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functional Ionic Liquid Polymer Stabilizer for High-Performance Perovskite Photovoltaics

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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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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Corrigendum to “The second network of soft-nanoparticles in linear polymers of the same chemistry” [Polymer 283 (2023) 126216]

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Polymer 2023年 285卷

作者： Xikai Ouyang Jintian Luo Tao Li Yihui Zhu Wancheng Yu Jinlin He Pengfei Zhang GengXin Liu State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Center for Advanced Low-dimension Materials College of Material Science and Engineering Donghua University Shanghai 201620 China School of Chemistry and Chemical Engineering Key Laboratory of Surface & Interface Science of Polymer Materials of Zhejiang Province Zhejiang Sci-Tech University Hangzhou 310018 China State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Soochow University Suzhou 215123 China College of Chemistry Chemical Engineering and Materials Science Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application Suzhou Key Laboratory of Macromolecular Design and Precision Synthesis Soochow University Suzhou Jiangsu 215123 China National Synchrotron Radiation Laboratory Anhui Provincial Engineering Laboratory of Advanced Functional Polymer Film CAS Key Laboratory of Soft Matter Chemistry University of Science and Technology of China Hefei 230026 China

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Nano-sheet stacked flower-like MoO₂ with synergistic adsorption-catalysis for wide-temperature lithium-sulfur batteries

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Electrochimica Acta 2025年 535卷

作者： Cheng-Wei Zhu Hai Huang Jin Wei Yan Yu-Han Yuan Ye Zeng Gui-Fang Li Jian-Chun Weng Xiao-Hong Fan Yi Li Qi-Hui Wu Ding-Rong Deng Jimei University College of Marine Equipment and Mechanical Engineering Key Laboratory of Energy Cleaning Utilization Development Cleaning Combustion and Energy Utilization Research Center of Fujian Province Xiamen Key Laboratory of Marine Corrosion and Smart Protective Materials Xiamen Fujian 361021 China Jiangsu Key Lab 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

Li-S batteries have been regarded as future energy storage solutions due to their high theoretical energy density and eco-friendliness. However, practical uses face obstacles such as the polysulfide shuttle effect and slow reaction rates at extreme temperatures. In this research, dendritic assembly MoO₂ nanosheets (DA-MoO₂) with flower-like structures were produced through a two-step solvothermal method and assessed as sulfur host materials for Li-S batteries. The hierarchical structure of DA-MoO₂ resulted in a large specific surface area (216.92 m² g -1 ) and numerous mesopores (3–4 nm), significantly enhancing polysulfide adsorption capability to mitigate the shuttle effect. This architectural design successfully reduces irreversible capacity loss due to intense shuttle effect at high temperatures while enhancing sulfur usage. Moreover, the plentiful catalytic active sites in DA-MoO₂ enhance slow redox reaction kinetics at low temperatures, allowing Li-S batteries to perform well across a wide temperature range. According to electrochemical evaluations, DA-MoO₂ maintains excellent functionality in severe environments: After 100 cycles, it holds a capacity of 542 mAh g⁻¹ at –20 °C and a 1C rate, and it could potentially perform well at -40 °C. At room temperature (2C), the capacity decreases by only 0.06 % per cycle across 300 cycles. Interestingly, the electrode maintains a steady capacity of 1161.05 mAh g⁻¹ at 60 °C and 2C rate, with a low decay rate of 0.019 % per cycle. These outcomes provide a feasible approach for wide-temperature-range energy storage applications, greatly outperforming the performance of traditional Super P and pure MoO₂ electrodes. DA-MoO₂ is positioned as a promising contender for enhanced Li-S battery systems operating under challenging environmental circumstances due to the synergistic integration of structural benefits and catalytic performance.

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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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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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Iodonium Initiators: Paving the Air-free Oxidation of Spiro-OMeTAD for Efficient and Stable Perovskite Solar Cells

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Angewandte Chemie 2023年第5期136卷

作者： Heyi Yang Tingting Xu Weijie Chen Yeyong Wu Xianming Guo Yunxiu Shen Chengqiang Ding Xining Chen Haiyang Chen Junyuan Ding Xiaoxiao Wu Prof. Guixiang Zeng Prof. Zhengbiao Zhang 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 School of Chemistry and Chemical Engineering Nanjing University Nanjing 210008 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 Kuang Yaming Honors School Nanjing University Nanjing 210008 China State Key Laboratory of Radiation Medicine and Protection 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

To date, perovskite solar cells (pero-SCs) with doped 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9,9′-spirobifluorene (Spiro-OMeTAD) hole transporting layers (HTLs) have shown the highest recorded power conversion efficiencies (PCEs). However, their commercialization is still impeded by poor device stability owing to the hygroscopic lithium bis(trifluoromethanesulfonyl)imide and volatile 4-tert-butylpyridine dopants as well as time-consuming oxidation in air. In this study, we explored a series of single-component iodonium initiators with strong oxidability and different electron delocalization properties to precisely manipulate the oxidation states of Spiro-OMeTAD without air assistance, and the oxidation mechanism was clearly understood. Iodine (III) in the diphenyliodonium cation (IP + ) can accept a single electron from Spiro-OMeTAD and forms Spiro-OMeTAD⋅ + owing to its strong oxidability. Moreover, because of the coordination of the strongly delocalized TFSI − with Spiro-OMeTAD⋅ + in a stable radical complex, the resulting hole mobility was 30 times higher than that of pristine Spiro-OMeTAD. In addition, the IP-TFSI initiator facilitated the growth of a homogeneous and pinhole-free Spiro-OMeTAD film. The pero-SCs based on this oxidizing HTL showed excellent efficiencies of 25.16 % (certified: 24.85 % for 0.062-cm 2 ) and 20.71 % for a 15.03-cm 2 module as well as remarkable overall stability.

关键词： Doping Perovskite Solar Cells Spiro-OMeTAD Stability

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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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Transfer, Amplification, Storage, and Complete Self-Recovery of Supramolecular Chirality in an Achiral Polymer System

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Angewandte Chemie 2021年第34期133卷

作者： Tengfei Miao Xiaoxiao Cheng Haotian Ma Zixiang He Prof. Zhengbiao Zhang Prof. Nianchen Zhou Prof. Wei Zhang Prof. Xiulin Zhu 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

Supramolecular chirality and its complete self-recovery ability are highly mystical in nature and biological systems, which remains a major challenge today. Herein, we demonstrate that partially cross-linked azobenzene (Azo) units can be employed as the potential chiral trigger to fully heal the destroyed helical superstructure in achiral nematic polymer system. Combining the self-assembly of Azo units and terminal hydroxyl groups in polymer side chains allows the vapor-induced chiral nematic phase and covalent fixation of the superstructure via acetal reaction. The induced helical structure of Azo units can be stored by inter-chain cross-linking, even after removal of the chiral source. Most interestingly, the stored chiral information can trigger perfect chiral self-recovery (CSR) behavior after being destroyed by UV light, heat, and solvents. The results pave a new way for producing novel chiroptical materials with reversible chirality from achiral sources.

关键词： chiral induction chiral self-recovery chiral storage supramolecular chirality

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Molecular Self-Assembly Regulated Dopant-Free Hole Transport Materials for Efficient and Stablen-i-pPerovskite Solar Cells and Scalable Modules

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Angewandte Chemie 2022年第42期134卷

作者： Qinrong Cheng Haiyang Chen Fu Yang Ziyuan Chen Weijie Chen Heyi Yang Yunxiu Shen Xue-Mei Ou 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 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

Dopant-free organic hole transport materials (HTMs) remain highly desirable for stable and efficient n - i - p perovskite solar cells (pero-SCs) but rarely succeed. Here, we propose a molecular assembly strategy to overcome the limited optoelectronic properties of organic HTMs by precisely designing a linear organic small molecule BDT-DPA-F from the atomic to the molecular levels. BDT-DPA-F can assemble into a fibril network, showing an obviously improved hole mobility and decreased energy disorder. The resultant pero-SCs showed a promising efficiency of 23.12 % (certified 22.48 %), which is the highest certified value of pero-SCs with dopant-free HTMs, to date. These devices also showed a weak-dependence of efficiency on size, enabling a state-of-the-art efficiency of 22.50 % for 1-cm 2 device and 20.17 % for 15.64-cm 2 module. For the first time, the pero-SCs based on dopant-free HTMs realized ultralong stabilities with T 80 lifetimes over 1200 h under operation or thermal aging at 85 °C.

关键词： Dopant-Free Hole Transport Materials Intermolecular Interactions Operational and Thermal Stabilities Perovskite Solar Cells Self-Assembly

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