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High-speed flexible near-infrared organic photodiode for optical communication

National science Review 2024年第3期11卷 227-238页

作者： Yu Zhu Hongbin Chen Ruiman Han Hao Qin Zhaoyang Yao Hang Liu Yanfeng Ma Xiangjian Wan Guanghui Li Yongsheng Chen The centre of nanoscale science and technology and key laboratory of Functional Polymer Materials Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer Materials College of Chemistry and Renewable Energy Conversion and Storage Center(RECAST) Nankai University state key laboratory of elemento-organic chemistry Nankai University

Optical communication is a particularly compelling technology for tackling the speed and capacity bottlenecks in data communication in modern society. Currently, the silicon photodetector plays a dominant role in high-speed optical communication across the visible-near-infrared spectrum. However, its intrinsic rigid structure, high working bias and low responsivity essentially limit its application in next-generation flexible optoelectronic devices. Herein, we report a narrow-bandgap non-fullerene acceptor（NFA） with a remarkable π-extension in the direction of both central and end units（CH17） with respect to the Y6 series, which demonstrates a more effective and compact 3D molecular packing, leading to lower trap states and energetic disorders in the photoactive film. Consequently, the optimized solution-processed organic photodetector（OPD） with CH17 exhibits a remarkable response time of 91 ns（λ = 880 nm） due to the high charge mobility and low parasitic capacitance, exceeding the values of most commercial Si photodiodes and all NFA-based OPDs operating in self-powered mode. More significantly, the flexible OPD exhibits negligible performance attenuation（<1%） after bending for 500 cycles, and maintains 96% of its initial performance even after 550 h of indoor exposure. Furthermore, the high-speed OPD demonstrates a high data transmission rate of 80 MHz with a bit error rate of 3.5 × 10-4, meaning it has great potential in next-generation high-speed flexible optical communication systems.

关键词： flexible organic photodetector high-speed NIR organic photodetector optical communication light fidelity narrow-bandgap non-fullerene acceptors

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Delicate chemical structure regulation of nonfullerene acceptor for efficient and large thickness organic solar cells

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science China chemistry 2024年第5期67卷 1596-1604页

作者： Zhe Zhang Wanying Feng Yunxin Zhang Shaohui Yuan Yuyang Bai Peiran Wang Zhaoyang Yao Chenxi Li Tainan Duan Xiangjian Wan Bin Kan Yongsheng Chen state key laboratory and Institute of elemento-organic chemistry Frontiers Science Center for New Organic MatterThe Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China School of Materials science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Chongqing Institute of Green and Intelligent technology Chongqing SchoolUniversity of Chinese Academy of Sciences(UCAS Chongqing)Chinese Academy of SciencesChongqing 400722China

Inspired by the success of CH-series acceptors, a small-molecular acceptor, CH-Tz was reported by adopting a new conjugationextended electron-deficient unit([1,2,5]thiadiazolo[3,4-b]pyrazine) on the central core. Owing to the enhanced inter-/intramolecular interactions, CH-Tz exhibited near-infrared absorption and an effective three-dimensional molecular packing network in its single crystal. When blended with polymer donor PM6, the binary device achieved a high power conversion efficiency(PCE) of 18.54%, with a notable short-circuit current density(J_(sc)) of 27.54 m A cm-2and an excellent fill factor(FF) over 80%,which can be partly ascribed to the balanced charge transport properties in the blend film. After employing D18-Cl as the third component, an enhanced PCE of 18.85% was achieved due to a more obvious fiber network. Impressively, the CH-Tz-based OSC devices show excellent thermal stability and thickness insensitivity. Record-breaking Jscof 28.92 m A cm-2was reached for PM6:D18-Cl:CH-Tz ternary device with a thickness of 560 nm. Besides, CH-Tz shows potential in fabricating multicomponent high-performance organic solar cells, where over 19% efficiency could be realized in the quaternary device. Our work advances the strong influence of electron-deficient central units on molecular photovoltaic properties and guides the design of acceptors for stable and large-thickness organic solar cells.

关键词： organic solar cells non-fullerene acceptor central unit large thickness molecular packing

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A case study of comparing two dimerized acceptor molecules built by different branch-connected and terminal-connected approaches

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science China chemistry 2024年第5期67卷 1687-1696页

作者： Kangqiao Ma Huazhe Liang Yuxin Wang Tengfei He Tainan Duan Xiaodong Si Wendi Shi Guankui Long Xiangjian Cao Zhaoyang Yao Xiangjian Wan Chenxi Li Bin Kan Yongsheng Chen state key laboratory and Institute of elemento-organic chemistry Frontiers Science Center for New Organic MatterThe Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsInstitute of Polymer ChemistryRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China School of Materials science and Engineering National Institute for Advanced MaterialsRenewable Energy Conversion and Storage Center(RECAST)Nankai UniversityTianjin 300350China Chongqing Institute of Green and Intelligent technology Chongqing SchoolUniversity of Chinese Academy of Sciences(UCAS Chongqing)Chinese Academy of SciencesChongqing 400015China

Dimerized small-molecule acceptors(SMAs) built by the conventional connection of terminal groups of monomers have contributed to exciting long-term stabilities of organic solar cells(OSCs). However, device efficiencies, especially fill factors(FFs), still need to be improved. This probably originates from unsymmetrical molecular structure/conformation-determined less compact/ordered molecular stackings, such as ineffective stackings of constraint terminals. Herein, an exotic dimerized SMA of BC-Th is established by bridging the branched groups(BC-type, branch coupling) of two monomers rather than conventional terminal units(TC-type, terminal coupling). Benefiting from the three-dimensional conformation and more uncurbed terminals,BC-Th exhibits multiple molecular orientations along with a larger dielectric constant and electron mobility compared with TCTh. Finally, an efficiency of 17.43% is achieved by BC-Th-based OSCs, along with the highest FF of 79.13% among all dimerized SMAs-based OSCs to date. When introducing L8-BO as the third component, overall enhanced efficiency of 18.05%and FF of 80.11% are further afforded. Contrarily, TC-Th-based OSCs exhibit much inferior PCE of 16.29% and FF of 74.81%,demonstrating the great advantages of “branch coupling” over “terminal coupling” when building dimerized SMAs.

关键词： organic solar cells dimerized acceptor molecules branch coupling morphology control stability

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The first chiral cerium halide towards circularly-polarized luminescence in the UV region

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science China chemistry 2024年第6期67卷 1961-1968页

作者： Xinyi Niu Zhichao Zeng Zhaoyu Wang Haolin Lu Bing Sun Hao-Li Zhang Yongsheng Chen Yaping Du Guankui Long Tianjin key Lab for Rare Earth Materials and Applications Renewable Energy Conversion and Storage CenterSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China Tianjin key Lab for Rare Earth Materials and Applications Center for Rare Earth and Inorganic Functional MaterialsHaihe Laboratory of Sustainable Chemical TransformationsSmart Sensing Interdisciplinary Science CenterSchool of Materials Science and EngineeringNational Institute for Advanced MaterialsNankai UniversityTianjin300350China state key laboratory of Applied organic chemistry Key Laboratory of Special Function Materials and Structure Design(Ministry of Education)College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000China the centre of nanoscale science and technology and state key laboratory of elemento-organic chemistry Frontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China

Chiral organic-inorganic hybrid metal halides(OIHMHs)have attracted broader scientific community recently in spin lightemitting diodes,and circularly polarized light-emitting ***,the emission peaks of the reported chiral OIHMHs mainly locate in the visible region,and chiral OIHMH with ultraviolet(UV)circularly polarized luminescence(CPL)has been rarely *** fill this gap,cerium,a unique rare-earth(RE)element with tunable luminescence from UV to the visible region owing to the 4 f-related electronic transition,was introduced to construct the first RE-based chiral OIHMHs,R/*** chirality is successfully transferred from the chiral organic cations to the inorganic cerium chloride framework in R/S-MCC,as confirmed by the single crystal structures,circular dichroism,and *** emission spectra of R/S-MCC are in the UV region,originating from the characteristic d-f transition of Ce^(3+),which making the Ce-based metal halides are ideal candidates towards CPL light sources in the UV ***,R-and S-MCC are the first RE-based OIHMHs,also the first chiral metalhalides with UV *** work opens a new avenue for the development of the chiral OIHMH family towards RE-based chiral *** RE-based chiral metal halides couple the unique and superior optical,electrical,magnetic,and spintronic properties of RE elements with chirality could accelerate the development of chiral optoelectronics and spintronics toward real applications.

关键词： chiral rare-earth halide ultraviolet circularly-polarized luminescence d-f transition rare-earth halide perovskite chiral perovskite

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一种实现任意窄带光谱检测的有机光电探测器通用策略

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science China Materials 2024年第3期67卷 852-862页

作者：朱玉秦灏郭婷婷杨艳青张哲张京李明朋陈红滨吴思敏韩蕊蔓万相见李光辉陈永胜 The centre of nanoscale science and technology and key laboratory of Functional Polymer Materials Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer MaterialsCollege of Chemistryand Renewable Energy Conversion and Storage Center(RECAST)Nankai UniversityTianjin 300071China state key laboratory of elemento-organic chemistry Nankai UniversityTianjin 300071China

窄带光电探测器因其优异的综合性能,在光谱仪、激光雷达、光通信和监控等关键应用领域广受欢迎.尽管窄带硅基探测器在当前市场上占据主导地位,但其本征刚性、光学带隙固定和尺寸大的特性极大地限制了其在新兴领域的应用,尤其是在柔性和... 详细信息

窄带光电探测器因其优异的综合性能,在光谱仪、激光雷达、光通信和监控等关键应用领域广受欢迎.尽管窄带硅基探测器在当前市场上占据主导地位,但其本征刚性、光学带隙固定和尺寸大的特性极大地限制了其在新兴领域的应用,尤其是在柔性和可穿戴光电子领域.在本工作中,我们报道了一种构筑窄带有机光电探测器(OPD)的简单通用策略.该策略通过溶液法将活性层中的给体和受体材料制备成光学调制层(OAL),并集成在OPD上,可实现对任意光谱的检测.利用该策略,我们成功地构筑了以750 nm为中心的窄带OPD,其半峰宽(FWHM)为40 nm,光谱响应率为3667,-3 dB截止频率为927 kHz,打破了自驱动窄带OPD的性能记录.值得注意的是,这种新颖的OAL策略在OPD中具有良好的通用性,可以实现对600至1000 nm范围内的任意窄光谱检测,具有FWHM可调(最小步长为2 nm)、响应度和探测率高、响应速度快的优势.受益于有机半导体固有的柔性特性,我们构筑了一种柔性且可弯曲的窄带近红外OPD线性阵列,并应用于全向激光雷达上,在无需机械旋转的情况下实现了360°水平扫描.

关键词： organic photodetector narrowband organic photodetector LiDAR flexible photodetector visible-near-infrared narrowband organic photodetector

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

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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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d-Orbital steered FeN_(4)moiety through N,S dual-site adjustation for zinc-air flow battery

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Journal of Energy chemistry 2024年第5期92卷 8-15页

作者： Chunzhu Bao Mingwei Tong Xueli Li Zhonghua Xiang state key laboratory of organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing 100029China

The implementation of pristine covalent organic polymer(CO_(2)P)with well-defined structure as air electrode may spark fresh vitality to rechargeable zinc-air flow batteries(ZAFBs),but it still remains challenges in synergistically regulating their electronic states and structural porosity for the great device ***,we conquer these issues by exploiting N and S co-doped graphene with COP rich in metal-ligand nitrogen to synergistically construct an effective catalyst for oxygen reduction reaction(ORR).Among them,the N and S co-doped sites with high electronegativity properties alter the number of electron occupations in the d orbital of the iron centre and form electron-transfer bridges,thereby boosting the selectivity of the ORR-catalysed four-electron ***,the introduction of COP materials aids the formation of pore interstices in the graphene lamellae,which both adequately expose the active sites and facilitate the transport of reactive *** from the synergistic effect,as-prepared catalyst exhibits excellent half-wave potentials(E_(1/2)=912 mV)and stability(merely 8.8%drop after a long-term durability test of 50000 s).Further,ZAFBs assembled with the N/SG@CO_(2)P catalyst demonstrate exceptional power density(163.8 mW cm^(-2))and continuous charge and discharge for approximately 140 h at 10 mA cm^(-2),outperforming the noble-metal benchmarks.

关键词： Nitrogen/sulfurdual sites Metal-coordinated nitrogen sites Covalent organic polymer Oxygen reduction reaction Zn-airflow battery

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Highly efficient and stable 2D/3D perovskite solar cells based on surface reconstruction and energy level alignment

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science China chemistry 2024年

作者： Qiaohui Li Hang Liu Tong Zhou key laboratory of Rubber-Plastics Ministry of Education/Shandong Provincial Key Laboratory of Rubber-Plastics Qingdao University of Science and Technology The centre of nanoscale science and technology and key laboratory of Functional Polymer Materials Institute of Polymer ChemistryCollege of Chemistry Nankai University

Realizing simultaneous adjustment of energy levels and work functions in two-dimensional/three-dimensional （2D/3D） perovskite solar cells （PSCs） is a ***,a pseudohalide 3,5-bis （trifluoromethyl） benzylammonium tetrafluoroborate （TF-PMABF4） was used to react with unreacted PbI2on the surface of 3D bulky perovskite to form a mixed halide of 2D perovskite denoted （TF-PMA）2FA2Pb3I8（BF4）*** novel 2D/3D perovskite enables the simultaneous adjustment of energy levels and work functions on the surface of active *** to the significantly enhanced quality of 2D/3D perovskite film,decreased surface defects and increased charge carrier lifetime,the 2D/3D PSCs exhibit an outstanding power conversion efficiency （PCE）of 25.15%and a high VOCof 1.194 ***,2D/3D PSCs exhibit remarkable enhancements in environmental stability,unencapsulated devices retaining more than 90%of their initial PCE at 50%humidity for 2,280 h.

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通过羧甲基纤维素和硅氧烷的协同作用提升锂离子电池干法正极的循环稳定性

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science China Materials 2024年第1期67卷 76-84页

作者：倪铭韩赵阳许诺孔萌昕马延风李晨曦张洪涛陈永胜 The centre of nanoscale science and technology and key laboratory of Functional Polymer Materials Institute of Polymer ChemistryCollege of ChemistryNankai UniversityTianjin 300071China state key laboratory of elemento-organic chemistry Nankai UniversityTianjin 300071China Renewable Energy Conversion and Storage Center(RECAST) Nankai UniversityTianjin 300071China Tianjin Plan Nano Co. LtdTianjin 300071China

近年来,无溶剂干法电极制备工艺由于其低成本和低污染等优点在锂电池领域获得了广泛关注.然而,现有干法制备工艺中采用的聚四氟乙烯(PTFE)粘结剂存在粘附力和循环稳定性不足等缺点,限制了其实际工业化应用.我们通过引入羧甲基纤维素(CMC... 详细信息

近年来,无溶剂干法电极制备工艺由于其低成本和低污染等优点在锂电池领域获得了广泛关注.然而,现有干法制备工艺中采用的聚四氟乙烯(PTFE)粘结剂存在粘附力和循环稳定性不足等缺点,限制了其实际工业化应用.我们通过引入羧甲基纤维素(CMC)和硅氧烷作为粘结剂复合材料,发展了一种与现有工业化生产兼容的锂离子电池干法电极制备工艺.CMC和硅氧烷的协同作用增强了电极活性材料的粘附性能,实现了干法电极膜片机械强度和电化学性能的大幅提升.基于这种干法电极工艺制备的铝掺杂锰酸锂(LMA/CS)半电池在1 C下循环200圈后展示出79.8%的保持率.进一步地,制备的高负载(20.6 mg cm^(-2))锰酸锂-钛酸锂全电池(LMA/CS||LTO)实现了1000圈的超长稳定循环,容量保持率高达89.2%,超过现有基于PTFE粘结剂干法工艺和传统湿法工艺的电池性能.

关键词：锂离子电池锰酸锂循环稳定性羧甲基纤维素硅氧烷干法工艺粘附性能粘附力

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A solubility limited pyrene-4,5,9,10-tetraone-based covalent organic framework for high-performance aqueous zinc-organic batteries

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Nano Research 2024年第6期17卷 5095-5103页

作者： Min Cheng Shibing Zheng Tianjiang Sun Diantao Li Weijia Zhang Zhengtai Zha Qiong Sun Jing Tian Kai Zhang Zhanliang Tao Frontiers science Center for New organic Matter State Key Laboratory of Advanced Chemical Power SourcesKey Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Renewable Energy Conversion and Storage CentreNankai UniversityTianjin 300071China Haihe laboratory of Sustainable Chemical Transformations Tianjin 300192China

Pyrene-4,5,9,10-tetraone(PTO),with a high theoretical capacity of 408 mAh·g^(−1),is a promising candidate for rechargeable aqueous zinc-ion batteries(RAZIBs),but its zincated products during discharge process suffer from high solubility in ***,aβ-ketoenamine-linked two-dimensional(2D)covalent organic framework(COF)based on a 2,7-diaminopyrene-4,5,9,10-tetraone(4KT-BD)monomer and a 2,4,6-trihydroxy-benzene-1,3,5-tricarbaldehyde(Tp)node(4KT-Tp-COF)is synthesized to address the above *** well-designed 4KT-Tp-COF displays low solubility in 3 M Zn(CF3SO3)2 owing to the favorableπ-πstacking as well as extended ***,the ingenious structural design of the active molecule and the long-range ordered nano-channels alter the intramolecular electron distribution,which facilitates the ionic ***,the 4KT-Tp-COF cathode exhibits a stable capacity of 181 mAh·g^(−1)at 0.2 A·g^(−1),superior rate capability of 139 mAh·g^(−1)at 20 A·g^(−1),and a long lifetime of 1000 cycles without capacity loss at 30 A·g^(−1).Even at a low temperature of−20°C,the electrode also performs an ultralong cycling life of 9000 cycles with a capacity of 106 mAh·g^(−1)at 5 A·g^(−1).The comprehensive characterizations of ex-situ analyses together with the theoretical calculations validate that the groups of C=O can contribute highly accessible redox-active sites for Zn^(2+)*** ultra-stable 4KT-Tp-COF cathode provides important insights for designing robust organic electrodes for sustainable and large-scale electrochemical energy storage.

关键词： pyrene-4,5,9,10-tetraone solubility limited covalent organic framework zinc batteries

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