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Heteroatom Substitution Strategy Modulates Thermodynamics Towards Chemically Recyclable Polyesters and Monomeric Unit Sequence by Temperature Switching

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Angewandte Chemie 2024年第24期136卷

作者： Da Zhang Xin Wang Zhengbiao Zhang Nikos Hadjichristidis State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123 China State Key Laboratory of Radiation Medicine and Protection 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 Note: Prof. Nikos Hadjichristidis is an Honorary Visiting Professor at Soochow University.

In this paper, we proposed a heteroatom substitution strategy (HSS) in the δ -valerolactone (VL) system to modulate thermodynamics toward chemically recyclable polyesters. Three VL-based monomers containing different heteroatoms (M 1 (N), M 2 (S), and M 3 (O)), instead of C-5 carbon, were designed and synthesized to verify our proposed HSS. All three monomers undergo organocatalytic living/controlled ROP and controllable depolymerization. Impressively, the resulting P(M 1 ) achieved over 99 % monomer recovery under both mild solution depolymerization and high vacuum pyrolysis conditions without any side reactions, and the recycled monomers can be polymerized again forming new polymers. The systematic study of the relationship between heteroatom substitution and recyclability shows that introducing heteroatoms does change the thermodynamics of the monomers (Δ H p o , Δ S p o and T c values), thereby adjusting the polymerizability and depolymerizability. DFT calculations found that the introduction of heteroatoms adjusts the ring strain by changing the angular strain of the monomers, and the order of their angular strain (M 2 >M 1 >M 3 ) is consistent with the order of the experimentally obtained enthalpy change. Notably, the one-pot/one-step copolymerization of two of each of the three monomers enables the synthesis of sequence-controlled copolymers from gradient to random to block structures, by simply switching the copolymerization temperature.

关键词： heteroatom ring-opening polymerization chemically recyclable sequence-control polyesters

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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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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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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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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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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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Organocatalytic Lithium Chloride Oxidation by Covalent Organic Frameworks for Rechargeable Lithium-Chlorine Batteries

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Angewandte Chemie 2023年第7期136卷

作者： Dr. Yan Xu Mingming Wang Muhammad Sajid Yahan Meng Zehui Xie Lidong Sun Prof. Jian Jin Prof. Wei Chen Dr. Shenxiang Zhang College of Energy Soochow Institute for Energy and Materials Innovations Light Industry Institute of Electrochemical Power Sources Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province Soochow University Suzhou Jiangsu 215006 China Department of Applied Chemistry School of Chemistry and Materials Science Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China Hefei Anhui 230026 China College of Chemistry Chemical Engineering and Materials Science Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou Jiangsu 215123 China

Rechargeable Li−Cl 2 battery is a promising high energy density battery system. However, reasonable cycle life could only be achieved under low specific capacities due to the sluggish oxidation of LiCl to Cl 2 . Herein, we propose an amine-functionalized covalent organic framework (COF) with catalytic activity, namely COF−NH 2 , that significantly decreases the oxidation barrier of LiCl and accelerates the oxidation kinetics of LiCl in Li−Cl 2 cell. The resulting Li−Cl 2 cell using COF−NH 2 (Li−Cl 2 @COF−NH 2 ) simultaneously exhibits low overpotential, ultrahigh discharge capacity up to 3500 mAh/g and a promoted utilization ratio of deposited LiCl at the first cycle (UR−LiCl) of 81.4 %, which is one of the highest reported values to date. Furthermore, the Li−Cl 2 @COF−NH 2 cell could be stably cycled for over 200 cycles when operating at a capacity of 2000 mAh/g at −20 °C with a Coulombic efficiency (CE) of ≈100 % and a discharge plateau of 3.5 V. Our superior Li−Cl 2 batteries enabled by organocatalyst enlighten an arena towards high-energy storage applications.

关键词： Covalent Organic Framework High Energy Density Lithium Chloride Oxidation Lithium-Chlorine Battery Organocatalysis

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Be2C5 Monolayer with Quasiplanar Pentacoordinate Carbon Atoms and Ultrahigh Energy Density as a Dirac Anode for Potassium-Ion Batteries

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PRX Energy 2023年第3期2卷 033012-033012页

作者： Feilong Wang Meiling Xu Shuyi Lin Jian Hao Yanchao Wang Hong Jian Zhao Yinwei Li Laboratory of Quantum Functional Materials Design and Application School of Physics and Electronic Engineering Jiangsu Normal University Xuzhou 221116 China International Center for Computational Method and Software State Key Laboratory of Superhard Materials Key Laboratory of Physics and Technology for Advanced Batteries Ministry of Education College of Physics Jilin University Changchun 130012 China

K-ion batteries (KIBs) are of potential importance in the future energy industries. Recent efforts were committed to increasing the energy storage density in KIBs. Here, we search for anode materials with high energy density that are compatible with KIBs, by a combination of the swarm-intelligence structure search method and first-principles calculations. We predict the Be2C5 monolayer to be a kind of material that showcases ultrahigh energy density (∼5455 mWh/g, referenced to the standard hydrogen electrode potential), thanks to an exceptional specific capacity of 2060 mAh/g and low average open-circuit voltage of 0.28 V. This energy density value is much larger than that of most currently known 2D KIB-based anode materials. Furthermore, the Be2C5 anode presents other intriguing behavior, such as (i) the fast diffusion of K ions, as suggested by an ultralow barrier energy of about 0.074 eV; (ii) excellent mechanical strength, with a Young’s modulus of about 243 N/m; (iii) robust compatibility with electrolytes; (iv) small-scale volume expansion of 0.68% during the process of potassiation; and (v) a unique “self-doping” effect, which is beneficial for high electronic conductivity.

关键词： Lithium-alternative batteries 2-dimensional systems First-principles calculations

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A Chiral COFs Membrane for Enantioselective Amino Acid Separation

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Angewandte Chemie 2024年第5期137卷

作者： Narmadha Manoranjan Wangxi Fang Yuzhang Zhu Prof. Dr. Jian Jin i-Lab Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Suzhou 215123 P.R. China College of Chemistry Chemical Engineering and Materials Science Jiangsu Key Laboratory of Advanced Functional Polymer Materials & Suzhou key Laboratory of Macromolecular Design and Precision Synthesis Soochow University Suzhou 215123 P.R. China

Incorporating chiral molecules in the covalent organic frameworks (COFs) with uniformly ordered pores results in chiral COFs, which have been highly promising candidates for enantioseparation. Herein, a homochiral COF nanochannel membrane is reported by introducing chiral centers (L-phenylalanine methyl ester) into one of the organic ligands for the enantioseparation of chiral amino acids. The separation results show that the D-isomer is preferentially transported through the porous membrane channel. This composite membrane exhibits excellent selectivity for racemic phenylalanine with the highest enantiomeric excess value of up to 99.4 %. The adsorption and molecular modeling studies substantiate the experiment results by showing higher bonding affinity towards D-isomer over L-isomer. The excellent enantioselective gating performance unveils the porous COF skeleton with chiral selectors and the size-matching synergy for stereoselective interactions with chiral isomers.

关键词： chiral separation composite membrane covalent organic framework homochiral membrane membrane chromatography

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