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第29届中国数据库学术会议

作者： Rong Chuitian 荣垂田 Xu Tianren 徐天任 Du Xiaoyong 杜小勇 Key Laboratory of Data Engineering and Knowledge Engineering(Renmin University of China) Ministry o 教育部数据工程与知识工程重点实验室(中国人民大学) 北京 100872 中国人民大学信息学院北京 100872 School of Information Renmin University of China Beijing 100872 Key Laboratory of Education Inform 中国人民大学信息学院北京 100872 民族教育信息化教育部重点实验室(云南师范大学) 昆明 650500

集合相似连接(set similarity join)是指在给定的数据集中，按照基于集合间覆盖关系的相似度计算方法来衡量数据之间的相似度、并找出所有相似度不小于给定阈值的数据对的操作。集合相似连接作为一种新的基本操作在很多领域中有重要应... 详细信息

集合相似连接(set similarity join)是指在给定的数据集中，按照基于集合间覆盖关系的相似度计算方法来衡量数据之间的相似度、并找出所有相似度不小于给定阈值的数据对的操作。集合相似连接作为一种新的基本操作在很多领域中有重要应用。随着社会网络、移动应用以及在线服务的发展，使得数据收集的效率和规模得到了很大的提高，同时给相似连接操作带来新的挑战。根据集合相似的必要条件，提出了相似集合之间的差异度。利用差异度和鸽巢原理，提出了一种新颖的基于数据划分的集合相似连接计算方法，该方法对集合进行自适应的均衡划分，并利用基于划分块的过滤方法来提高过滤的效率。为了进一步提高过滤的效果和相似连接的效率，利用划分块的位置信息提出了增强的过滤方法。针对提出的方法，在不同的环境下进行了实验，实验结果表明，该方法与已有的方法相比可以有效地提高相似连接的效率。

关键词：数据库集合相似连接均衡划分法阈值

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Wide Band-Gap Polymer Donors Functionalized with Unconventional Carbamate Side Chains for Polymer Solar Cells

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Angewandte Chemie 2022年第50期134卷

作者： Jie Tang Chentong Liao Yuwei Duan Xiaopeng Xu Min Deng Liyang Yu Ruipeng Li Qiang Peng School of Chemical Engineering College of Chemistry and State Key Laboratory of Polymer Materials Engineering Sichuan University Chengdu 610065 P. R. China Contribution: Conceptualization (equal) Data curation (lead) Formal analysis (lead) Methodology (lead) Contribution: Data curation (equal) Formal analysis (equal) Methodology (equal) Key Laboratory of Applied Surface and Colloid Chemistry of Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science & Engineering Shaanxi Normal University Xi'an 710119 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Contribution: Conceptualization (supporting) Formal analysis (supporting) Investigation (supporting) Supervision (supporting) Writing - original draft (lead) Writing - review & editing (supporting) National Synchrotron Light Source II Brookhaven National Lab Suffolk Upton NY 11973 USA Contribution: Conceptualization (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - review & editing (lead)

Side-chain engineering with heteroatoms is not only effective in tuning frontier molecular orbitals, but also possible for forming secondary bonds which can be utilized to planarize the molecular backbone, hence, improving the photon absorption as well as charge-transport abilities of polymer solar-cell (PSC) materials. Herein, two types of unconventional side chains, namely carboxylate and carbamate, containing various heteroatoms are introduced to the thiophene bridges in high performance benzodithiophene (BDT) based donor polymers to from the novel polymers PTzTz-C and PTzTz-N, respectively. In these polymers, non-covalent O⋅⋅⋅S and N⋅⋅⋅H interactions induce a high tendency to aggregation. In a ternary-blend PSC with PTzTz-N added to the high-performance D18 : BTP-eC9 blend, complimentary absorption and improved thin-film morphology were observed with a top power conversion efficiency of 18.76 %, which is an improvement of almost 5 % over the D18 : BTP-eC9 binary blends.

关键词： Carbamate Conformation Locks Donor Polymer Solar Cells

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Crystallization Regulation by Self-Assembling Liquid Crystal Template Enables Efficient and Stable Perovskite Solar Cells

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Angewandte Chemie 2023年第52期135卷

作者： Meizi Wu Hongyan Wang Yong Li Dr. Ran Chen Hui Zhou Shaomin Yang Dongfang Xu Kun Li Prof. Dr. Zhongwei An Shengzhong (Frank) Liu Prof. Dr. Zhike 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 School of Materials Science & Engineering Shaanxi Normal University Xi'an 710119 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Contribution: Data curation (equal) Investigation (equal) School of Materials Science and Engineering Xi' an University of Science and Technology Xi'an 710054 P. R. China Contribution: Conceptualization (lead) Methodology (equal) Contribution: Formal analysis (equal) Investigation (equal) Contribution: Methodology (equal) Contribution: Data curation (equal) Contribution: Investigation (equal) Contribution: Conceptualization (equal) Methodology (equal) Contribution: Conceptualization (equal) Methodology (equal) Writing - review & editing (lead)

It is found that the disordered growth of bottom perovskite film deteriorates the buried interface of perovskite solar cells (PSCs), so developing a new material to modify the buried interface for regulating the crystal growth and defect passivation is an effective approach for improving the photovoltaic performance of PSCs. Here, we developed a new ionic liquid crystal (ILC, 1-Dodecyl-3-methylimidazolium tetrafluoroborate) as both crystal regulator and defect passivator to modify the buried interface of PSCs. The high lattice matching between this ILC and perovskite promotes preferential growth of perovskite film along [001] direction, while the oriented ILC with mesomorphic phase has a strong chemical interaction with perovskite to passivate the interface defect, as a result, the modified buried interface exhibits suppressed defects, improved band alignment, reduced nonradiative recombination losses, and enhanced charge extraction. The ILC-modified PSC delivers a power conversion efficiency of 24.92 % and maintains 94 % of the original value after storage in ambient for 3000 h.

关键词： Crystallization Regulation Ionic Liquid Crystals Perovskite Solar Cells Self-Assembling

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A Targeting Singlet Oxygen Battery for Multidrug-Resistant Bacterial Deep-Tissue Infections

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Angewandte Chemie 2023年第36期135卷

作者： Yiwen Zhu Minzheng Gao Mengrui Su Yanzhe Shen Kai Zhang Bingran Yu Fu-Jian Xu State Key Laboratory of Chemical Resource Engineering Key Lab of Biomedical Materials of Natural Macromolecules (Beijing University of Chemical Technology Ministry of Education) Laboratory of Biomedical Materials Beijing University of Chemical Technology Beijing 100029 China Contribution: Methodology (equal) Software (equal) Writing - original draft (lead) Contribution: Methodology (equal) Software (equal) Writing - original draft (equal) Contribution: Methodology (equal) Contribution: Methodology (supporting) Contribution: Data curation (lead) Contribution: Conceptualization (lead) Funding acquisition (equal) Writing - review & editing (lead)

Traditional photodynamic therapy (PDT) is dependent on externally applied light and oxygen, and the depth of penetration of these factors can be insufficient for the treatment of deep infections. The short half-life and short diffusion distance of reactive oxygen species (ROS) also limit the antibacterial efficiency of PDT. Herein, we designed a targeting singlet oxygen delivery system, CARG-Py, for irradiation-free and oxygen-free PDT. This system was converted to the “singlet oxygen battery” CARG- 1 O 2 and released singlet oxygen without external irradiation or oxygen. CARG- 1 O 2 is composed of pyridones coupled to a targeting peptide that improves the utilization of singlet oxygen in deep multidrug-resistant bacterial infections. CARG- 1 O 2 was shown to damage DNA, protein, and membranes by increasing the level of reactive oxygen inside bacteria; the attacking of multiple biomolecular sites caused the death of methicillin-resistant Staphylococcus aureus (MRSA). An in vivo study in a MRSA-infected mouse model of pneumonia demonstrated the potential of CARG- 1 O 2 for the efficient treatment of deep infections. This work provides a new strategy to improve traditional PDT for irradiation- and oxygen-free treatment of deep infections while improving convenience of PDT.

关键词： Antibacterial Mechanism Deep-Tissue Infections Multidrug-Resistant Singlet Oxygen Battery Targeting Therapy

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

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Angewandte Chemie 2023年第38期135卷

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

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

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

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

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Angewandte Chemie 2022年第6期135卷

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

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

关键词： Chelation Defect Passivation Inorganic Perovskite Solar Cells

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Changing life expectancy in European countries 1990–2021: a subanalysis of causes and risk factors from the Global Burden of Disease Study 2021

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The Lancet Public Health 2025年第3期10卷 e172-e188页

作者： Steel, Nicholas Bauer-Staeb, Clarissa Maria Mercedes Ford, John A. Abbafati, Cristiana Abdalla, Mohammed Altigani Abdelkader, Atef Abdi, Parsa Zuñiga, Roberto Ariel Abeldaño Abiodun, Olugbenga Olusola Abolhassani, Hassan Abu-Gharbieh, Eman Abukhadijah, Hana J. Abu-Zaid, Ahmed Addo, Isaac Yeboah Addolorato, Giovanni Adekanmbi, Victor Adetunji, Juliana Bunmi Adeyeoluwa, Temitayo Esther Agardh, Emilie E. Agyemang-Duah, Williams Ahmad, Danish Ahmed, Ayman Ahmed, Syed Anees Akinosoglou, Karolina Akkaif, Mohammed Ahmed Al Awaidy, Salah Al Hasan, Syed Mahfuz Al Zaabi, Omar Ali Mohammed Aldridge, Robert W. Algammal, Abdelazeem M. Al-Gheethi, Adel Ali Saeed Ali, Abid Ali, Mohammed Usman Ali, Syed Shujait Ali, Waad Alicandro, Gianfranco Alif, Sheikh Mohammad Al-Jumaily, Adel Allebeck, Peter Alrawashdeh, Ahmad Al-Rifai, Rami H. Alsabri, Mohammed A. Alshahrani, Najim Z. Aluh, Deborah Oyine Al-Wardat, Mohammad Al-Zyoud, Walid A. Amiri, Sohrab Anderlini, Deanna Andrei, Catalina Liliana Anil, Abhishek Anvari, Saeid Anyasodor, Anayochukwu Edward Appiah, Seth Christopher Yaw Aquilano, Michele Arabloo, Jalal Arafat, Mosab Areda, Demelash Aremu, Abdulfatai Armani, Keivan Armocida, Benedetta Ärnlöv, Johan Asaduzzaman, Muhammad Astell-Burt, Thomas Aujayeb, Avinash Ausloos, Marcel Azadnajafabad, Sina Aziz, Shahkaar Azzam, Ahmed Y. Babu, Giridhara Rathnaiah Badache, Andreea Corina Badiye, Ashish D. Bahramian, Saeed Baig, Atif Amin Baker, Jennifer L. Bansal, Hansi Bärnighausen, Till Winfried Barone, Mark Thomaz Ugliara Barrow, Amadou Barteit, Sandra Bashir, Shahid Bashiru, Hameed Akande Basso, João Diogo Bastan, Mohammad-Mahdi Basu, Sanjay Batra, Kavita Bauckneht, Matteo Baune, Bernhard T. Beghi, Massimiliano Beiranvand, Maryam Béjot, Yannick Bell, Michelle L. Bello, Olorunjuwon Omolaja Belo, Luis Beloukas, Apostolos Beneke, Alice A. Bettencourt, Paulo J.G. Bhagavathula, Akshaya Srikanth Bhala, Neeraj Bhaskar, Sonu Bisulli, Francesca Bjørge, Tone Bodunrin, Aadam Olalekan Carvajal, Alejandro Botero Bouaoud, Souad Brayne, Carol Brenner, H Department of Primary Care and Public Health University of East Anglia Norwich United Kingdom Office for Health Improvement and Disparities Department of Health and Social Care London United Kingdom Department of Legal and Economic Studies La Sapienza University Rome Italy Rome Italy Hull York Medical School University of Hull Hull United Kingdom Department of Mathematics and Sciences Ajman University Ajman United Arab Emirates Department of Medicine Memorial University St. John's NL Canada Postgraduate Department University of Sierra Sur Miahuatlan de Porfirio Diaz Mexico Yhteiskuntadatatieteen keskus (Centre for Social Data Science) Helsinki Finland Department of Internal Medicine Federal Medical Centre Abuja Nigeria Research Center for Immunodeficiencies Tehran University of Medical Sciences Tehran Iran Department of Medical Biochemistry and Biophysics Karolinska Institutet (Karolinska Institute) Stockholm Sweden Department of Clinical Sciences University of Sharjah Sharjah United Arab Emirates Department of Biopharmaceutics and Clinical Pharmacy University of Jordan Amman Jordan Medical Research Center Hamad Medical Corporation Doha Qatar Department of Biochemistry and Molecular Medicine Alfaisal University Riyadh Saudi Arabia College of Graduate Health Sciences University of Tennessee Memphis TN United States School of Medicine Sydney NSW Australia Centre for Social Research in Health University of New South Wales Sydney NSW Australia Internal Medicine and Alcohol Related Disease Unit Fondazione Policlinico Universitario A. Gemelli IRCCS Rome Italy Department of Medical and Surgical Sciences Università Cattolica di Roma (Catholic University of Rome) Rome Italy Department of Obstetrics and Gynecology University of Texas Medical Branch Galveston TX United States Department of Biochemistry Osun State University Osogbo Nigeria Department of Pharmacology and Therapeutics University of Medical Sciences Ondo Ondo Nigeria Department of Veteri

Background: Decades of steady improvements in life expectancy in Europe slowed down from around 2011, well before the COVID-19 pandemic, for reasons which remain disputed. We aimed to assess how changes in risk factors and cause-specific death rates in different European countries related to changes in life expectancy in those countries before and during the COVID-19 pandemic. Methods: We used data and methods from the Global Burden of Diseases, Injuries, and Risk Factors Study 2021 to compare changes in life expectancy at birth, causes of death, and population exposure to risk factors in 16 European Economic Area countries (Austria, Belgium, Denmark, Finland, France, Germany, Greece, Iceland, Ireland, Italy, Luxembourg, the Netherlands, Norway, Portugal, Spain, and Sweden) and the four UK nations (England, Northern Ireland, Scotland, and Wales) for three time periods: 1990–2011, 2011–19, and 2019–21. Changes in life expectancy and causes of death were estimated with an established life expectancy cause-specific decomposition method, and compared with summary exposure values of risk factors for the major causes of death influencing life expectancy. Findings: All countries showed mean annual improvements in life expectancy in both 1990–2011 (overall mean 0·23 years [95% uncertainty interval [UI] 0·23 to 0·24]) and 2011–19 (overall mean 0·15 years [0·13 to 0·16]). The rate of improvement was lower in 2011–19 than in 1990–2011 in all countries except for Norway, where the mean annual increase in life expectancy rose from 0·21 years (95% UI 0·20 to 0·22) in 1990–2011 to 0·23 years (0·21 to 0·26) in 2011–19 (difference of 0·03 years). In other countries, the difference in mean annual improvement between these periods ranged from –0·01 years in Iceland (0·19 years [95% UI 0·16 to 0·21] vs 0·18 years [0·09 to 0·26]), to –0·18 years in England (0·25 years [0·24 to 0·25] vs 0·07 years [0·06 to 0·08]). In 2019–21, there was an overall decrease in mean annual life expectancy a

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Polyoxometalate-Cyclodextrin-Based Cluster-Organic Supramolecular Framework for Polysulfide Conversion and Guest–Host Recognition in Lithium-sulfur Batteries

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Angewandte Chemie 2023年第36期135卷

作者： Prof. Lubin Ni Jie Gu Xinyuan Jiang Hongjie Xu Zhen Wu Yuchao Wu Yi Liu Prof. Ju Xie Prof. Yongge Wei Prof. Guowang Diao School of Chemistry and Chemical Engineering Yangzhou University Yangzhou 225002 Jiangsu P. R. China Contribution: Conceptualization (lead) Data curation (lead) Funding acquisition (lead) Methodology (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Resources (equal) Software (equal) Contribution: Data curation (equal) Investigation (equal) Software (equal) Contribution: Data curation (equal) Investigation (equal) Software (equal) Validation (equal) Visualization (equal) Contribution: Validation (equal) Visualization (equal) Contribution: Methodology (equal) Visualization (equal) Key Lab of Organic Optoelectronics & Molecular Engineering of Ministry of Education Department of Chemistry Tsinghua University Beijing 100084 P. R. China Contribution: Conceptualization (equal) Project administration (equal) Resources (equal) Supervision (lead) Writing - original draft (equal) Writing - review & editing (lead) Contribution: Resources (lead) Supervision (equal) Writing - review & editing (lead)

Developing polyoxometalate-cyclodextrin cluster-organic supramolecular framework (POM-CD-COSF) still remains challenging due to an extremely difficult task in rationally interconnecting two dissimilar building blocks. Here we report an unprecedented POM-CD-COSF crystalline structure produced through the self-assembly process of a Krebs -type POM, [Zn 2 (WO 2 ) 2 (SbW 9 O 33 ) 2 ] 10− , and two β-CD units. The as-prepared POM-CD-COSF-based battery separator can be applied as a lightweight barrier (approximately 0.3 mg cm −2 ) to mitigate the polysulfide shuttle effect in lithium-sulfur batteries. The designed Li−S batteries equipped with the POM-CD-COSF modified separator exhibit remarkable electrochemical performance, attributed to fast Li + diffusion through the supramolecular channel of β-CD, efficient polysulfide-capture ability by the dynamic host–guest interaction of β-CD, and improved sulfur redox kinetics by the bidirectional catalysis of POM cluster. This research provides a broad perspective for the development of multifunctional supramolecular POM frameworks and their applications in Li−S batteries.

关键词： Cluster-Organic Supramolecular Framework Cyclodextrin Lithium–Sulfur Batteries Polyoxometalates Polysulfide

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

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Angewandte Chemie 2023年第33期135卷

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

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

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

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Managing Multiple Halide-Related Defects for Efficient and Stable Inorganic Perovskite Solar Cells

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Angewandte Chemie 2023年第30期135卷

作者： Zhiteng Wang Prof. Qingwen Tian Hao Zhang Prof. Huidong Xie Yachao Du Lei Liu Xiaolong Feng Adel Najar Xiaodong Ren Prof. Shengzhong (Frank) Liu Key Laboratory of Applied Surface and Colloid Chemistry Ministry of Education Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy Technology School of Materials Science and Engineering Shaanxi Normal University Xi'an 710119 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Investigation (lead) Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (lead) Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 P. R. China Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) School of Chemistry and Chemical Engineering Xi'an University of Architecture and Technology Xi'an 710055 P. R. China Contribution: Formal analysis (supporting) Validation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Resources (supporting) Department of Physics College of Science United Arab Emirates University Al Ain 15551 United Arab Emirates Contribution: Supervision (supporting) Validation (supporting) Writing - review & editing (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Methodology (supporting) Contribution: Funding acquisition (lead) Project administration (lead) Validation (lead) Writing - review & editing (lead)

Halide-related surface defects on inorganic halide perovskite not only induce charge recombination but also severely limit the long-term stability of perovskite solar cells. Herein, adopting density functional theory calculation, we verify that iodine interstitials (I i ) has a low formation energy similar to that of the iodine vacancy (V I ) and is also readily formed on the surface of all-inorganic perovskite, and it is regarded to function as an electron trap. We screen a specific 2,6-diaminopyridine (2,6-DAPy) passivator, which, with the aid of the combined effects from halogen-N pyridine and coordination bonds, not only successfully eliminates the I i and dissociative I 2 but also passivates the abundant V I . Furthermore, the two symmetric neighboring -NH 2 groups interact with adjacent halides of the octahedral cluster by forming hydrogen bonds, which further promotes the adsorption of 2,6-DAPy molecules onto the perovskite surface. Such synergetic effects can significantly passivate harmful iodine-related defects and undercoordinated Pb 2+ , prolong carrier lifetimes and facilitate the interfacial hole transfer. Consequently, these merits enhance the power-conversion efficiency (PCE) from 19.6 % to 21.8 %, the highest value for this type of solar cells, just as importantly, the 2,6-DAPy-treated CsPbI 3− x Br x films show better environmental stability.

关键词： All-Inorganic Perovskite CsPbI3−xBrx Defect Passivation Iodine-Related Defects Solar Cells

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