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Influencing Factors on Li-ion Conductivity and Interfacial Stability of Solid Polymer Electrolytes, Exampled by Polycarbonates, Polyoxalates and Polymalonates

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Angewandte Chemie 2023年第13期135卷

作者： Dr. Xiaoxin Xie Prof. Zhaoxu Wang Dr. Shuang He Kejun Chen Qiu Huang Peng Zhang Prof. Shu-Meng Hao Dr. Jiantao Wang Prof. Weidong Zhou Beijing Advanced Innovation Center for Soft Matter Science and Engineering State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China Contribution: Data curation (lead) Investigation (lead) Writing - original draft (lead) Key Laboratory of Theoretical Organic Chemistry and Functional Molecule of Ministry of Education Hunan University of Science and Technology Hunan 411201 China Contribution: Data curation (equal) Investigation (supporting) Software (equal) Contribution: Investigation (supporting) Software (supporting) Contribution: Investigation (supporting) Contribution: Supervision (supporting) China Automotive Battery Research Institute Co. Ltd. Beijing 101407 China

The application of solid polymer electrolytes (SPEs) in all-solid-state(ASS) batteries is hindered by lower Li + -conductivity and narrower electrochemical window. Here, three families of ester-based F-modified SPEs of poly-carbonate (PCE), poly-oxalate (POE) and poly-malonate (PME) were investigated. The Li + -conductivity of these SPEs prepared from pentanediol are all higher than the counterparts made of butanediol, owing to the enhanced asymmetry and flexibility. Because of stronger chelating coordination with Li + , the Li + -conductivity of PME and POE is around 10 and 5 times of PCE. The trifluoroacetyl-units are observed more effective than −O−CH 2 −CF 2 −CF 2 −CH 2 −O− during the in situ passivation of Li-metal. Using trifluoroacetyl terminated POE and PCE as SPE, the interfaces with Li-metal and high-voltage-cathode are stabilized simultaneously, endowing stable cycling of ASS Li/LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) cells. Owing to an enol isomerization of malonate, the cycling stability of Li/PME/NCM622 is deteriorated, which is recovered with the introduce of dimethyl-group in malonate and the suppression of enol isomerization. The coordinating capability with Li + , molecular asymmetry and existing modes of elemental F, are all critical for the molecular design of SPEs.

关键词： All-Solid-State Battery High Voltage Cathode Interfacial Stability Lithium Metal Anode Solid Polymer Electrolyte

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Fluorine-Containing Passivation Layer via Surface Chelation for Inorganic Perovskite Solar Cells

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Angewandte Chemie 2022年第6期135卷

作者： Hao Zhang Prof. Wanchun Xiang Xuejiao Zuo Xiaojing Gu Shiang Zhang Yachao Du Zhiteng Wang Yali Liu Haifeng Wu Peijun Wang Qingyue Cui Hang Su Prof. Qingwen Tian Prof. Shengzhong (Frank) Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University No. 620 West Chang'an Avenue Xi'an 710119 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Writing - original draft (lead) Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (equal) Investigation (equal) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) State Key Laboratory of Organic-Inorganic Composites Key Lab of Biomedical Materials of Natural Macromolecules Ministry of Education Beijing Laboratory of Biomedical Materials Beijing University of Chemical Technology No. 15 East Road North Third Ring Chaoyang District Beijing 100029 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Validation (lead) Visualization (lead) Writing - review & editing (lead) Dalian National Laboratory for Clean Energy iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences No. 457 Zhongshan Road Dalian Liaoning 116023 P. R. China Contribution: Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (equal)

Minimizing surface defect is vital to further improve power conversion efficiency (PCE) and stability of inorganic perovskite solar cells (PSCs). Herein, we designed a passivator trifluoroacetamidine (TFA) to suppress CsPbI 3− x Br x film defects. The amidine group of TFA can strongly chelate onto the perovskite surface to suppress the iodide vacancy, strengthened by additional hydrogen bonds. Moreover, three fluorine atoms allow strong intermolecular connection via intermolecular hydrogen bonds, thus constructing a robust shield against moisture. The TFA-treated PSCs exhibit remarkably suppressed recombination, yielding the record PCEs of 21.35 % and 17.21 % for 0.09 cm 2 and 1.0 cm 2 device areas, both of which are the highest for all-inorganic PSCs so far. The device also achieves a PCE of 39.78 % under indoor illumination, the highest for all-inorganic indoor photovoltaic devices. Furthermore, TFA greatly improves device ambient stability by preserving 93 % of the initial PCE after 960 h.

关键词： Chelation Defect Passivation Inorganic Perovskite Solar Cells

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Amorphous Mo-doped NiS0.5Se0.5Nanosheets@Crystalline NiS0.5Se0.5Nanorods for High Current-density Electrocatalytic Water Splitting in Neutral Media

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Angewandte Chemie 2022年第6期135卷

作者： Dr. Yang Wang Dr. Xiaopeng Li Dr. Zhong Huang Dr. Haozhi Wang Dr. Zelin Chen Dr. Jinfeng Zhang Prof. Xuerong Zheng Prof. Yida Deng Prof. Wenbin Hu State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and Engineering Hainan University Haikou 570228 P. R. China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Validation (lead) Writing - original draft (lead) School of Materials Science and Engineering Tianjin Key Laboratory of Building Green Functional Materials Tianjin Chengjian University Tianjin 300384 China Contribution: Formal analysis (equal) State Key Laboratory of Marine Resource Utilization in South China Sea College of Information and Communication Engineering Hainan University Haikou 570228 P. R. China Contribution: Methodology (equal) Software (equal) Validation (equal) Contribution: Methodology (equal) Software (equal) School of Materials Science and Engineering Tianjin Key Laboratory of Composite and Functional Materials Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education Tianjin University Tianjin 300072 P. R. China Contribution: Methodology (equal) Contribution: Conceptualization (equal) Investigation (equal) Supervision (equal) Contribution: Funding acquisition (lead) Supervision (equal) Contribution: Funding acquisition (supporting)

It is vitally important to develop highly active, robust and low-cost transition metal-based electrocatalysts for overall water splitting in neutral solution especially at large current density. In this work, amorphous Mo-doped NiS 0.5 Se 0.5 nanosheets@crystalline NiS 0.5 Se 0.5 nanorods (Am−Mo−NiS 0.5 Se 0.5 ) was synthesized using a facil one-step strategy. In phosphate buffer saline solution, the Am−Mo−NiS 0.5 Se 0.5 shows tiny overpotentials of 48 and 209 mV for hydrogen evolution reaction (HER), 238 and 514 mV for oxygen evolution reaction (OER) at 10 and 1000 mA cm −2 , respectively. Moreover, Am−Mo−NiS 0.5 Se 0.5 delivers excellent stability for at least 300 h without obvious degradation. Theoretical calculations revealed that the Ni sites in the defect-rich amorphous structure of Am−Mo−NiS 0.5 Se 0.5 owns higher electron state density and strengthened the binding energy of H 2 O, which will optimize H adsorption/desorption energy barriers and reduce the adsorption energy of OER determining step.

关键词： Amorphous Crystalline High-Current-Density Neutral Environment Water Splitting

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Synthesis of tamarind seed gum-based semi-IPN hydrogels with integration of fertilizer retention and anti-evaporation

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Journal of Applied Polymer Science 2022年第3期140卷

作者： Xiaomei Liu Tao Feng Wenbin Ding Wei Zeng Na Wang Fenghong Yang Cailing Yang Shenghua Yang Yanrong Kong Ziqiang Lei Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education Key Laboratory of Eco-environmental Polymer Materials of Gansu Province College of Chemistry and Chemical Engineering Northwest Normal University Lanzhou China Contribution: Data curation (lead) Formal analysis (lead) Methodology (lead) Software (lead) Visualization (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Data curation (supporting) Investigation (supporting) Contribution: Investigation (supporting) Software (supporting) Contribution: Software (supporting) Contribution: Investigation (supporting) Contribution: Conceptualization (lead) Funding acquisition (lead) Methodology (equal) Software (equal) Writing - review & editing (equal)

In this article, a tamarind seed gum-g-poly (acrylic acid-co-2-Acrylamido-2-methyl-1-propane sulfonic acid/polyvinyl alcohol) (TSG-g-P[AA-co-AMPS/PVA]) was prepared by aqueous solution polymerization. The Fourier transform infrared spectroscopy, scanning electron microscopy, and thermogravimetric analysis were used to characterize. The swelling behaviors, reusability and water-retention capabilities of hydrogels were evaluated. Under optimum synthesis conditions, the maximum equilibrium absorption of hydrogel was 1295 g·g −1 , 208 g·g −1 , 116 g·g −1 in deionized water, tap water and NaCl solution (0.9 wt%) respectively. Application of the hydrogel to soils increased their water-holding and fertilizer retention capacities. Furthermore, the excellent water retention anti-evaporation performance indicated that the hydrogel has the potential for applications in future sustainable agriculture and forestry.

关键词： anti-evaporation performance fertilizer retention hydrogels interpenetrating network structure tamarind seed gum

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Highly Stereoselective Diels–Alder Reactions Catalyzed by Diboronate Complexes**

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Angewandte Chemie 2023年第33期135卷

作者： Dr. Yuan-He Li Dr. Su-Lei Zhang Dr. Yong Lu Bo Xiao Dr. Tian-Yu Sun Qian-Qian Xu Prof. Dr. Jia-Hua Chen Prof. Dr. Zhen Yang Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of Education and Beijing National Laboratory for Molecular Science (BNLMS) Peking-Tsinghua Center for Life Sciences Peking University Beijing 100871 China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Methodology (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Writing - review & editing (supporting) Lab of Computational Chemistry and Drug Design State Key Laboratory of Chemical Oncogenomics Peking University Shenzhen Graduate School Shenzhen 518055 China Contribution: Supervision (supporting) Writing - review & editing (supporting) Shenzhen Bay Laboratory Shenzhen 518055 China State Key Laboratory of Chemical Oncogenomics Key Laboratory of Chemical Genomics Peking University Shenzhen Graduate School Shenzhen 518055 China Contribution: Conceptualization (lead) Funding acquisition (lead) Supervision (lead) Writing - review & editing (supporting)

A highly enantioselective catalytic system for exo -Diels–Alder reactions was developed based on the newly discovered bispyrrolidine diboronates (BPDB). Activated by various Lewis or Brønsted acids, BPDB can catalyze highly stereoselective asymmetric exo -Diels–Alder reactions of monocarbonyl-based dienophiles. When 1,2-dicarbonyl-based dienophiles are used, the catalyst can sterically distinguish between the two binding sites, which leads to highly regioselective asymmetric Diels–Alder reactions. BPDB can be prepared as crystalline solids on a large scale and are stable under ambient condition. Single-crystal X-ray analysis of the structure for acid-activated BPDB indicated that its activation involves cleavage of a labile B←N bond.

关键词： Asymmetric Catalysis Bispyrrolidine Diboronates Diels–Alder Reaction Exo-Selectivity Pericyclic Reaction

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GECAM Localization of High Energy Transients and the Systematic Error

arXiv

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arXiv 2022年

作者： Zhao, Yi Xue, Wang-Chen Xiong, Shao-Lin Wang, Yuan-Hao Liu, Jia-Cong Luo, Qi Zhang, Yan-Qiu Sun, Jian-Chao Zhao, Xiao-Yun Cai, Ce Xiao, Shuo Huang, Yue Li, Xiao-Bo Zhang, Zhen Liao, Jin-Yuan Yang, Sheng Qiao, Rui Guo, Dong-Ya Zheng, Chao Yi, Qi-Bin Xie, Sheng-Lun Guo, Zhi-Wei Li, Chao-Yang Wang, Chen-Wei Tan, Wen-Jun Wang, Yue Peng, Wen-Xi Zheng, Shi-Jie He, Jian-Jian Wang, Ping Wang, Jin Ma, Xiang Song, Xin-Ying Zhang, Hong-Mei Li, Bing Zhang, Peng Wu, Hong Du, Yan-Qi Liang, Jing Zhao, Guo-Ying Li, Xin-Qiao Wen, Xiang-Yang An, Zheng-Hua Sun, Xi-Lei Xu, Yan-Bing Zhang, Fan Zhang, Da-Li Gong, Ke Liu, Ya-Qing Liang, Xiao-Hua Liu, Xiao-Jing Gao, Min Wang, Jin-Zhou Song, Li-Ming Chen, Gang Zhang, Ke-Ke Han, Xing-Bo Wu, Hai-Yan Hu, Tai Geng, Hao Lu, Fang-Jun Zhang, Shu Zhang, Shuang-Nan Lu, Gao-Peng Zeng, Ming Yu, Heng Department of Astronomy Beijing Normal University Beijing100875 China Key Laboratory of Particle Astrophysics Institute of High Energy Physics Chinese Academy of Sciences Beijing100049 China University of Chinese Academy of Sciences Beijing100049 China College of Physics Hebei Normal University 20 South Erhuan Road Hebei Shijiazhuang050024 China Guizhou Provincial Key Laboratory of Radio Astronomy and Data Processing Guizhou Normal University GuiZhou Guiyang550001 China School of Physics and Electronic Science Guizhou Normal University GuiZhou Guiyang550001 China School of Physics and Optoelectronics Xiangtan University Hunan Xiangtan411105 China Institute of Astrophysics Central China Normal University Wuhan430079 China College of Physics Sciences Technology Hebei University No. 180 Wusi Dong Road Lian Chi District Hebei Province Baoding City071002 China Physics and Space Science College China West Normal University Nanchong637002 China College of Electronic and information Engineering Tongji University Shanghai201804 China School of Computing and Artificial Intelligence Southwest Jiaotong University Chengdu611756 China Innovation Academy for Microsatellites Chinese Academy of Sciences Shanghai201304 China National Space Science Center Chinese Academy of Sciences Beijing100190 China School of Earth and Space Sciences University of Science and Technology of China Hefei230026 China Ministry of Education Beijing100084 China Department of Engineering Physics Tsinghua University Beijing100084 China

Gravitational wave high-energy Electromagnetic Counterpart All-sky Monitor (GECAM) is a pair of microsatellites (i.e. GECAM-A and GECAM-B) dedicated to monitoring gamma-ray transients including gravitational waves high-energy electromagnetic counterparts, Gamma-ray Bursts, Soft Gamma-ray Repeaters, Solar Flares and Terrestrial Gamma-ray Flashes. Since launch in December 2020, GECAM-B has detected hundreds of astronomical and terrestrial events. For these bursts, localization is the key for burst identification and classification as well as follow-up observations in multi-wavelength. Here, we propose a Bayesian localization method with Poisson data with Gaussian background profile likelihood to localize GECAM bursts based on the burst counts distribution in detectors with different orientations. We demonstrate that this method can work well for all kinds of bursts, especially for extremely short ones. In addition, we propose a new method to estimate the systematic error of localization based on a confidence level test, which can overcome some problems of the existing method in literature. We validate this method by Monte Carlo simulations, and then apply it to a burst sample with accurate location and find that the mean value of the systematic error of GECAM-B localization is ∼ 2.5◦. By considering this systematic error, we can obtain a reliable localization probability map for GECAM bursts. Our methods can be applied to other gamma-ray monitors. Copyright © 2022, The Authors. All rights reserved.

关键词： Errors

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Erratum: “Influence of heavy metal materials on magnetic properties of Pt/Co/heavy metal tri-layered structures” [Appl. Phys. Lett. 110, 012405 (2017)]

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Applied Physics Letters 2017年第10期110卷

作者： Boyu Zhang Anni Cao Junfeng Qiao Minghong Tang Kaihua Cao Xiaoxuan Zhao Sylvain Eimer Zhizhong Si Na Lei Zhaohao Wang Xiaoyang Lin Zongzhi Zhang Mingzhong Wu Weisheng Zhao 1Fert Beijing Research Institute Beihang University Beijing 100191 China 2Beijing Advanced Innovation Center for Big Data and Brain Computing (BDBC) Beihang University Beijing 100191 China 3School of Electronic and Information Engineering Beihang University Beijing 100191 China 4Key Laboratory of Micro and Nano Photonic Structures (Ministry of Education) Department of Optical Science and Engineering Fudan University Shanghai 200433 China 5Department of Physics Colorado State University Fort Collins Colorado 80523 USA

The following errors appeared in the above article.1

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Fiber-spinning Asymmetric Assembly for Janus-structured Bifunctional Nanofiber Films towards All-Weather Smart Textile

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Angewandte Chemie 2022年第40期134卷

作者： Dr. An-Quan Xie Prof. Liangliang Zhu Yunzheng Liang Jian Mao Prof. Yijiang Liu Prof. Su Chen State Key Laboratory of Materials-Oriented Chemical Engineering and College of Chemical Engineering Nanjing Tech University Nanjing 210009 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Project administration (lead) Writing - original draft (lead) Contribution: Conceptualization (equal) Funding acquisition (lead) Investigation (equal) Resources (lead) Supervision (equal) Writing - review & editing (equal) Contribution: Investigation (supporting) Methodology (supporting) Validation (supporting) Contribution: Data curation (supporting) Investigation (supporting) Methodology (supporting) College of Chemistry Key Laboratory of Environmentally Friendly Chemistry and Application of Ministry of Education Xiangtan University Xiangtan 411105 Hunan Province P. R. China Contribution: Supervision (supporting) Writing - review & editing (supporting)

Given health threat by global warming and increased energy consumption in regulating body temperature, it is an urgent need to construct smart temperature-regulating materials. Herein, a novel fiber-spinning asymmetric chemical assembly (FACA) method is proposed to construct nanofiber materials with asymmetric photothermal properties. The silver nanowires (AgNWs) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) with opposite thermal radiation are assembled on reduced graphene oxide (rGO) film, imparting AgNW/rGO/PVDF-HFP film with Janus structure that can realize the AgNWs side consistently keeps temperature of ca. 11 °C lower than the side of PVDF-HFP nanofiber regardless of the irradiation directions under 1 sun, suggesting the adjustable photothermal regulation. Such photothermally selective hybrid nanofiber film provides great potential as fabrics to achieve all-weather smart clothes, promoting controllable and comprehensive utilization of solar energy.

关键词： Electrospinning Janus Film Passive Cooling Photothermal Management Thermoregulatory Textile

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Tunable Fluorescence from 2D Assemblies of LnW10and P2W18Polyoxometalates Clusters with Quaternary Ammonium-type AIEgens

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Angewandte Chemie 2023年第38期135卷

作者： Dr. Shujian Rong Dr. Mengshi Wang Prof. Dr. Xun Wang Key Lab of Organic Optoelectronics and Molecular Engineering Department of Chemistry Tsinghua University Beijing 100084 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) The Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology (Ministry of Education) Department of Chemistry Tsinghua University Beijing 100084 China Contribution: Data curation (equal) Formal analysis (equal) Methodology (equal) Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Methodology (lead) Project administration (lead) Resources (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Two-dimensional (2D) AIE-inorganic nanocomposites exhibit high stability and high fluorescence activity. However, limited by the types and properties of 2D inorganic materials, it's challenging to realize complex structures and functions. We designed a quaternary ammonium-type AIE ligand, TPECholine. We chose TPECholine and POM clusters as building blocks and synthesized a series of single-layer nanosheets (SLNSs) by assembling LnW 10 or P 2 W 18 POM clusters with TPECholine. By regulating the types of POM clusters and ligands, the morphology and fluorescence intensity of the SLNSs can be finely tuned. Due to the restriction of the intramolecular motions of AIEgens by the SLNSs, nanosheets can exhibit promoted quantum yield (up to 76 %). In addition, thanks to the sub-nanometric sizes and excess surface charges, SLNSs exhibit excellent solvent compatibility, including water, chloroform, ethanol, etc. And the nanosheets showed high fluorescence intensity in these solvents.

关键词： Aggregation-Induced Emission (AIE) Nanosheets Self-Assembly Surface Modification Tunable Fluorescence

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π–π Interaction-Induced Organic Long-wavelength Room-Temperature Phosphorescence forIn VivoAtherosclerotic Plaque Imaging

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Angewandte Chemie 2023年第2期136卷

作者： Yufan Zhang Jisen Li Jiliang Zhao Xuefei Li Zhimei Wang Yicheng Huang Prof. Hongkai Zhang Prof. Qian Liu Prof. Yunxiang Lei Prof. Dan Ding Frontiers Science Center for Cell Responses State Key Laboratory of Medicinal Chemical Biology Key Laboratory of Bioactive Materials Ministry of Education College of Life Sciences Nankai University 300071 Tianjin China Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (lead) Writing - original draft (lead) Contribution: Conceptualization (equal) Data curation (equal) Formal analysis (equal) Contribution: Investigation (equal) Methodology (equal) Contribution: Conceptualization (supporting) Software (equal) School of Chemistry and Materials Engineering Wenzhou University 325035 Wenzhou China Contribution: Investigation (supporting) Methodology (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Department of Urology Tianjin First Central Hospital 300192 Tianjin China Contribution: Data curation (supporting) Software (supporting) Contribution: Visualization (lead) Writing - review & editing (supporting) Contribution: Funding acquisition (lead) Writing - review & editing (lead)

Room-temperature phosphorescent (RTP) materials have great potential for in vivo imaging because they can circumvent the autofluorescence of biological tissues. In this study, a class of organic-doped long-wavelength (≈600 nm) RTP materials with benzo[c][1,2,5] thiadiazole as a guest was constructed. Both host and guest molecules have simple structures and can be directly purchased commercially at a low cost. Owing to the long phosphorescence wavelength of the doping system, it exhibited good tissue penetration (10 mm). Notably, these RTP nanoparticles were successfully used to image atherosclerotic plaques, with a signal-to-background ratio (SBR) of 44.52. This study provides a new approach for constructing inexpensive red organic phosphorescent materials and a new method for imaging cardiovascular diseases using these materials.

关键词： Atherosclerotic Plaque Imaging Benzo[c][1,2,5] Thiadiazole Guest Host-Guest Doped Systems Room Temperature Phosphorescence

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