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Chemistry of Inorganic materials 2024年 3卷

作者： Yue Ming Youwei Jiang Jinghao Li Jie Huang Peng Xiang Cheng Qiu Yaoguang Rong Electronic and Communication Engineering Shenzhen Polytechnic University Shenzhen 518055 Guangdong PR China School of Chemistry Chemical Engineering and Life Sciences State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei PR China International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 Hubei PR China School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 Hubei PR China Solar Energy High Value Utilization and Green Conversion Hubei Provincial Engineering Research Center College of Electrical Engineering & New Energy China Three Gorges University Yichang 443002 Hubei PR China Hebei Provincial Collaborative Innovation Center of Transportation Power Grid Intelligent Integration Technology and Equipment School of Electrical and Electronic Engineering Shijiazhuang Tiedao University 050043 Shijiazhuang PR China

In recent years, there has been notable progress in the development of perovskite solar cells (PSCs), marked by significant advancements in efficiency, stability, and scalability. Among different device architectures and technical routes, mesoporous perovskite solar cells (MPSCs) based on TiO 2 /ZrO 2 /carbon scaffold and screen-printing fabrication process have shown unique advantages for mass production and commercialization due to the low material cost and scalable fabrication process. Through efforts on material optimization, interface engineering, and device design, the power conversion efficiency of MPSCs has steadily increased from the initial 6.64 % in 2013 to current 22.22 %. Attributing to the screen-printing-based fabrication process, printable mesoscopic PSCs have enabled large-area devices, from mini-modules to modules, and solar panels. In this review, we discuss the development and latest advances of MPSCs, and provide outlooks for further improving the performance of this promising photovoltaic technology.

关键词： Mesoporous perovskite solar cells Printable Mesoscopic structure Stability Upscaling

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Rapid Charge Transfer Endowed by Interfacial Ni-O Bonding in S-scheme Heterojunction for Efficient Photocatalytic H2and Imine Production

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Angewandte Chemie 2023年第50期135卷

作者： Dr. Bowen He Dr. Peng Xiao Dr. Sijie Wan Dr. Jianjun Zhang Prof. Tao Chen Prof. Liuyang Zhang Prof. Jiaguo Yu Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences 68 Jincheng Street Wuhan 430078 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Methodology (lead) Writing - original draft (equal) Hefei National Laboratory for Physical Sciences at Microscale CAS Key Laboratory of Materials for Energy Conversion Department of Materials Science and Engineering University of Science and Technology of China Hefei Anhui 230026 China Contribution: Data curation (equal) Formal analysis (equal) State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China Contribution: Formal analysis (supporting) Methodology (supporting) Software (lead) Contribution: Methodology (supporting) Validation (supporting) Contribution: Methodology (supporting) Resources (supporting) Contribution: Formal analysis (equal) Funding acquisition (equal) Supervision (supporting) Writing - review & editing (lead)

Cooperative coupling of H 2 evolution with oxidative organic synthesis is promising in avoiding the use of sacrificial agents and producing hydrogen energy with value-added chemicals simultaneously. Nonetheless, the photocatalytic activity is obstructed by sluggish electron-hole separation and limited redox potentials. Herein, Ni-doped Zn 0.2 Cd 0.8 S quantum dots are chosen after screening by DFT simulation to couple with TiO 2 microspheres, forming a step-scheme heterojunction. The Ni-doped configuration tunes the highly active S site for augmented H 2 evolution, and the interfacial Ni−O bonds provide fast channels at the atomic level to lower the energy barrier for charge transfer. Also, DFT calculations reveal an enhanced built-in electric field in the heterojunction for superior charge migration and separation. Kinetic analysis by femtosecond transient absorption spectra demonstrates that expedited charge migration with electrons first transfer to Ni 2+ and then to S sites. Therefore, the designed catalyst delivers drastically elevated H 2 yield (4.55 mmol g −1 h −1 ) and N-benzylidenebenzylamine production rate (3.35 mmol g −1 h −1 ). This work provides atomic-scale insights into the coordinated modulation of active sites and built-in electric fields in step-scheme heterojunction for ameliorative photocatalytic performance.

关键词： Benzylamine Coupling Oxidation Hydrogen Production Interfacial Charge Transfer S-Scheme Photocatalyst

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Lithium/Sodium-Ion Batteries: In Situ, Atomic-Resolution Observation of Lithiation and Sodiation of WS2Nanoflakes: Implications for Lithium-Ion and Sodium-Ion Batteries (Small 24/2021)

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Small 2021年第24期17卷

作者： Yaobin Xu Ke Wang Zhenpeng Yao Joohoon Kang David Lam Dan Yang Wei Ai Chris Wolverton Mark C. Hersam Ying Huang Wei Huang Vinayak P. Dravid Jinsong Wu Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA NUANCE Center Northwestern University Evanston IL 60208 USA Frontiers Science Center for Flexible Electronics (FSCFE) Institute of Flexible Electronics (IFE) Northwestern Polytechnical University (NPU) 127 West Youyi Road Xi'an 710072 China Department of Chemistry and Chemical Biology Harvard University 12 Oxford Street Cambridge MA 02138 USA Department of Chemistry and Computer Science University of Toronto Toronto Ontario Canada School of Advanced Materials Science and Engineering Sungkyunkwan University (SKKU) Suwon 16419 Republic of Korea MOE Key Laboratory of Material Physics and Chemistry Under Extraordinary Conditions School of Chemistry and Chemical Engineering Northwestern Polytechnical University Xi'an 710072 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research Centre Wuhan University of Technology 122 Luoshi Road Wuhan Hubei 430070 China

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Ethylenedioxythiophene-Based Small Molecular Donor with Multiple Conformation Locks for Organic Solar Cells with Efficiency of 19.3 %

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Angewandte Chemie 2024年第25期136卷

作者： Dr. Qian Xie Xiangmeng Deng Prof. Chaowei Zhao Dr. Jie Fang Dr. Dongdong Xia Yuefeng Zhang Feng Ding Jiali Wang Mengdi Li Zhou Zhang Dr. Chengyi Xiao Prof. Xunfan Liao Prof. Lang Jiang Dr. Bin Huang Dr. Runying Dai Prof. Weiwei Li Institute of Applied Chemistry Jiangxi Academy of Sciences Nanchang 330096 P. R. China Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry School of Chemistry and Chemical Engineering Jiangxi University of Science and Technology Ganzhou 341000 P. R. China National Engineering Research Center for Carbohydrate Synthesis/Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education Jiangxi Normal University Nanchang 330022 P. R. China Beijing Advanced Innovation Center for Soft Matter Science and Engineering & State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 P. R. China Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 China

Ternary organic solar cells (T-OSCs) represent an efficient strategy for enhancing the performance of OSCs. Presently, the majority of high-performance T-OSCs incorporates well-established Y-acceptors or donor polymers as the third component. In this study, a novel class of conjugated small molecules has been introduced as the third component, demonstrating exceptional photovoltaic performance in T-OSCs. This innovative molecule comprises ethylenedioxythiophene (EDOT) bridge and 3-ethylrhodanine as the end group, with the EDOT unit facilitating the creation of multiple conformation locks. Consequently, the EDOT-based molecule exhibits two-dimensional charge transport, distinguishing it from the thiophene-bridged small molecule, which displays fewer conformation locks and provides one-dimensional charge transport. Furthermore, the robust electron-donating nature of EDOT imparts the small molecule with cascade energy levels relative to the electron donor and acceptor. As a result, OSCs incorporating the EDOT-based small molecule as the third component demonstrate enhanced mobilities, yielding a remarkable efficiency of 19.3 %, surpassing the efficiency of 18.7 % observed for OSCs incorporating thiophene-based small molecule as the third component. The investigations in this study underscore the excellence of EDOT as a building block for constructing conjugated materials with multiple conformation locks and high charge carrier mobilities, thereby contributing to elevated photovoltaic performance in OSCs.

关键词： Organic solar cells ethylenedioxythiophene conformation locks power conversion efficiency

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Formulating the Electrolyte Towards High-Energy and Safe Rechargeable Lithium–Metal Batteries

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Angewandte Chemie 2021年第30期133卷

作者： Qiang Ma Dr. Junpei Yue Min Fan Shuang-Jie Tan Dr. Juan Zhang Dr. Wen-Peng Wang Dr. Yuan Liu Yi-Fan Tian Dr. Quan Xu Prof. Ya-Xia Yin Prof. Ya You Prof. An Luo Prof. Sen Xin Prof. Xiong-Wei Wu Prof. Yu-Guo Guo College of Electrical and Information Engineering Hunan University Changsha Hunan 410082 P. R. China School of Chemistry and Materials Science College of Agronomy Hunan Agricultural University Changsha Hunan 410128 P. R. China CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular Sciences Beijing National Laboratory for Molecular Sciences (BNLMS) Institute of Chemistry Chinese Academy of Sciences (CAS) Beijing 100190 P. R. China Nanozyme Medical Center School of Basic Medical Sciences Zhengzhou University Zhengzhou 450001 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei P. R. China

Rechargeable lithium–metal batteries with a cell-level specific energy of >400 Wh kg −1 are highly desired for next-generation storage applications, yet the research has been retarded by poor electrolyte–electrode compatibility and rigorous safety concerns. We demonstrate that by simply formulating the composition of conventional electrolytes, a hybrid electrolyte was constructed to ensure high (electro)chemical and thermal stability with both the Li-metal anode and the nickel-rich layered oxide cathodes. By employing the new electrolyte, Li∥LiNi 0.6 Co 0.2 Mn 0.2 O 2 cells show favorable cycling and rate performance, and a 10 Ah Li∥LiNi 0.8 Co 0.1 Mn 0.1 O 2 pouch cell demonstrates a practical specific energy of >450 Wh kg −1 . Our findings shed light on reasonable design principles for electrolyte and electrode/electrolyte interfaces toward practical realization of high-energy rechargeable batteries.

关键词： hybrid electrolytes in situ polymerization interfacial chemistry rechargeable lithium–metal batteries

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Three-dimensionally ordered macroporous materials for photo/electrocatalytic sustainable energy conversion, solar cell and energy storage

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EnergyChem 2022年第4期4卷

作者： Yang Ding Chunhua Wang Runtian Zheng Soumyajit Maitra Genwei Zhang Tarek Barakat Subhasis Roy Bao-Lian Su Li-Hua Chen Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 rue de Bruxelles B-5000 Namur Belgium Department of Chemistry KU Leuven Celestijnenlaan 200F B-3001 Leuven Belgium Department of Chemical Engineering University of Calcutta 92 APC Road Kolkata West Bengal 700009 India Department of Chemistry Fudan University 2005 Songhu Road 200438 Shanghai China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Clare Hall University of Cambridge Cambridge CB2 1EW UK

Three-dimensionally ordered macroporous (3DOM) materials have aroused tremendous interest in solar light to energy conversion, sustainable and renewable products generation, and energy storage fields owing to their convenient mass transfer channels, high surface area, enhanced interaction between matter and light, plentiful reactive sites as well as tunable composition. In this review, the state-of-the-art 3DOM materials as well as their preparation methods and the relevant applications including photo/electrocatalytic sustainable energy conversion, solar cells, Li ion batteries and supercapacitor are thoroughly outlined. Meanwhile, the unique merits and mechanisms for 3DOM materials in various applications are revealed and discussed in depth. Moreover, the strategies for designing 3DOM materials and the enhanced performance for applications are correlated, which can be significantly valuable to help readers to promptly acquire the comprehensive knowledge and to inspire some new ideas in developing 3DOM materials for further improved performances. Finally, the challenges and perspectives of 3DOM materials for sustainable energy conversion/production, solar cells and energy storage fields are outlooked. We sincerely look forward to that this critical review can facilitate the fast developments in designing highly efficient 3DOM materials and the relevant applications.

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Kinetics Controlled Perovskite Crystallization for High Performance Solar Cells

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Angewandte Chemie 2024年第14期136卷

作者： Jinghao Ge Ran Chen Yabin Ma Yunfan Wang Yingjie Hu Lu Zhang Fengzhu Li Xiaokang Ma Sai-Wing Tsang Jiaxue You Alex K. Y. Jen 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 International Joint Research Center of Shaanxi Province for Photoelectric Materials Science Institute for Advanced Energy Materials School of Materials Science and Engineering Shaanxi Normal University No. 620 West Chang'an Avenue Xi'an 710119 China These authors contributed equally. School of Materials Science and Engineering Xi'an University of Science and Technology No. 67 Xiaozhai East Road Xi'an Shaanxi 710054 PR China Department of Materials Science and Engineering Hong Kong Institute for Clean Energy City University of Hong Kong Tat Chee Avenue Kowloon Hong Kong SAR China State Key Laboratory of Solidification Processing Northwestern Polytechnical University No. 127 Laodong West Road Xi'an Shaanxi 710072 PR China Dalian National Laboratory for Clean Energy iChEM Dalian Institute of Chemical Physics Chinese Academy of Sciences No.457 Zhongshan Road Shahekou District Dalian 116023 China University of the Chinese Academy of Sciences No. 80 Zhongguancun East Road Beijing 100039 China

The power conversion efficiencies (PCEs) of perovskite solar cells have recently developed rapidly compared to crystalline silicon solar cells. To have an effective way to control the crystallization of perovskite thin films is the key for achieving good device performance. However, a paradox in perovskite crystallization is from the mismatch between nucleation and Oswald ripening. Usually, the large numbers of nucleation sites tend to weak Oswald ripening. Here, we proposed a new mechanism to promote the formation of nucleation sites by reducing surface energy from 44.9 mN/m to 36.1 mN/m, to spontaneously accelerate the later Oswald ripening process by improving the grain solubility through the elastic modulus regulation. The ripening rate is increased from 2.37 Åm ⋅ s −1 to 4.61 Åm ⋅ s −1 during annealing. Finally, the solar cells derived from the optimized films showed significantly improved PCE from 23.14 % to 25.32 %. The long-term stability tests show excellent thermal stability (the optimized device without encapsulation maintaining 82 % of its initial PCE after 800 h aging at 85 °C) and an improved light stability under illumination. This work provides a new method, the elastic modulus regulation, to enhance the ripening process.

关键词： Perovskite solar cells Oswald ripening crystallization kinetics nucleation surface energy

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High-Performance Thermoelectric α-Ag9Ga1−xTe6Compounds with Ultralow Lattice Thermal Conductivity Originating from Ag9Te2Motifs

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Angewandte Chemie 2022年第36期134卷

作者： Yingfei Tang Yimeng Yu Na Zhao Keke Liu Haijie Chen Constantinos C. Stoumpos Yixuan Shi Shuo Chen Lingxiao Yu Jinsong Wu Qingjie Zhang Xianli Su Xinfeng Tang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Investigation (equal) Methodology (equal) Visualization (equal) Writing - original draft (lead) Nanostructure Research Center Wuhan University of Technology Wuhan 430070 China Contribution: Data curation (equal) Software (equal) Visualization (supporting) Contribution: Investigation (equal) Methodology (equal) Contribution: Investigation (equal) Methodology (equal) Visualization (equal) State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Institute of Functional Materials College of Materials Science and Engineering Donghua University Shanghai 201620 China Contribution: Methodology (equal) Visualization (equal) Writing - review & editing (equal) Department of Materials Science and Technology Voutes Campus University of Crete Iraklio Heraklion 70013 Greece Contribution: Methodology (equal) Visualization (equal) Contribution: Investigation (equal) Visualization (equal) Contribution: Conceptualization (equal) Investigation (equal) Contribution: Methodology (equal) Contribution: Conceptualization (equal) Methodology (equal) Contribution: Conceptualization (equal) Investigation (equal) Methodology (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Funding acquisition (lead) Methodology (equal) Supervision (equal) Writing - review & editing (equal)

We have determined the complex atomic structure of high-temperature α-Ag 9 GaTe 6 phase with a hexagonal lattice ( P 6 3 mc space group, a = b =8.2766 Å, c =13.4349 Å). The structure has outer [GaTe 4 ] 5− tetrahedrons and inner [Ag 9 Te 2 ] 5+ clusters. All of the Ag ions are disorderly distributed in the lattice. Seven types of the Ag atoms constitute the cage-like [Ag 9 Te 2 ] 5+ clusters. The highly disordered Ag ions vibrate in-harmonically, producing strong coupling between low frequency optical phonons and acoustic phonons. This in conjunction with a low sound velocity of 1354 m s −1 leads to an ultralow thermal conductivity of 0.20 W m −1 K −1 at 673 K. Meanwhile, the deficiency of Ga in Ag 9 Ga 1− x Te 6 compounds effectively optimizes the electronic transport properties. Ag 9 Ga 0.91 Te 6 attains a highest power factor of 0.40 mW m −1 K −2 at 673 K. All these contribute to a much-improved ZT value of 1.13 at 623 K for Ag 9 Ga 0.95 Te 6 , which is 41 % higher than that of the pristine Ag 9 GaTe 6 sample.

关键词： α-Ag9GaTe6 Crystal Structure Ga Deficiency Thermoelectrics Ultralow Lattice Thermal Conductivity

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[email protected] 2 hybrid microcapsules with high in vivo biocompatibility and stability for cell therapy

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Colloids and Surfaces B: Biointerfaces 2021年 203卷

作者： Grégory Leroux Myriam Neumann Christophe F. Meunier Virginie Voisin Isabelle Habsch Nathalie Caron Carine Michiels Li Wang Bao-Lian Su Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Namur Institute of Structured Matter (NISM) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Molecular Physiology Research Unit (URPhyM) Namur Research Institute for Life Sciences (NARILIS) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium Laboratory of Biochemistry and Cell Biology (URBC) Namur Research Institute for Life Sciences (NARILIS) University of Namur 61 Rue de Bruxelles B-5000 Namur Belgium State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Luoshi Road 122 Wuhan 430070 China

Designing new materials to encapsulate living therapeutic cells for the treatment of the diseases caused by protein or hormone deficiencies is a great challenge. The desired materials need to be biocompatible towards both entrapped cells and host organisms, have long-term in vivo stability after implantation, allow the diffusion of nutrients and metabolites, and ensure perfect immune-isolation. The current work investigates the in vivo biocompatibility and stability of [email protected] 2 hybrid microcapsules and the immune-isolation of entrapped HepG2 cells, to assess their potential for cell therapy. A comparison was made with alginate-silica hybrid microcapsules (ASA). These two hybrid microcapsules are implanted subcutaneously in female Wistar rats. The inflammatory responses of the rats are monitored by the histological examination of the implants and the surrounding tissues, to indicate their in vivo biocompatibility towards the hosts. The in vivo stability of the microcapsules is evaluated by the recovery rate of the intact microcapsules after implantation. The immune-isolation of the entrapped cells is assessed by their morphology, membrane integrity and intracellular enzymatic activity. The results show high viability of the entrapped cells and insignificant inflammation of the hosts, suggesting the excellent biocompatibility of [email protected] 2 and ASA microcapsules towards both host organisms and entrapped cells. Compared to the ASA microcapsules, more intact [email protected] 2 hybrid microcapsules are recovered 2-day and 2-month post-implantation and more cells remain alive, proving their better in vivo biocompability, stability, and immune-isolation. The present study demonstrates that the [email protected] 2 hybrid microcapsule is a highly promising implantation material for cell therapy.

关键词： Hybrid hydrogels Cell encapsulation In vivo biocompatibility In vivo stability Immune isolation

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Engineering a Local Free Water Enriched Microenvironment for Surpassing Platinum Hydrogen Evolution Activity

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Angewandte Chemie 2022年第35期134卷

作者： Qunlei Wen Junyuan Duan Wenbin Wang Dr. Danji Huang Dr. Youwen Liu Dr. Yongliang Shi Prof. JiaKun Fang Prof. Anmin Nie Prof. Huiqiao Li Prof. Tianyou Zhai State Key Laboratory of Materials Processing and Die & Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Conceptualization (equal) Investigation (lead) Writing - original draft (lead) Contribution: Formal analysis (equal) Investigation (equal) Contribution: Investigation (supporting) Writing - original draft (supporting) State Key Lab of Advanced Electromagnetic Engineering and Technology School of Electrical and Electronic Engineering Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China Contribution: Formal analysis (supporting) Investigation (supporting) Contribution: Conceptualization (lead) Formal analysis (lead) Writing - review & editing (lead) Center for Spintronics and Quantum Systems State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and Engineering Xi'an Jiaotong University Xi'an Shanxi 710049 P. R. China Contribution: Investigation (lead) Writing - review & editing (equal) Contribution: Conceptualization (supporting) Formal analysis (equal) Investigation (equal) Writing - review & editing (equal) Center for High Pressure Science State Key Laboratory of Metastable Materials Science and Technology Yanshan University Qinhuangdao Hebei 066004 P. R. China Contribution: Formal analysis (equal) Contribution: Writing - review & editing (equal) Contribution: Conceptualization (supporting) Project administration (lead) Supervision (equal) Writing - review & editing (equal)

Manipulating the catalyst–electrolyte interface to push reactants into the inner Helmholtz plane (IHP) is highly desirable for efficient electrocatalysts, however, it has rarely been implemented due to the elusive electrochemical IHP and inherent inert catalyst surface. Here, we propose the introduction of local force fields by the surface hydroxyl group to engineer the electrochemical microenvironment and enhance alkaline hydrogen evolution activity. Taking a hydroxyl group immobilized Ni/Ni 3 C heterostructure as a prototype, we reveal that the local hydrogen bond induced by the surface hydroxyl group drags 4-coordinated hydrogen-bonded H 2 O molecules across the IHP to become free H 2 O and thus continuously supply reactants forcatalytic sites catalytic sites. In addition, the hydroxyl group coupled with the Ni/Ni 3 C heterostructure further lowers the water dissociation energy by polarization effects. As a direct outcome, hydroxyl-rich catalysts surpass Pt/C activity at high current density (500 mA cm −2 @ ≈276 mV) in alkaline medium.

关键词： Electrochemical Double Layer High Current Densities Hydrogen Evolution Local Hydrogen Bond Surface Hydroxyl

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