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A General and Mild Two-Step Strategy Using Bioderived Diols and CO2for Chemically Recyclable Polycarbonates and Closed-Loop CO2Fixation

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Angewandte Chemie 2025年

作者： Jiaming Tian Nikos Hadjichristidis Xin Wang Zhengbiao Zhang State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Materials Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Polymer Synthesis Laboratory KAUST Catalysis Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology (KAUST) Thuwal 23955 Saudi Arabia State Key Laboratory of Radiation Medicine and Protection Soochow University Suzhou 215123 China

Developing chemically recyclable polymers using CO 2 and sustainable co-feedstocks is an important strategy for achieving carbon-neutral production of new polymers and mitigating plastic pollution. Herein, a series of six-membered cyclic carbonate monomers with different alkyl α -substituents were synthesized using CO 2 and bioderived 1,3-alkanediol as raw materials at room temperature and atmospheric pressure. The organocatalytic ring-opening polymerization was systematically studied using a range of common and readily available organocatalysts. Phosphazene base ( t -BuP 2 ) was identified as the most effective catalyst, offering excellent control over the entire polymerization. The regioselectivity of the synthesized polycarbonates, ranged from 0.74 to 0.99, with the highest value achieved when the side group was isopropyl (highest steric hindrance). Notably, the α -substituent in the monomers reduced the ring strains, allowing the resulting polycarbonates to be fully recycled to the monomers without decarboxylation. The recycling process effectively traps CO 2 in a closed loop between monomers and polymers, preventing its release into the atmosphere. The alkyl side groups enhanced the hydrophobicity of the polycarbonates, thereby reducing the likelihood of CO 2 release through hydrolysis during their lifecycle, achieving a robust CO 2 closed-loop fixation. The utility of CO 2 -based aliphatic polycarbonates as adhesives and the ability of copolymerization with l -lactide were explored.

关键词： Adhesives Chemically recyclable polycarbonates CO2 closed-loop fixation Ring-opening polymerization

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Intrinsic and extrinsic anomalous transport properties in noncollinear antiferromagnetic Mn3Sn from first-principle calculations

arXiv

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arXiv 2023年

作者： Yang, Xiuxian Feng, Wanxiang Zhou, Xiaodong Mokrousov, Yuriy Yao, Yugui Beijing Key Lab of Nanophotonics & Ultrafine Optoelectronic Systems School of Physics Beijing Institute of Technology Beijing100081 China School of Physics Jiangsu Normal University Xuzhou221116 China Laboratory of Quantum Functional Materials Design and Application School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou221116 China Institute of Physics Johannes Gutenberg University Mainz Mainz55099 Germany Peter Grünberg Institut Institute for Advanced Simulation Forschungszentrum Jülich and JARA Jülich52425 Germany

Mn3Sn has garnered significant attention due to its kagome lattice, 120◦ noncollinear antiferromagnetic order, and substantial anomalous Hall effect. In this study, we comprehensively explore intrinsic and extrinsic contributions to anomalous Hall, anomalous Nernst, and anomalous thermal Hall effects, employing first-principle calculations and group theory analysis. Comparative analysis between our theoretical results and available experimental data underscores the predominance of intrinsic mechanism in shaping anomalous transport properties at low temperatures. Specifically, Weyl fermions are identified as the primary contributors to intrinsic anomalous Hall conductivity. The significance of extrinsic mechanisms becomes evident at high temperatures, especially when the longitudinal charge conductivity falls into the dirty regime, where the side jump mechanism plays a vital role. Extrinsic contributions to anomalous transport properties are primarily influenced by the electronic states residing at the Fermi surfaces. Furthermore, anomalous transport properties exhibit periodic variations when subjected to spin rotations within the kagome plane, achievable by applying an external magnetic field. Our findings advance the understanding of anomalous transport phenomena in Mn3Sn and offer insights into potential applications of noncollinear antiferromagnetic materials in spintronics and spin caloritronics. Copyright © 2023, The Authors. All rights reserved.

关键词： Tin alloys

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Synthesis of ultrathin semicircle-shaped copper nanowires in ethanol solution for low haze flexible transparent conductors

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Nano Research 2018年第7期11卷 3899-3910页

作者： Ye Zhan~ Jiangna Guo Dan Xu Yi Sun Feng Yan Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and EngineeringCollege of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China

Copper nanowires （CuNWs） are becoming an indispensable item for next- generation transparent optical devices due to their excellent conductivity and transparency. In this work, ultrathin semicircle-shaped copper nanowires （SCuNWs） with a diameter of - 15 nm and a length of - 30 μm （aspect ratio of -2,000） were synthesized in ethanol solution. The mechanism and factors that affect the morphology and dispersity of the SCuNWs were investigated. The prepared SCuNWs were coated on polyethylene terephthalate （PET） or polyd- imethylsiloxane （PDMS） substrate to fabricate flexible transparent conductors （FTCs）. The fabricated FTCs exhibited excellent optoelectrical performance and low haze. In addition, the fabricated FTCs showed high mechanical stability during stretching and bending, indicating their great potential in flexible optical devices.

关键词： copper nanowires semicircle-shaped ultrathin low haze flexible transparent conductors

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The Highly Effective Therapy of Ovarian Cancer by Bi-Doped Oxygen-Deficient Batio3 with Enhanced Sono-Piezocatalytic Effects

SSRN

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SSRN 2022年

作者： Wang, Hongbo Cheng, Shuangshuang Luo, Yue Zhang, Jun Shi, Rui Wei, Sitian Dong, Kejun Liu, Xiangmei Wu, Shuilin Department of Obstetrics and Gynecology Union Hospital Tongji Medical College Huazhong University of Science and Technology Wuhan430022 China Biomedical Materials Engineering Research Center Collaborative Innovation Center for Advanced Organic Chemical Materials Co-constructed by The Province and Ministry Hubei Key Laboratory of Polymer Materials Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials School of Materials Science & Engineering Hubei University Wuhan430062 China School of Materials Science & Engineering Peking University Beijing100871 China

Ovarian cancer (OC) is the leading cause of death of gynecological malignancy. Sonodynamic therapy (SDT) with high penetration ability and biosafety is considered as a minimally invasive method for the elimination of deep tumor. However, sonosensitizers with high efficiency are still urgently needed. Here, we developed an oxygen defect-rich piezoelectric nanocomposite barium titanate nanocubes with bismuth dope for enhanced sonodynamic ovarian cancer therapy. The oxygen defect engineering decreases the band gap, and Schottky junction modified by Bi nanoparticles effectively enhance the transfer and separation of charge carriers and inhibited the recombination under US irradiation, leading to product more reactive oxygen species (ROS), which significantly enhance the SDT efficiency. The in vitro results demonstrated that Bi doped oxygen-deficient BaTO 3 significantly promote the apoptosis of tumor cells because of the high ROS generation efficiency. RNA sequencing further proved that antitumor activity may be through extracellular matrix disassembly pathway. At last, the in vivo results showed that Bi doped oxygen-deficient BaTO 3 can significantly eliminate ovarian cancer through SDT. This work proposed an oxygen defect-rich piezoelectric nanocomposite as a new kind of sonosensitizer with high SDT efficiency for enhanced sonodynamic ovarian cancer therapy. © 2022, The Authors. All rights reserved.

关键词： Tumors

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Program-Modulated Kinetics of Perovskite-Film Growth by Molecular “Thruster” for High-Efficiency and Stable Perovskite Solar Cells

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Angewandte Chemie 2024年第7期137卷

作者： Chuanshuai Han Yeyong Wu Prof. Guiying Xu Xiaoxiao Wu Jiacheng Xu Tingting Xu Shihao Huang Yunxiu Shen Zhiyun Cao Weijie Chen Prof. Xiaoping Xu Prof. Yaowen Li Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Laboratory of Organic Synthesis of Jiangsu Province College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Innovation Center of Chemical Science Soochow University Suzhou 215123 China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Suzhou 215123 China

The rapid reaction between lead iodide (PbI 2 ) and formamidinium iodide (FAI) complicates the fabrication of high-quality formamidinium lead iodide (FAPbI 3 ) films. Conventional methods, such as using nonvolatile small molecular additives to slow the reaction, often result in buried interfacial voids and molecule diffusion, compromising the devices’ operational stability. In this study, we introduced a molecular “thruster”—a hypervalent iodine (III) compound with three carbonyl groups and a C − −I + bond—that possesses coordination and dissociation abilities, enabling programed modulation of perovskite-film growth kinetics. Initially, the three carbonyl groups coordinate with PbI 2 to slow the reaction between FAI and PbI 2 , preventing δ-phase formation. As temperature rises, the C − −I + bond dissociates, promoting perovskite growth and the dissociated product iodobenzene will promote solvent volatilization, thus avoiding buried interfacial voids. Another product, a carbene compound with eight lone pair electrons sufficiently passivate the undercoordinated Pb 2+ defects and anchors at grain boundaries without diffusion. Consequently, the resultant FAPbI 3 film displays high-quality with enhanced phase purity, compact morphology, and reduced defects. Evidently, 0.062- and 1.004-cm 2 pero-SCs achieve power conversion efficiencies (PCEs) of up to 26.06 % (25.79 % certified) and 24.65 %, respectively. This approach also controls perovskite-film growth on plastic substrates, resulting in flexible pero-SCs with an impressive PCE of 25.12 %.

关键词： perovskite solar cells phase purity FAPbI3 thermally-induced homolytic-bond cleavage reaction stable

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Thermally Responsive Selenide-containing Materials Based on Transalkylation of Selenonium Salts

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Angewandte Chemie 2023年第49期135卷

作者： Sisi Chen Vincent Scholiers Mengyao Zhang Jiandong Zhang Prof. Dr. Jian Zhu Prof. Dr. Filip E. Du Prez Prof. Dr. Xiangqiang Pan State and Local Joint Engineering Laboratory for Novel Functional Department Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Department of Polymer Science and Engineering College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Polymer Chemistry Research group Centre of Macromolecular Chemistry (CMaC) Department of Organic and Macromolecular Chemistry Faculty of Sciences Ghent University Krijgslaan 281 S4-bis 9000 Ghent Belgium

Covalent adaptable networks (CANs) possess unique properties as a result of their internal dynamic bonds, such as self-healing and reprocessing abilities. In this study, we report a thermally responsive C−Se dynamic covalent chemistry (DCC) that relies on the transalkylation exchange between selenonium salts and selenides, which undergo a fast transalkylation reaction in the absence of any catalyst. Additionally, we demonstrate the presence of a dissociative mechanism in the absence of selenide groups. After incorporation of this DCC into selenide-containing polymer materials, it was observed that the cross-linked networks display varying dynamic exchange rates when using different alkylation reagents, suggesting that the reprocessing capacity of selenide-containing materials can be regulated. Also, by incorporating selenonium salts into polymer materials, we observed that the materials exhibited good healing ability at elevated temperatures as well as excellent solvent resistance at ambient temperature. This novel dynamic covalent chemistry thus provides a straightforward method for the healing and reprocessing of selenide-containing materials.

关键词： Covalent Adaptable Networks Dynamic Covalent Chemistry Selenide Selenonium Salts Transalkylation

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Crystal Thermal Transport in Altermagnetic RuO2

arXiv

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arXiv 2023年

作者： Zhou, Xiaodong Feng, Wanxiang Zhang, Run-Wu Šmejkal, Libor Sinova, Jairo Mokrousov, Yuriy Yao, Yugui Centre for Quantum Physics Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement MOE School of Physics Beijing Institute of Technology Beijing100081 China Beijing Key Lab of Nanophotonics and Ultrafine Optoelectronic Systems School of Physics Beijing Institute of Technology Beijing100081 China Laboratory of Quantum Functional Materials Design and Application School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou221116 China Institute of Physics Johannes Gutenberg University Mainz Mainz55099 Germany Institute of Physics Czech Academy of Sciences Cukrovarnická 10 Praha 6162 00 Czech Republic Peter Grünberg Institut Institute for Advanced Simulation Forschungszentrum Jülich and JARA Jülich52425 Germany

We demonstrate the emergence of a pronounced thermal transport in the recently discovered class of magnetic materials − altermagents. From symmetry arguments and first principles calculations performed for the showcase altermagnet, RuO2, we uncover that crystal Nernst and crystal thermal Hall effects in this material are very large and strongly anisotropic with respect to the Néel vector. We find the large crystal thermal transport to originate from three sources of Berry’s curvature in momentum space: the Weyl fermions due to crossings between well-separated bands, the strong spin-flip pseudo-nodal surfaces, and the weak spin-flip ladder transitions, defined by transitions among very weakly spin-split states of similar dispersion crossing the Fermi surface. Moreover, we reveal that the anomalous thermal and electrical transport coefficients in RuO2 are linked by an extended Wiedemann-Franz law in a temperature range much wider than expected for conventional magnets. Our results suggest that altermagnets may assume a leading role in realizing concepts in spincaloritronics not achievable with ferromagnets or antiferromagnets. Copyright © 2023, The Authors. All rights reserved.

关键词： Ruthenium compounds

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Green Solvent Processable, Asymmetric Dopant-Free Hole Transport Layer Material for Efficient and Stablen-i-pPerovskite Solar Cells and Modules

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Angewandte Chemie 2023年第46期135卷

作者： Qinrong Cheng Haiyang Chen Weijie Chen Junyuan Ding Ziyuan Chen Yunxiu Shen Xiaoxiao Wu Yeyong Wu Prof. Yaowen Li Prof. Yongfang Li Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

The use of dopant-free hole transport layers (HTLs) is critical in stabilizing n-i-p perovskite solar cells (pero-SCs). However, these HTL materials are often processed with toxic solvents, which is not ideal for industrial production. Upon substituting them with green solvents, a trade-off emerges between maintaining the high crystallinity of the HTL materials and ensuring high solubility in the new solvents. In this paper, we designed a novel, linear, organic small molecule, BDT-C8-3O, by introducing an asymmetric polar oligo(ethylene glycol) side chain. This method not only overcomes the solubility limitations in green solvents but also enables stacking the conjugated main chains in two patterns, which further enhances crystallinity and hole mobility. As a result, the n - i - p pero-SCs based on chlorobenzene- or green (natural compound) solvent 3-methylcyclohexanone-processed BDT-C8-3O HTL that without any dopant delivered world-recorded power conversion efficiencies of 24.11 % (certified of 23.82 %) and 23.53 %, respectively. The devices also demonstrated remarkable operational and high-temperature stabilities, maintaining over 84 % and 79.5 % of their initial efficiency for 2000 h, respectively. Encouragingly, dopant-free BDT-C8-3O HTL exhibits significant advantages in large-area fabrication, achieving state-of-the-art PCEs exceeding 20 % for 5×5 cm 2 modules (active area: 15.64 cm 2 ), even when processed using green solvents.

关键词： Asymmetric Molecule Dopant-Free Green Solvent Hole Transport Layer Materials Perovskite Solar Cells

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functional Ionic Liquid polymer Stabilizer for High-Performance Perovskite Photovoltaics

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Angewandte Chemie 2023年第16期135卷

作者： Yunxiu Shen Guiying Xu Jiajia Li Xia Lin Fu Yang Heyi Yang Weijie Chen Yeyong Wu Xiaoxiao Wu Qinrong Cheng Prof. Jian Zhu Prof. Yaowen Li Prof. Yongfang Li Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123 China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

The stability-related issues arising from the perovskite precursor inks, films, device structures and interdependence remain severely under-explored to date. Herein, we designed an ionic-liquid polymer (poly[Se-MI][BF 4 ]), containing functional moieties like carbonyl (C=O), selenium (Se + ), and tetrafluoroborate (BF 4 − ) ions, to stabilize the whole device fabrication process. The C=O and Se + can coordinate with lead and iodine (I − ) ions to stabilize lead polyhalide colloids and the compositions of the perovskite precursor inks for over two months. The Se + anchored on grain boundaries and the defects passivated by BF 4 − efficiently suppress the dissociation and migration of I − in perovskite films. Benefiting from the synergistic effects of poly[Se-MI][BF 4 ], high efficiencies of 25.10 % and 20.85 % were exhibited by a 0.062-cm 2 device and 15.39-cm 2 module, respectively. The devices retained over 90 % of their initial efficiency under operation for 2200 h.

关键词： Ionic Liquid Perovskite polymer Precursor Ink Solar Cells

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A facile fabrication of novel stuff with antibacterial property and osteogenic promotion utilizing red phosphorus and near-infrared light

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Bioactive Materials 2019年第1期4卷 17-21页

作者： Bo Huang Lei Tan Xiangmei Liu Jun Li Shuilin Wu Ministry-of-Education Key Laboratory for the Green Preparation and Application of Functional Materials Hubei Key Laboratory of Polymer MaterialsSchool of Materials Science&EngineeringHubei UniversityWuhan430062China School of Materials Science&Engineering The Key Laboratory of Advanced Ceramics and Machining Technology by the Ministry of Education of ChinaTianjin UniversityTianjin300072China

Bone-implant materials are important for bone repairing and orthopedics surgery,which include bone plates and bone *** materials need to be designed not only considering its biostability and biocompatibility,but also their by-products induced infection after therapy or long-time treatment in ***,the development of novel implant materials is quite *** phosphorus has great biocompatibility and exhibits efficient photothermal ***,a red phosphorus/IR780/arginine-glycine-asparticacid-cysteine(RGDC)coating on titanium bone-implant was *** temperature sensitivity of Staphylococcus aureus biofilm is enhanced in the presence of ROS produced by IR780 with 808 nm light *** keeping the cells and tissues normal,a high antibacterial performance can be realized by near-infrared(808 nm)irradiated within 10 min at 50℃.Besides the high effective antibacterial efficacy provided by photothermal therapy(PTT)and photodynamic therapy(PDT),the RGDC decorated surface can also possess an excellent performance in osteogenesis in vivo.

关键词： Implants Red phosphorus Near-infrared Osteogenesis Antibacterial Biofilm

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