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Over 19 % Efficiency Organic Solar Cells Enabled by Manipulating the Intermolecular Interactions through Side Chain Fluorine Functionalization

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Angewandte Chemie 2024年第15期136卷

作者： Prof. Huawei Hu Shuai Liu Jiaoyu Xu Dr. Ruijie Ma Dr. Zhengxing Peng Top Archie Dela Peña Dr. Yongjie Cui Wenting Liang Xiaoli Zhou Dr. Siwei Luo Dr. Han Yu Prof. Mingjie Li Prof. Jiaying Wu Prof. Shangshang Chen Prof. Gang Li Prof. Yiwang Chen State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Shanghai 201620 P. R. China Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education/National Engineering Research Center for Carbohydrate Synthesis Jiangxi Normal University 99 Ziyang Avenue Nanchang 330022 P. R. China Department of Electrical and Electronic Engineering Research Institute for Smart Energy (RISE) Guangdong-Hong Kong-Macao (GHM) Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices The Hong Kong Polytechnic University Hung Hom Kowloon Hong Kong 999077 P. R. China Advanced Light Source Lawrence Berkeley National Laboratory Berkeley CA 94720 USA Function Hub Advanced Materials Thrust The Hong Kong University of Science and Technology Nansha 511400 Guangzhou P. R. China The Hong Kong Polytechnic University Faculty of Science Department of Applied Physics Kowloon Hong Kong 000000 P. R. China Department of Chemistry Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong 999077 P. R. China School of Chemistry and Chemical Engineering Nanjing University Nanjing 210023 P. R. China

Fluorine side chain functionalization of non-fullerene acceptors (NFAs) represents an effective strategy for enhancing the performance of organic solar cells (OSCs). However, a knowledge gap persists regarding the relationship between structural changes induced by fluorine functionalization and the resultant impact on device performance. In this work, varying amounts of fluorine atoms were introduced into the outer side chains of Y-series NFAs to construct two acceptors named BTP-F0 and BTP-F5. Theoretical and experimental investigations reveal that side-chain fluorination significantly increase the overall average electrostatic potential (ESP) and charge balance factor, thereby effectively improving the ESP-induced intermolecular electrostatic interaction, and thus precisely tuning the molecular packing and bulk-heterojunction morphology. Therefore, the BTP-F5-based OSC exhibited enhanced crystallinity, domain purity, reduced domain spacing, and optimized phase distribution in the vertical direction. This facilitates exciton diffusion, suppresses charge recombination, and improves charge extraction. Consequently, the promising power conversion efficiency (PCE) of 17.3 % and 19.2 % were achieved in BTP-F5-based binary and ternary devices, respectively, surpassing the PCE of 16.1 % for BTP-F0-based OSCs. This work establishes a structure-performance relationship and demonstrates that fluorine functionalization of the outer side chains of Y-series NFAs is a compelling strategy for achieving ideal phase separation for highly efficient OSCs.

关键词： non-fullerene acceptors fluorine functionalization intermolecular interactions solar cells molecular packing

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The Nature of Structural Defects in ZIF-8 Revealed with1H and31P MAS NMR and X-Ray Absorption Spectroscopy

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Angewandte Chemie 2024年第2期137卷

作者： Dr. Anton A. Gabrienko Dr. Somboon Chaemchuen Dr. Zongkui Kou Prof. Naoki Ogiwara Prof. Hiroshi Kitagawa Dr. Alexander E. Khudozhitkov Prof. Alexander G. Stepanov Dr. Daniil I. Kolokolov Prof. Francis Verpoort Boreskov Institute of Catalysis Novosibirsk Ac. Lavrentiev av. 5 Novosibirsk 630090 Russia Both authors contributed equally State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China Department of Chemical Engineering Faculty of Engineering Mahidol University Nakhon Pathom 73170 Thailand Department of Basic Science School of Arts and Sciences The University of Tokyo 3-8-1 Komaba Meguro-ku Tokyo 153-8902 Japan Division of Chemistry Graduate School of Science Kyoto University Kitashirakawa-Oiwakecho Sakyo-ku Kyoto 606-8502 Japan School of Chemistry and Chemical Engineering Shandong University of Technology Zibo 255049 China Joint Institute of Chemical Research (FFMiEN) Peoples Friendship University of Russia (RUDN University) 6 Miklukho-Maklaya Str. 117198 Moscow Russia

The metal–organic frameworks (MOFs) attract interest as potential catalysts whose catalytic properties are driven by defects. Several methods have been proposed for the defects-inducing synthesis of MOFs. However, the active species formed on the defective sites remain elusive and uncharacterized, as the spectroscopic fingerprints of these species are hidden by the regular structure signals. In this work, we have performed the synthesis of ZIF-8 MOF with defect-inducing procedures using fully deuterated 2-methylimidazolate ligands to enhance the defective sites′ visibility. By combining 1 H and 31 P MAS NMR spectroscopy and X-ray absorption spectroscopy, we have found evidence for the presence of different structural hydroxyl Zn−OH groups in the ZIF-8 materials. It is demonstrated that the ZIF-8 defect sites are represented by Zn−OH hydroxyl groups with the signals at 0.3 and −0.7 ppm in the 1 H MAS NMR spectrum. These species are of basic nature and may be responsible for the catalytic activity of the ZIF-8 material.

关键词： metal–organic framework defects solid state NMR XAS catalysis

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Enhanced exchange bias in all-oxide heterostructures with cation-ordered ferrimagnetic double-perovskite

npj Spintronics

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npj Spintronics 2024年第1期2卷 1-6页

作者： Xiaofu Qiu Hetian Chen Yuhan Liang Xiaoyu Jiang Jing Ma Di Yi Zelin Wang Tianxiang Nan Yujun Zhang Fangyuan Zhu Zhen Chen State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China School of Integrated Circuits Beijing National Research Center for Information Science and Technology Tsinghua University Beijing 100084 China National Center for Electron Microscopy in Beijing School of Materials Science and Engineering Tsinghua University Beijing 100084 China Institute of High Energy Physics Chinese Academy of Sciences Beijing 100049 China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of Sciences Shanghai 201204 China Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences Beijing 100190 China School of Physical Sciences University of Chinese Academy of Sciences Beijing 100049 China

The realization and control of exchange bias (EB) are highly desirable for spintronic applications. All-oxide heterostructures comprised of ferromagnetic and antiferromagnetic/multiferroic oxides provide an ideal platform to enable the electric-field control of EB, promising for energy-efficient memory and logic devices. However, the low block temperature (TB) and small bias field (HEB) hinder further advances towards room-temperature applications. Here, we report an alternative approach to enhance the interface-induced EB by using ferrimagnetic double-perovskite with B-site cation ordering. In heterostructures comprised of double-perovskite Sr2FeReO6(SFRO) and LaFeO3(LFO), a high TB(about 250 K) and large HEBare observed, which is significantly larger than the counterparts with LFO and ferromagnetic oxides. Further analysis suggests that the cation-ordering and ferrimagnetic spin structure of the double-perovskite could contribute significantly to the enhanced exchanged bias when interfacing with G-type antiferromagnets. Our results open a new avenue for developing all-oxides heterostructures for future magnetic technologies.

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Publisher Correction:Vertical‑Aligned and Ordered‑Active Architecture of Heterostructured Fibers for High Electrochemical Capacitance

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advanced Fiber materials 2024年第6期6卷 1992-1992页

作者： Xiaolin Zhu Hui Qiu Yang Zhang Zengming Man Wangyang Lu Ningzhong Bao Guan Wu National Engineering Lab for Textile Fiber Materials and Processing Technology Zhejiang Sci-Tech UniversityHangzhou 310018People’s Republic of China Zhejiang Provincial Innovation Center of Advanced Textile Technology Shaoxing 312000People’s Republic of China State Key Laboratory of Materials‑Oriented Chemical Engineering College of Chemical EngineeringNanjing Tech UniversityNanjing 210009People’s Republic of China

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Double Network Elastomers: Self‐Assembly Strategy for Double Network Elastomer Nanocomposites with Ultralow Energy Consumption and Ultrahigh Wear Resistance (Adv. Funct. Mater. 34/2020)

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advanced Functional materials 2020年第34期30卷

作者： Xuan Qin Jiadong Wang Yanli Zhang Zhao Wang Sai Li Shaoquan Zhao Tianwei Tan Jun Liu Liqun Zhang Krzysztof Matyjaszewski Key Laboratory of Beijing City on Preparation and Processing of Novel Polymer Materials North Third Ring Road 15 Beijing 100029 P. R. China Beijing Engineering Research Center of Advanced Elastomers North Third Ring Road 15 Beijing 100029 P. R. China State Key Laboratory of Organic‐Inorganic Composites Beijing University of Chemical Technology North Third Ring Road 15 Beijing 100029 P. R. China Department of Chemistry Carnegie Mellon University 4400 Fifth Avenue Pittsburgh PA 15213 USA National Institute of Metrology North Third Ring Road 18 Beijing 100029 P. R. China

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Atomic Ruthenium-Promoted Cadmium Sulfide for Photocatalytic Production of Amino Acids from Biomass Derivatives

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Angewandte Chemie 2024年第27期136卷

作者： Wulin Li Xiuhui Zheng Bei-Bei Xu Yue Yang Yifei Zhang Lingchao Cai Zhu-Jun Wang Ye-Feng Yao Bing Nan Lina Li Xue-Lu Wang Xiang Feng Markus Antonietti Zupeng Chen Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and Materials Nanjing Forestry University Longpan Road 159 Nanjing 210037 China These authors contributed equally to this work State Key Laboratory of Heavy Oil Processing China University of Petroleum Changjiang West Road 66 Qingdao 266580 China Physics Department Shanghai Key Laboratory of Magnetic Resonance East China Normal University Shanghai 200062 China School of New Energy Nanjing University of Science and Technology Wu Xi Shi Jiangyin 214400 China School of Physical Science and Technology Shanghai Tech University Huaxia Middle Road 393 Shanghai 201210 China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Zhangheng Road 293 Shanghai 201204 China Department of Colloid Chemistry Max-Planck Institute of Colloids and Interfaces Research Campus Golm Am Mühlenberg 1 Potsdam 14476 Germany

Amino acids are the building blocks of proteins and are widely used as important ingredients for other nitrogen-containing molecules. Here, we report the sustainable production of amino acids from biomass-derived hydroxy acids with high activity under visible-light irradiation and mild conditions, using atomic ruthenium-promoted cadmium sulfide (Ru 1 /CdS). On a metal basis, the optimized Ru 1 /CdS exhibits a maximal alanine formation rate of 26.0 mol Ala ⋅ g Ru −1 ⋅ h −1 , which is 1.7 times and more than two orders of magnitude higher than that of its nanoparticle counterpart and the conventional thermocatalytic process, respectively. Integrated spectroscopic analysis and density functional theory calculations attribute the high performance of Ru 1 /CdS to the facilitated charge separation and O−H bond dissociation of the α -hydroxy group, here of lactic acid. The operando nuclear magnetic resonance further infers a unique “double activation” mechanism of both the CH−OH and CH 3 −CH−OH structures in lactic acid, which significantly accelerates its photocatalytic amination toward alanine.

关键词： photocatalysis single-atom catalysis amination amino acids biomass derivatives

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Author Correction: Stabilization of layered lithium-rich manganese oxide for anion exchange membrane fuel cells and water electrolysers

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Nature Catalysis 2024年 604页

作者： Xuepeng Zhong Lijun Sui Menghao Yang Jiwei Ma Toshinari Koketsu Malte Klingenhof Peter Strasser Sören Selve Kyle G. Reeves Chuangxin Ge Lin Zhuang Wang Hay Kan Maxim Avdeev Miao Shu Nicolas Alonso-Vante Jin-Ming Chen Shu-Chih Haw Chih-Wen Pao Yu-Chung Chang Yunhui Huang Zhiwei Hu Shanghai Key Laboratory for R&D and Application of Metallic Functional Materials Institute of New Energy for Vehicles School of Materials Science and Engineering Tongji University Shanghai China Department of Chemistry Technical University Berlin Berlin Germany Battery Materials Development Section Business Creation Sector R&D Center Mitsui Mining and Smelting Company Limited Saitama Japan Center for Electron Microscopy (ZELMI) Technical University Berlin Berlin Germany Maison de la Simulation CEA CNRS Université Paris-Sud UVSQ Université Paris-Saclay Gif-sur-Yvette France The Institute for Advanced Studies Wuhan University Wuhan China Spallation Neutron Source Science Center Dongguan China Institute of High Energy Physics Chinese Academy of Sciences Beijing China Australian Nuclear Science and Technology Organisation Kirrawee DC New South Wales Australia School of Chemistry The University of Sydney Sydney Australia Institute of Advanced Science Facilities Shenzhen China IC2MP UMR-CNRS 7285 University of Poitiers Poitiers France National Synchrotron Radiation Research Center Hsinchu Taiwan State Key Laboratory of Material Processing and Die and Mould Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan China Max Planck Institute for Chemical Physics of Solids Dresden Germany

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Zeolite-Tailored Active Site Proximity for the Efficient Production of Pentanoic Biofuels

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Angewandte Chemie 2021年第44期133卷

作者： Jiang He Prof. Zhijie Wu Dr. Qingqing Gu Dr. Yuanshuai Liu Dr. Shengqi Chu Dr. Shaohua Chen Dr. Yafeng Zhang Dr. Bing Yang Prof. Tiehong Chen Prof. Aiqin Wang Prof. Bert M. Weckhuysen Prof. Tao Zhang Dr. Wenhao Luo CAS Key Laboratory of Science and Technology on Applied Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 P. R. China University of Chinese Academy of Science 19A Yuquan Road Shijingshan District Beijing 100049 P. R. China State Key Laboratory of Heavy Oil Processing and Key Laboratory of Catalysis of CNPC China University of Petroleum 18 Fuxue Road ChangPing Beijing 102249 P. R. China Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 P. R. China Inorganic Chemistry and Catalysis group Debye Institute for Nanomaterials Science Utrecht University Universiteitsweg 99 3584 CG Utrecht The Netherlands Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Sciences 19B Yuquan Road Shijingshan District Beijing 100049 P. R. China Key Laboratory of Advanced Energy Materials Chemistry Institute of New Catalytic Materials Science Nankai University 38 Tongyang Road Tianjin 300350 P. R. China

Biofuel production can alleviate reliance on fossil resources and thus carbon dioxide emission. Hydrodeoxygenation (HDO) refers collectively to a series of important biorefinery processes to produce biofuels. Here, well-dispersed and ultra-small Ru metal nanoclusters (ca. 1 nm), confined within the micropores of zeolite Y, provide the required active site intimacy, which significantly boosts the chemoselectivity towards the production of pentanoic biofuels in the direct, one-pot HDO of neat ethyl levulinate. Crucial for improving catalyst stability is the addition of La, which upholds the confined proximity by preventing zeolite lattice deconstruction during catalysis. We have established and extended an understanding of the “intimacy criterion” in catalytic biomass valorization. These findings bring new understanding of HDO reactions over confined proximity sites, leading to potential application for pentanoic biofuels in biomass conversion.

关键词： bifunctional catalysis biomass conversion hydrodeoxygenation proximity zeolites

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Inside Back Cover: Adamantylidene Addition to M3N@Ih-C80(M=Sc, Lu) and Sc3N@D5h-C80: synthesis and Crystallographic Characterization of the -Open and -Open Adducts (Chem. Eur. J. 27/2017)

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Chemistry – A European Journal 2017年第27期23卷 6701-6701页

作者： Prof. Dr. Michio Yamada Tsuneyuki Abe Chiharu Saito Toshiki Yamazaki Dr. Satoru Sato Dr. Naomi Mizorogi Prof. Dr. Zdenek Slanina Prof. Dr. Filip Uhlík Dr. Mitsuaki Suzuki Prof. Dr. Yutaka Maeda Prof. Dr. Yongfu Lian Prof. Dr. Xing Lu Prof. Dr. Marilyn M. Olmstead Prof. Dr. Alan L. Balch Prof. Dr. Shigeru Nagase Prof. Dr. Takeshi Akasaka Department of Chemistry Tokyo Gakugei University Tokyo 184–8501 Japan Life Science Center of Tsukuba Advanced Research Alliance University of Tsukuba Ibaraki 305–8577 Japan Department of Chemistry and Biochemistry National Chung-Cheng University Chia-Yi 62117 Taiwan R.O.C. Department of Physical and Macromolecular Chemistry Charles University in Prague 128 43 Prague 2 Czech Republic Department of Chemistry Faculty of Science Josai University Saitama 350–0295 Japan Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education School of Chemistry and Materials Science Heilongjiang University Harbin 150080 P.R. China State Key Laboratory of Materials Processing and Die and Mold Technology School of Materials Science and Engineering Huazhong University of Science and Technology Wuhan 430074 P.R. China Department of Chemistry University of California Davis California 95616 USA Fukui Institute for Fundamental Chemistry Kyoto University Kyoto 606–8103 Japan Foundation for Advancement of International Science Ibaraki 305–0821 Japan

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Cooperative Bimetallic Catalysis via One-Metal/Two-Ligands: Mechanistic Insights of Polyfluoroarylation-Allylation of Diazo Compounds

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Angewandte Chemie 2023年第34期135卷

作者： Gao-Yin Wang Zhaoliang Ge Prof. Kuiling Ding Prof. Xiaoming Wang Department of Chemistry University of Science and Technology of China 96 Jinzhai Road Hefei Anhui 230026 P. R. China State Key Laboratory of Oganometallic Chemistry Center for Excellence in Molecular Synthesis Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences 345 Lingling Road Shanghai 200032 P. R. China Frontier Science Center for Transformative Molecules School of Chemistry and Chemical Engineering Shanghai Jiao Tong University 800 Dongchuan Road Shanghai 200240 China School of Chemistry and Materials Science Hangzhou Institute for Advanced Study University of Chinese Academy of Sciences 1 Sub-lane Xiangshan Hangzhou 310024 China

Metal/ligand in situ assembly is crucial for tailoring the reactivity & selectivity in transition metal catalysis. Cooperative catalysis via a single metal/two ligands is still underdeveloped, since it is rather challenging to harness the distinct reactivity profiles of the species generated by self-assembly of a single metal precursor with a mixture of different ligands. Herein, we report a catalytic system composed of a single metal/two ligands for a three-component reaction of polyfluoroarene, α-diazo ester, and allylic electrophile, leading to highly efficient construction of densely functionalized quaternary carbon centers, that are otherwise hardly accessible. Mechanistic studies suggest this reaction follows a cooperative bimetallic pathway via two catalysts with distinct reactivity profiles, which are assembled in situ from a single metal precursor and two ligands and work in concert to escort the transformation.

关键词： Cooperative Bimetallic Catalysis Diazo Compounds Difunctionalization Metal/Ligand Assembly One-Metal/Two-Ligands

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