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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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Supramolecular polymer network constructed by a functionalized polyimidazolium salt derived from metal-carbene template approach

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Science China chemistry 2024年第4期67卷 1224-1228页

作者： Ming-Ming Gan Zi-En Zhang Yi-Fan Zhang Heng Zhang Li-Ying Sun Ying-Feng Han Key laboratory of Synthetic and Natural Functional Molecule chemistry of the Ministry of Education Xi’an Key Laboratory of Functional Supramolecular Structure and MaterialsCollege of Chemistry and Materials ScienceNorthwest UniversityXi’an 710127China

In this study,we present a supramolecular templating approach for constructing polyimidazolium salt containing crown ether and cyclobutane *** strategy involves the formation of metal-carbene templates,photochemical cycloaddition,and subsequent demetallation of metal *** by the host-guest chemistry between crown ether units and ammonium salts,we successfully fabricated a supramolecular polymer SPN1,which features imidazolium receptors and cyclobutane *** obtained SPN1 demonstrates outstanding reversible stimulus-response,antibacterial behavior and conductivity.

关键词： metal-carbene template crown ether polyimidazolium salt host-guest chemistry

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Hydrothermal synthesis of polyimide-linked covalent organic frameworks towards ultrafast and stable cathodic sodium storage

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Science China chemistry 2024年第4期67卷 1300-1310页

作者： Xiya Yang Lei Gong Zhixin Liu Qianjun Zhi Baoqiu Yu Xin Chen Kang Wang Xiaofeng Li Dongdong Qi Jianzhuang Jiang Beijing Advanced Innovation Center for materials Genome Engineering Beijing Key Laboratory for Science and Application of Functional Molecular and Crystalline MaterialsDepartment of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China State Key laboratory of Organic-Inorganic Composites College of Materials Science and EngineeringBeijing University of Chemical TechnologyBeijing 100029China

Redox-active organic materials are capturing growing attention as cathode materials for sustainable alkaline metal ion ***,the storage of Na+in most organic materials-based cathodes is plagued by low capacity and unsatisfying rate performance due to their low active site densities and limited exposed active ***,two polyimide-linked covalent organic frameworks(COFs),namely HATN-PD-COF and HATN-TAB-COF,were fabricated from hydrothermal synthesis with redoxactive triphenylene-2,3,6,7,10,11-hexacarboxylic acid and aromatic amines as starting *** X-ray diffraction and electron microscopy analysis indicate the high crystalline nature of these COFs with AA stacking configuration and orderly mesoporous tunnel.N_(2) sorption measurement discloses the permanent porosity of these two COFs with a Brunauer-EmmettTeller surface area of 1,065-1,200 m^(2)g^(-1)and a large pore size of 2.0-3.1 *** intermittent titration technique and density functional theory calculations reveal the facile Na+ion diffusion along the mesoporous tunnel of these COFs with a small energy barrier of 0.13-0.40 e *** particular,the as-prepared COFs based-cathodes show ultrafast and stable Na+storage associated with their conjugated electronic structure,highly ordered mesoporous tunnel,robust structure,and redox-active C=N/C=O-rich framework as exemplified by the high reversible capacity of 210 m A h g^(-1)at 200 m A g^(-1),record-high rate performance(195 m A h g^(-1)at a high current density of 10,000 m A g^(-1))among organic electrodes and the capacity retention of nearly 91%at 10,000 m A g^(-1)after 7,000 cycles for HATN-PD-COF.

关键词： covalent organic framework sodium ion battery cathode high rate organic electrode

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Selective oxygen electroreduction to hydrogen peroxide in acidic media:The superiority of single-atom catalysts

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Nano Research 2024年第6期17卷 4668-4681页

作者： Ergui Luo Tongtong Yang Jingyi Liang Yuhong Chang Junming Zhang Tianjun Hu Junjie Ge Jianfeng Jia Key laboratory of Magnetic Molecules and Magnetic Information materials of Ministry of Education School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China School of chemistry and materials Science University of Science and Technology of ChinaHefei 230026China State Key laboratory of Electroanalytic chemistry Jilin Province Key Laboratory of Low Carbon Chemistry PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

Two-electron oxygen reduction reaction(2e-ORR)provides an environmentally friendly direction for the on-site production of hydrogen peroxide(H_(2)O_(2)).Central to this technology is the exploitation of efficient,economical,and safe 2e-ORR *** overview starts with the fundamental chemistry of ORR to highlight the decisive role of adsorbing intermediates on the reaction pathway and activity,followed by a comprehensive survey of the tuning strategies to favor 2e-ORR on traditional precious *** latest achievements in designing efficient and selective precious-metal-based single-atom catalysts(SACs)and metal-nitrogen-carbon(M-Nx/C)catalysts,from the aspects of material synthesis,theoretical calculations,and mass transport promotion,are systematically *** introductions on the evaluation metrics for 2e-ORR catalysts and the primary reactor designs for cathodic H_(2)O_(2)synthesis are also *** conclude this review with an outlook on the challenges and direction of efforts to advance electrocatalytic 2e-ORR into realistic H_(2)O_(2)production.

关键词： oxygen reduction reaction H_(2)O_(2)production single-atom catalysts selectivity

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New sustainable polymers with on-demand depolymerization property

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Science China chemistry 2024年第9期67卷 2803-2841页

作者： Yangyang Sun Zesheng An Yanshan Gao Rongrong Hu Ye Liu Hua Lu Xiao-Bing Lu Xuan Pang Anjun Qin Yong Shen Youhua Tao Yu-Zhong Wang Junpeng Wang Gang Wu Guang-Peng Wu Tie-Qi Xu Xing-Hong Zhang Yuetao Zhang Zhenbiao Zhang Jian-Bo Zhu Miao Hong Zhibo Li State Key laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China State Key laboratory Base of Eco-Chemical Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao266042China State Key laboratory of Supramolecular Structure and materials College of ChemistryJilin UniversityChangchun 130012China State Key laboratory of Luminescent materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesSouth China University of TechnologyGuangzhou 510640China State Key laboratory of Fine Chemicals Frontiers Science Center for Smart MaterialsDalian University of TechnologyDalian 116024China 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 Key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)College of ChemistryState Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610064China School of Polymer Science and Polymer Engineering the University of AkronAkronOH 44325USA MOE Key laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China State and Local Joint Engineering laboratory for Novel Functional Polymeric materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

To combat the crisis of today's synthetic polymers arising from unsustainable production and disposal,it is essential for the synthetic polymer community to reshape the current polymer industry with sustainable *** an emerging class of sustainable polymers,the development of chemically depolymerizable polymers(CDPs),which can undergo closed-loop depolymerization/repolymerization cycles to reproduce virgin polymers without the loss of properties from recovered monomers,offers an ideal solution to preserve finite natural resources,provides a feasible solution to the end-of-life issue of polymer waste,and thereby establishes a circular materials ***,two grand key challenges have been encountered in the establishment of practically useful CDPs:how to balance polymerization and depolymerization ability and how to unify conflicted depolymerizability and physical ***,this critical review article presents our vision for summarizing feasible strategies to overcome the above two significant challenges and the design principles for constructing an ideal CDP by highlighting selected major progress made in this rapidly expanding field.

关键词： chemically depolymerizable polymers sustainable polymers depolymerization monomer recovery degradation plastics

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Integrating Homogeneous and Heterogeneous Catalysis in a Copper Nanocluster with Lewis Acid–Base Sites for Chemical Conversion of CO_(2) and Propargylamine

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CCS chemistry 2024年第9期6卷 2131-2141页

作者： Wan-Zhen Qiao Yu-Jue Wang Si Li Rui Wang Jie Wu Shuang-Quan Zang Henan Key laboratory of Crystalline molecular Functional materials Henan International Joint Laboratory of Tumor Theranostical Cluster MaterialsGreen Catalysis and College of ChemistryZhengzhou UniversityZhengzhou 450001

It remains a significant challenge to develop a catalyst that merges the advantages of homogeneous and heterogeneous catalysis with high reactivity and great ***,an atomically precise Cu_(6)-NH_(2) nanocluster with distorted octahedral Cu_(6) core and NH_(2)-functionalized ligands has been developed as the first homo/heterogeneous catalyst to catalyze the cyclization reaction of propargylic amines with carbon dioxide(CO_(2))under mild *** a homogeneous catalyst,Cu_(6)-NH_(2) shows excellent catalytic activity with high turnover frequency due to highly accessible active *** definite coordination geometry and homogeneity nature of active centers make it convenient to investigate the structure–activity relationship at the atomic level through experiments and theory *** addition,the nanocluster exhibits excellent stability,great recrystallizability,and reusability in five catalytic cycles,in which its catalytic performance has no obvious ***,Cu_(6)-NH_(2) incorporates Lewis acid and base sites in metal and ligand,respectively,which can promote catalytic efficiency in a synergistic effect in the absence of any ***,Cu_(6)-NH_(2) can realize direct conversion of CO_(2) in simulated flue gas into oxazolidinones with high *** metal-ligand cooperative effect and integrated advantages of homogeneous and heterogeneous catalysis would provide new perspectives to achieve advanced metal nanocluster catalysts for CO_(2) conversion.

关键词： copper nanocluster atomically precise structure Lewis acid-base sites CO_(2)cyclization reaction cocatalyst-free

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Regulation of Lithium-Ion Flux by Nanotopology Lithiophilic Boron-Oxygen Dipole in Solid Polymer Electrolytes for Lithium-Metal Batteries

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Energy & Environmental materials 2024年第4期7卷 74-82页

作者： Manying Cui Hongyang Zhao Yanyang Qin Shishi Zhang Ruxin Zhao Miao Zhang Wei Yu Guoxin Gao Xiaofei Hu Yaqiong Su Kai Xi Shujiang Ding School of chemistry Engineering Research Center of Energy Storage Materials and Devices Ministry of Education State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Department of materials and Environmental chemistry Stockholm University

Inhomogeneous lithium-ion （Li+） deposition is one of the most crucial problems,which severely deteriorates the performance of solid'State lithium metal batteries （LMBs）.Herein,we discovered that covalent organic framework （COF-1） with periodically arranged boron-oxygen dipole lithiophilic sites could directionally guide Li+even deposition in asymmetric solid polymer electrolytes.

关键词： covalent organic framework ion transport regulation lithium metal battery solid polymer electrolyte

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Engineering the Interface Between Au Nanoparticles and CoO-Ov to Enhance the Catalytic Performance of 5-Hydroxymethylfurfural(HMF)to 2,5-Dimethylfuran(DMF)

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Chemical Research in Chinese Universities 2024年第1期40卷 47-54页

作者： XIANG Shuang GUO Yong LIU Xiaohui WANG Yanqin Key laboratory for Advanced materials and Joint International Research laboratory of Precision chemistry and molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterResearch Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237P.R.China

The interface between Au and support has attracted extensive interest because of its unique catalytic ability for hydrogen activation in catalytic hydrogenation/hydrogenolysis ***,we create the Au-CoO-OV interface in the 1.0%Au/Co3O4-Rod-250 catalyst,which could dissociate H2 via the heterolytic way to yield rich hydride species and achieve excellent catalytic performance in the hydrogenolysis of biomass-derived 5-hydroxymethylfurfural(HMF)to 2,5-dimethylfuran(DMF).The XRD and HRTEM analyses show that Au nanoparticles are uniformly dispersed on CoO-OV surface and in situ DRIFTS spectra show the enhancement of heterolytic dissociation of hydrogen(signals of Au-D and O-D vibration)compared with bare CoO(Co3O4-Rod-250).This work provides insights for fabricating highly active Au-support catalysts for catalytic hydrogenation/hydrogenolysis reactions.

关键词： Au-CoO-OV interface Hydride species Heterolytic dissociation 5-Hydroxymethylfurfural(HMF) 2 5-Dimethylfuran(DMF)

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Production of Functional materials Derived from Regenerated Silk Fibroin by Utilizing 3D Printing and Biomimetic Enzyme-induced Mineralization

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Chinese Journal of Polymer Science 2024年第3期42卷 299-310,I0005页

作者： Ni Chen Fei-Yu Luo Gong-Wen Yang Jin-Rong Yao Xin Chen Zheng-Zhong Shao State Key laboratory of molecular Engineering of Polymers Laboratory of Advanced Materials and Department of Macromolecular ScienceFudan UniversityShanghai 200433China

Critical-sized bone defects, commonly encountered in clinical orthopedic surgery, present a significant challenge. One of the promising solutions is to prepare synthetic bone substitute materials with precise structural control, mechanical compatibility, and enhanced osteogenic induction performance, nevertheless the successful preparation of such materials remains difficult. In this study, a two-step technique,integrating an extrusion-based printing process with biomimetic mineralization induced by alkaline phosphatase(ALP), was developed. Initially,a pre-cured hydrogel of regenerated silk fibroin(RSF) with a small quantity of hydroxypropyl cellulose(HPC) and ALP was prepared through heating the mixed aqueous solution. This pre-cured hydrogel demonstrated thixotropic property and could be directly extruded into predetermined structures through a 3D-printer. Subsequently, the 3D-printed RSF-based materials with ALP underwent biomimetic in situ mineralization in calcium glycerophosphate(Ca-GP) mineralizing solution, utilizing the polymer chains of RSF as templates and ALP as a trigger for cleaving phosphate bonds of Ca-GP. The resulting 3D-printed RSF-mineral composites including hydrogel and sponge possessed adjustable compression modulus of megapascal grade and variable hydroxyapatite content, which could be controlled by manipulating the duration of the mineralization ***, these 3D-printed RSF-mineral composites demonstrated non-cytotoxicity towards rat bone marrow mesenchymal stem cells. Therefore, they may hold great potential for applications involving the replacement of tissues characterized by osteoinductivity and intricate structures.

关键词： Silk protein Alkaline phosphatase Extrusion-based printing Biomineralization

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A High-Performance Electrochemical Analysis Platform for Ultrasensitive Detection of HTLV-1 DNA: Integrating Cascade Signal Amplifi cation with λ-Exonuclease-Assisted Target Recycling and Enzyme Catalysis

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Journal of Analysis and Testing 2024年第3期8卷 361-373页

作者： Qi Xiao Shuai Liu Yali Wang Huihao Li Mingli Yang Yi Fang Sijing Chen Shan Huang Guangxi Key laboratory of Natural Polymer chemistry and Physics College of Chemistry and Materials Nanning Normal University

Human T-cell lymphophilic virus type 1 (HTLV-1), the known retrovirus causing cancer in humans, is closely associated with adult T-cell leukemia/lymphoma and HTLV-1 associated myelopathy/tropical spastic paraparesis. Due to its ability to evade the host's defense mechanisms, early tracking of HTLV-1 becomes crucial. In this study, we integrateλ-Exonuclease(λ-Exo)-assisted target recycling with a terminal deoxynucleotidyl transferase (TdT)-mediated template-free DNA extension process to develop an electrochemical analysis platform for the specifi c and sensitive detection of HTLV-1 DNA. During theλ-Exo-assisted target recycling, HTLV-1 DNA is recognized by hairpin DNA (Hp-DNA), forming double-stranded DNA(dsDNA) through DNA hybridization. The dsDNA, featuring blunt 5'terminal phosphorylation, is cleaved byλ-Exo, generating abundant short output sequence (sDNA). HTLV-1 DNA is released, initiating a cyclic hybridization-cleavage ***, thiol-labelled capture DNA (CP-DNA) assembled on gold electrode surface captures a substantial amount of the generated sDNA, forming CP-DNA-sDNA nanostructures. When TdT and dNTPs are present on the electrode surface, the3'-OH terminal of sDNA extends to generate long single-stranded DNA (ssDNA) structure. Methylene blue (MB) is selected as the electrochemical signal molecule. MB not only binds with ssDNA but also interacts specifi cally with dsDNA, resulting in a signifi cantly enhanced electrochemical signal on modifi ed electrode surface. The detection limit of HTLV-1 DNA is as low as 19 amol/L (S/N=3) when the two signal amplifi cation strategies are combined. The analysis platform exhibits excellent analytical performance and holds promise as a novel tool for the early tracing and diagnosis of HTLV-1 DNA.

关键词： Cascade signal amplification Electrochemical DNA sensor Enzyme-assisted target recycling HTLV-1 DNA

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