiyou UniversityXi’an 710065ShaanxiChina Shandong provincial key laboratory for Science of Material Creation and Energy Conversion Institute of Frontier ChemistrySchool of Chemistry and Chemical EngineeringShandong UniversityQingdao 266237ShandongChina State key laboratory for Mechanical Behavior of materials Xi’an Jiaotong UniversityXi’an 710049ShaanxiChina Department of materials Science and Engineering City University of Hong KongKowloonHong Kong 99907China School of Microelectronics Fudan UniversityShanghai 200433China

Design and synthesis of superior cost-effective non-fullerene acceptors(NFAs)are still big challenges for facilitating the commercialization of organic solar cells(OSCs),yet to be realized.Herein,two medium bandgap fully non-fused ring electron acceptors(NFREAs,medium bandgap,i,e.,1,3-1,8 eV),namely PTR-2Cl and PTR-4Cl are synthesized with only four steps by using intramolecular noncovalent interaction central core,structured alkyl side chain orientation linking units and flanking with different electron-withdrawing end group.Among them,PTR-4C1 exhibits increased average electrostatic potential(ESP)difference with polymer donor,enhanced crystallinity and compactπ-πstacking compared with the control molecule PTR-2CI.As a result,the PTR-4Cl-based OSC achieved an impressive power conversion efficiency(PCE)of 14.72%,with a much higher open-circuit voltage(V_(OC))of 0.953 V and significantly improved fill factor(FF)of 0.758,demonstrating one of the best acceptor material in the top-performing fully NFREA-based OSCs with both high PCE and V_(OC).Notably,PTR-4Cl-based cells maintain a good T_80lifetime of its initial PCE after over 936 h under a continuous thermal annealing treatment and over1300 h T_(80)lifetime without encapsulation.This work provides a cost-effective design strategy for NFREAs on obtaining high V_(OC),efficient exciton dissociation,and ordered molecular packing and thus high-efficiency and stable OSCs.

关键词： organic solar cells Fully non-fused ring acceptors End group engineering Morphology regulation High efficiency

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Aza-BODIPY dye with unexpected bromination and high singlet oxygen quantum yield for photoacoustic imaging-guided synergetic photodynamic/photothermal therapy

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Chinese Chemical Letters 2024年第6期35卷 445-450页

作者： Leichen Wang Anqing Mei Na Li Xiaohong Ruan Xu Sun Yu Cai Jinjun Shao Xiaochen Dong key laboratory of Flexible electronics(KLOFE)&Institute of Advanced materials(IAM) Nanjing Tech University(NanjingTech)Nanjing 211800China School of Chemistry&materials Science Jiangsu Normal UniversityXuzhou 221116China Center for Rehabilitation Medicine Rehabilitation&Sports Medicine Research Institute of Zhejiang ProvinceDepartment of Rehabilitation MedicineZhejiang Provincial People’s Hospital(Affiliated People’s HospitalHangzhou Medical College)Hangzhou 310014China

Introducing heavy halogen atoms into organic small molecules is a practical strategy for efficient singlet oxygen(^(1)O_(2))generation.Generally,bromine or iodine atoms are introduced on the aza-borondipyrromethene(aza-BODIPY)core,rather than on the periphery aryl rings for efficient~1O_(2) generation.Herein,an aza-BODIPY dye NBDPBr with unexpected bromination on the periphery aryl rings was synthesized for photoacoustic(PA)imaging-guided synergistic photothermal therapy(PTT)and photodynamic therapy(PDT)in tumor cells.Owing to unexcepted bromination at the periphery aryl rings,NBDPBr demonstrated an outstanding singlet oxygen quantum yield(Φ_(Δ))of 66% which was superior to similar brominated photosensitizers previously reported.After encapsulation with amphiphilic polymer F-127,hydrophilic NBDPBr nanoparticles(NPs)were fabricated and exhibited an excellent photothermal conversion efficiency(η)of 43.0% under 660 nm photoirradiation.In vivo PA imaging results demonstrated that NBDPBr NPs could specifically accumulate at tumor sites and realized the maximum tumor retention at 7 h post-injection.All the in vitro and in vivo results indicated the significant potence of NBDPBr with unexpected bis-bromination for PA imaging-guided synergetic PDT/PTT.

关键词： Unexpected bromination Aza-BODIPY Photodynamic therapy Photothermal therapy Synergetic therapy

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Metal to insulator transition for conducting polymers in plasmonic nanogaps

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Light(Science & Applications) 2024年第1期13卷 23-32页

作者： Yuling Xiong Rohit Chikkaraddy Charlie Readman Shu Hu Kunli Xiong Jialong Peng Qianqi Lin Jeremy J.Baumberg NanoPhotonics Centre Cavendish LaboratoryDepartment of PhysicsUniversity of CambridgeCambridgeCB30HEUK School of Physics&Astronomy University of BirminghamEdgbastonBirminghamUK College of Advanced Interdisciplinary Studies and Hunan provincial key laboratory of Novel Nano-Optoelectronic Information materials and Devices National University of Defense TechnologyChangshaChina Hybrid materials for Opto-electronics Group Department of Molecules and MaterialsMESA+Institute for NanotechnologyMolecules Center and Center for Brain-Inspired Nano SystemsFaculty of Science and TechnologyUniversity of TwenteEnschedeNetherlands

Conjugated polymers are promising material candidates for many future applications in flexible displays, organic circuits, and sensors. Their performance is strongly affected by their structural conformation including both electrical and optical anisotropy. Particularly for thin layers or close to crucial interfaces, there are few methods to track their organization and functional behaviors. Here we present a platform based on plasmonic nanogaps that can assess the chemical structure and orientation of conjugated polymers down to sub-10 nm thickness using light. We focus on a representative conjugated polymer, poly(3,4-ethylenedioxythiophene) (PEDOT), of varying thickness (2-20 nm) while it undergoes redox in situ. This allows dynamic switching of the plasmonic gap spacer through a metal-insulator transition. Both dark-field (DF) and surface-enhanced Raman scattering (SERS) spectra track the optical anisotropy and orientation of polymer chains close to a metallic interface. Moreover, we demonstrate how this influences both optical and redox switching for nanothick PEDOT devices.

关键词： transition insulator conjugated

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