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Favoring CO Intermediate Stabilization and Protonation by Crown Ether for CO2Electromethanation in Acidic Media

Angewandte Chemie 2023年第50期135卷

作者： Keqiang Xu Jinhan Li Fangming Liu Xijie Chen Tete Zhao Fangyi Cheng Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Engineering Research Center on High-Efficiency Energy Storage (Ministry of Education) Renewable Energy Conversion and Storage Center College of Chemistry Nankai University Tianjin 300071 China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Visualization (lead) Writing - original draft (equal) Contribution: Data curation (supporting) Formal analysis (equal) Investigation (supporting) Methodology (equal) Software (equal) Validation (equal) Frontiers Science Center for New Organic Matter Nankai University Tianjin 300071 China Contribution: Formal analysis (equal) Funding acquisition (supporting) Methodology (equal) Project administration (lead) Validation (supporting) Writing - review & editing (lead) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Validation (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Visualization (supporting) Haihe Laboratory of Sustainable Chemical Transformations Tianjin 300192 China Contribution: Conceptualization (lead) Formal analysis (equal) Methodology (equal) Resources (lead) Supervision (lead) Writing - review & editing (equal)

The large-scale deployment of CO 2 electroreduction is hampered by deficient carbon utilization in neutral and alkaline electrolytes due to CO 2 loss into (bi)carbonates. Switching to acidic media mitigates carbonation, but suffers from low product selectivity because of hydrogen evolution. Here we report a crown ether decoration strategy on a Cu catalyst to enhance carbon utilization and selectivity of CO 2 methanation under acidic conditions. Macrocyclic 18-Crown-6 is found to enrich potassium cations near the Cu electrode surface, simultaneously enhancing the interfacial electric field to stabilize the *CO intermediate and accelerate water dissociation to boost *CO protonation. Remarkably, the mixture of 18-Crown-6 and Cu nanoparticles affords a CH 4 Faradaic efficiency of 51.2 % and a single pass carbon efficiency of 43.0 % toward CO 2 electroreduction in electrolyte with pH=2. This study provides a facile strategy to promote CH 4 selectivity and carbon utilization by modifying Cu catalysts with supramolecules.

关键词： CO2 Electroreduction Copper Catalyst Crown Ether Methanation Protonation

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Highly Selective Electrocatalytic Olefin Hydrogenation in Aqueous Solution

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Angewandte Chemie 2023年第41期135卷

作者： Chengyu Xing Prof. Yurui Xue Xuchen Zheng Dr. Yang Gao Siao Chen Prof. Yuliang Li Beijing Advanced Innovation Centre for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 P. R. China CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Methodology (lead) Validation (lead) Writing - original draft (equal) Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion Science Center for Material Creation and Energy Conversion Science School of Chemistry and Chemical Engineering Shandong University Jinan 250100 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Methodology (lead) Supervision (lead) Writing - original draft (lead) University of Chinese Academy of Sciences Beijing 100190 P. R. China Contribution: Formal analysis (lead) Methodology (lead) Contribution: Formal analysis (equal) Methodology (equal)

Selective hydrogenation of olefins with water as the hydrogen source at ambient conditions is still a big challenge in the field of catalysis. Herein, the electrocatalytic hydrogenation of purely aliphatic and functionalized olefins was achieved by using graphdiyne based copper oxide quantum dots (Cu x O/GDY) as cathodic electrodes and water as the hydrogen source, with high activity and selectivity in aqueous solution at high current density under ambient temperature and pressure. In particular, the sp-/sp 2 -hybridized graphdiyne catalyst allows the selective hydrogenation of cis-trans isomeric olefins. The chemical and electronic structure of the GDY results in the incomplete charge transfer between GDY and Cu atoms to optimize the adsorption/desorption of the reaction intermediates and results in high reaction selectivity and activity for hydrogenation reactions.

关键词： Atomic Active Sites Electrocatalysis Graphdiyne Highly Selectivity Hydrogenation

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Topic specificity: A descriptive metric for algorithm selection and finding the right number of topics

Natural Language Processing Journal

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Natural Language Processing Journal 2024年 8卷

作者： Emil Rijcken Kalliopi Zervanou Pablo Mosteiro Floortje Scheepers Marco Spruit Uzay Kaymak Jheronimus Academy of Data Science Eindhoven University of Technology ’s Hertogenbosch The Netherlands Department of Information and Computing Sciences Utrecht University Utrecht The Netherlands Department of Methodology and Statistics Utrecht University Utrecht The Netherlands Psychiatry University Medical Center Utrecht Utrecht The Netherlands Leiden Institute of Advanced Computer Science Leiden The Netherlands Public Health & Primary Care Leiden University Medical Center Leiden The Netherlands

Topic modeling is a prevalent task for discovering the latent structure of a corpus, identifying a set of topics that represent the underlying themes of the documents. Despite its popularity, issues with its evaluation metric, the coherence score, result in two common challenges: algorithm selection and determining the number of topics . To address these two issues, we propose the topic specificity metric, which captures the relative frequency of topic words in the corpus and is used as a proxy for the specificity of a word. In this work, we formulate the metric firstly. Secondly, we demonstrate that algorithms train topics at different specificity levels. This insight can be used to address algorithm selection as it allows users to distinguish and select algorithms with the desired specificity level. Lastly, we show a strictly positive monotonic correlation between the topic specificity and the number of topics for LDA, FLSA-W, NMF and LSI. This correlation can be used to address the selection of the number of topics, as it allows users to adjust the number of topics to their desired level. Moreover, our descriptive metric provides a new perspective to characterize topic models, allowing them to be understood better.

关键词： Topic modeling Metric Algorithm selection

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Iridium-Catalyzed Chemo-, Diastereo-, and Enantioselective Allyl-Allyl Coupling: Accessing All Four Stereoisomers of (E)-1-Boryl-Substituted 1,5-Dienes by Chirality Pairing

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Angewandte Chemie 2023年第13期135卷

作者： Yongsuk Jung Seok Yeol Yoo Yonghoon Jin Jaehyun You Seungcheol Han Jeongwoo Yu Prof. Dr. Yoonsu Park Prof. Dr. Seung Hwan Cho Department of Chemistry Pohang University of Science and Technology (POSTECH) Pohang 37673 (Republic of Korea Contribution: Conceptualization (supporting) Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Writing - original draft (supporting) Writing - review & editing (supporting) Department of Chemistry Korea Advanced Institute of Science and Technology (KAIST) Daejeon 34141 (Republic of Korea Contribution: Data curation (lead) Writing - original draft (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Contribution: Data curation (supporting) Contribution: Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Writing - original draft (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Project administration (lead) Writing - original draft (lead) Writing - review & editing (lead)

Here, we report a highly chemo-, diastereo-, and enantioselective allyl-allyl coupling between branched allyl alcohols and α-silyl-substituted allylboronate esters, catalyzed by a chiral iridium complex. The α-silyl-substituted allylboronate esters can be chemoselectively coupled with allyl electrophiles, affording a diverse set of enantioenriched ( E )-1-boryl-substituted 1,5-dienes in good yields, with excellent stereoselectivity. By permuting the chiral iridium catalysts and the substrates, we efficiently and selectively obtained all four stereoisomers bearing two consecutive chiral centers. Mechanistic studies via density functional theory calculations revealed the origins of the diastereo- and chemoselectivities, indicating the pivotal roles of the steric interaction, the β-silicon effect, and a rapid desilylation process. Additional synthetic modifications for preparing a variety of enantioenriched compounds containing contiguous chiral centers are also included.

关键词： Allyl-Allyl Coupling Chemoselectivity Diastereoselectivity Enantioselectivity Stereoisomers

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Configuration-Induced Multichromism of Phenanthridine Derivatives: A Type of Versatile Fluorescent Probe for Microenvironmental Monitoring

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Angewandte Chemie 2023年第9期135卷

作者： Wei Huang Dr. Shiyu Feng Jie Liu Baoshuai Liang Ya Zhou Mengya Yu Jiayuan Liang Prof. Jiaguo Huang Prof. Xujie Lü Prof. Weiguo Huang State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences 155 Yangqiao West Road Fuzhou Fujian 350002 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Investigation (lead) Methodology (lead) Validation (lead) Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou Fujian 350108 P. R. China University of Chinese Academy of Sciences 19 A Yuquan Road Beijing 100049 P. R. China Contribution: Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Investigation (lead) Methodology (lead) Validation (lead) Visualization (lead) Contribution: Data curation (equal) Formal analysis (equal) Investigation (equal) Methodology (equal) Software (equal) Validation (equal) Visualization (equal) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Validation (supporting) School of Pharmaceutical Sciences Sun Yat-sen University Guangzhou 510006 P. R. China Contribution: Data curation (supporting) Investigation (supporting) Methodology (supporting) Contribution: Data curation (supporting) Formal analysis (supporting) Investigation (supporting) Methodology (supporting) Center for High Pressure Science and Technology Advanced Research (HPSTAR) Shanghai 201203 P. R. China Contribution: Conceptualization (lead) Funding acquisition (lead) Project administration (lead) Resources (lead) Supervision (lead) Validation (lead) Writing - original draft (lead) Writing - review & editing (lead)

Fluorescent probes are attractive in diagnosis and sensing. However, most reported fluorophores can only detect one or few analytes/parameters, notably limiting their applications. Here we have designed three phenanthridine-based fluorophores (i.e., B1 , F1 , and T1 with 1D, 2D, and 3D molecular configuration, respectively) capable of monitoring various microenvironments. In rigidifying media, all fluorophores show bathochromic emissions but with different wavelength and intensity changes. Under compression, F1 shows a bathochromic emission of over 163 nm, which results in organic fluorophore-based full-color piezochromism. Moreover, both B1 and F1 exhibit an aggregation-caused quenching (ACQ) behavior, while T1 is an aggregation-induced emission (AIE) fluorophore. Further, F1 and T1 selectively concentrate in cell nucleus, whereas B1 mainly stains the cytoplasm in live cell imaging. This work provides a general design strategy of versatile fluorophores for microenvironmental monitoring.

关键词： Bioimaging Configuration-Induced Multichromism Microenvironmental Monitoring Optical Sensing Phenanthridine Derivatives

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Nano Proteolysis Targeting Chimeras (PROTACs) with Anti-Hook Effect for Tumor Therapy

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Angewandte Chemie 2023年第37期135卷

作者： Ni-Yuan Zhang Da-Yong Hou Xing-Jie Hu Jian-Xiao Liang Man-Di Wang Zhang-Zhi Song Li Yi Zhi-Jia Wang Prof. Hong-Wei An Prof. Wanhai Xu Prof. Hao Wang CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety CAS Center for Excellence in Nanoscience National Center for Nanoscience and Technology (NCNST) Beijing 100190 China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of Sciences Beijing 100049 P. R. China Contribution: Conceptualization (lead) Data curation (lead) Methodology (lead) Project administration (lead) Writing - original draft (lead) Writing - review & editing (lead) Department of Urology Harbin Medical University Cancer Hospital Heilongjiang Key Laboratory of Scientific Research in Urology Harbin 150001 China NHC Key Laboratory of Molecular Probes and Targeted Diagnosis and Therapy Harbin Medical University Harbin 150001 China Henan Institute of Advanced Technology Zhengzhou University Zhengzhou 450052 China Contribution: Data curation (equal) Investigation (equal) Methodology (equal) Supervision (equal) Contribution: Formal analysis (equal) Investigation (equal) Methodology (equal) Supervision (equal) Contribution: Formal analysis (equal) Investigation (equal) Supervision (equal) Contribution: Investigation (equal) Methodology (equal) Supervision (equal) Contribution: Data curation (equal) Formal analysis (equal) Methodology (equal) Contribution: Conceptualization (lead) Data curation (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Data curation (lead) Methodology (lead) Project administration (lead) Supervision (lead) Writing - review & editing (lead)

Proteolysis targeting chimera (PROTAC) is an emerging pharmacological modality with innovated post-translational protein degradation capabilities. However, off-target induced unintended tissue effects and intrinsic “hook effect” hinder PROTAC biotechnology to be maturely developed. Herein, an intracellular fabricated nano proteolysis targeting chimeras (Nano-PROTACs) modality with a center-spoke degradation network for achieving efficient dose-dependent protein degradation in tumor is reported. The PROTAC precursors are triggered by higher GSH concentrations inside tumor cells, which subsequently in situ self-assemble into Nano-PROTACs through intermolecular hydrogen bond interactions. The fibrous Nano-PROTACs can form effective polynary complexes and E3 ligases degradation network with multi-binding sites, achieving dose-dependent protein degradation with “anti-hook effect”. The generality and efficacy of Nano-PROTACs are validated by degrading variable protein of interest (POI) such as epidermal growth factor receptor (EGFR) and androgen receptor (AR) in a wide-range dose-dependent manner with a 95 % degradation rate and long-lasting potency up to 72 h in vitro. Significantly, Nano-PROTACs achieve in vivo dose-dependent protein degradation up to 79 % and tumor growth inhibition in A549 and LNCap xenograft mice models, respectively. Taking advantages of in situ self-assembly strategy, the Nano-PROTACs provide a generalizable platform to promote precise clinical translational application of PROTAC.

关键词： Nanomedicine PROTACs Peptide Self-Assembly Tumor

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Deploying Cationic Cellulose Nanofiber Confinement to Enable High Iodine Loadings Towards High Energy and High-Temperature Zn-I2Battery

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Angewandte Chemie 2023年第5期136卷

作者： Zhenglin Li Wenwen Cao Tao Hu Yichan Hu Rong Zhang Huilin Cui Funian Mo Chaozheng Liu Chunyi Zhi Guojin Liang Institute of Technology for Carbon Neutrality Shenzhen Institute of Advanced Technology Chinese Academy of Sciences (CAS) Shenzhen 518055 China Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of Materials Science and Engineering Nanjing Forestry University Nanjing 210000 China Contribution: Data curation (lead) Investigation (lead) Methodology (lead) Writing - original draft (lead) School of Chemistry and Chemical Engineering University of Jinan Jinan 250022 China Contribution: Conceptualization (equal) Data curation (lead) Investigation (lead) Methodology (lead) School of Materials Science and Engineering Key Laboratory of Structure and Functional Regulation of Hybrid Materials Ministry of Education Anhui University Hefei 230601 China Contribution: Data curation (equal) Formal analysis (equal) Investigation (supporting) Methodology (supporting) Contribution: Conceptualization (equal) Data curation (supporting) Formal analysis (equal) Investigation (equal) Department of Materials Science and Engineering City University of Hong Kong 83 Tat Chee Avenue Kowloon Hong Kong 999077 Hong Kong Contribution: Data curation (equal) Investigation (equal) Methodology (equal) Contribution: Conceptualization (supporting) Data curation (supporting) Formal analysis (equal) Investigation (equal) Shenzhen Key Laboratory of Flexible Printed Electronics Technology Center Harbin Institute of Technology Shenzhen Guangdong 518055 China Contribution: Conceptualization (lead) Data curation (lead) Resources (lead) Supervision (equal) Contribution: Conceptualization (equal) Data curation (lead) Investigation (lead) Supervision (equal) Contribution: Supervision (lead) Visualization (lead) Writing - review & editing (lead) Contribution: Conceptualization (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

High iodine loading and high-temperature adaptability of the iodine cathode are prerequisites to achieving high energy density at full battery level and promoting the practical application for the zinc-iodine (Zn-I 2 ) battery. However, it would aggravate the polyiodide shuttle effect when employing high iodine loading and working temperature. Here, a sustainable cationic cellulose nanofiber (cCNF) was employed to confine the active iodine species through strong physiochemical adsorption to enlarge the iodine loading and stabilize it even at high temperatures. The cCNF could accommodate dual-functionality by enlarging the iodine loading and suppressing the polyiodide shuttle effect, owing to the unique framework structure with abundant surface positive charges. As a result, the iodine cathode based on the cCNF could deliver high iodine mass loading of 14.1 mg cm −2 with a specific capacity of 182.7 mAh g −1 , high areal capacity of 2.6 mAh cm −2 , and stable cycling over 3000 cycles at 2 A g −1 , thus enabling a high energy density of 34.8 Wh kg −1 and the maximum power density of 521.2 W kg −1 at a full Zn-I 2 battery level. In addition, even at a high temperature of 60 °C, the Zn-I 2 battery could still deliver a stable cycling.

关键词： Cationic Cellulose High- Temperature Battery Iodine Shuttle-Free Zn-I2 Battery

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Organic Zinc-Ion Battery: Planar, π-Conjugated Quinone-Based Polymer Endows Ultrafast Ion Diffusion Kinetics

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Angewandte Chemie 2022年第51期134卷

作者： Dr. Fei Ye Qiang Liu Dr. Hongliang Dong Kailin Guan Zhaoyang Chen Na Ju Prof. Linfeng Hu School of Materials Science and Engineering Southeast University Nanjing 211189 China Contribution: Conceptualization (supporting) Data curation (lead) Investigation (lead) Writing - original draft (lead) Contribution: Data curation (equal) Formal analysis (equal) Software (lead) Center for High Pressure Science and Technology Advanced Research Shanghai 201203 P. R. China Contribution: Investigation (equal) Methodology (equal) Resources (equal) Validation (lead) Contribution: Formal analysis (equal) Investigation (lead) Methodology (equal) Contribution: Investigation (equal) Software (equal) Validation (lead) Visualization (lead) Contribution: Data curation (equal) Formal analysis (equal) Writing - original draft (supporting) Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Funding acquisition (lead) Project administration (lead) Supervision (lead) Writing - original draft (lead) Writing - review & editing (lead)

A novel poly(phenazine-alt-pyromellitic anhydride) (PPPA) has been successfully designed and synthesized via a condensation polymerization strategy as promising cathode material in organic zinc-ion batteries. Electrochemical quartz crystal microbalance (EQCM), FTIR and XPS characterizations verify a reversible Zn 2+ -coordination mechanism in our PPPA cathode. Intriguingly, an ultrahigh Zn 2+ diffusion coefficient of 1.2×10 −7 cm 2 s −1 was found in this large π-conjugated system, which is the highest one among all organic cathode materials for zinc-ion batteries. Theoretical calculations reveal the extended π-conjugated plane in our PPPA sample results in a significant reduction on energy gap, effectively accelerating intramolecular electron transfer during charge/discharge process. Our finding provides insights to achieve high zinc-ion transport kinetics by a design strategy on planar polymer system.

关键词： Energy Gap Linear Polymer Organic Zinc-Ion Batteries Quinone-Based Polymer Zn2+ Diffusion Coefficient

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On the Conformation of Dimeric Acceptors and Their Polymer Solar Cells with Efficiency over 18 %

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Angewandte Chemie 2023年第45期135卷

作者： Jingnan Wu Zhaoheng Ling Leandro R. Franco Sang Young Jeong Zewdneh Genene Josué Mena Si Chen Cailing Chen Prof. C. Moyses Araujo Prof. Cleber F. N. Marchiori Joost Kimpel Xiaoming Chang Furkan H. Isikgor Qiaonan Chen Hendrik Faber Prof. Yu Han Frédéric Laquai Prof. Maojie Zhang Prof. Han Young Woo Prof. Donghong Yu Prof. Thomas D. Anthopoulos Prof. Ergang Wang Department of Chemistry and Chemical Engineering Chalmers University of Technology 41296 Göteborg Sweden Department of Chemistry and Bioscience Aalborg University 9220 Aalborg Denmark Contribution: Conceptualization (lead) Data curation (lead) Formal analysis (lead) Writing - original draft (lead) Writing - review & editing (lead) King Abdullah University of Science and Technology (KAUST) KAUST Solar Center Thuwal 23955 Saudi Arabia Contribution: Data curation (lead) Formal analysis (lead) Writing - original draft (equal) Writing - review & editing (equal) Department of Engineering and Physics Karlstad University 65188 Karlstad Sweden Contribution: Data curation (equal) Writing - review & editing (equal) Department of Chemistry Korea University Seoul 02841 (Republic of Korea Contribution: Data curation (equal) Formal analysis (equal) Advanced Membranes and Porous Materials Center Physical Sciences and Engineering Division King Abdullah University of Science and Technology Thuwal 23955-6900 Saudi Arabia Contribution: Data curation (equal) Methodology (equal) Materials Theory Division Department of Physics and Astronomy Uppsala University 75120 Uppsala Sweden Contribution: Data curation (equal) Funding acquisition (equal) Software (equal) Writing - review & editing (equal) Contribution: Data curation (equal) Methodology (equal) Writing - review & editing (equal) Contribution: Data curation (equal) Writing - review & editing (supporting) Contribution: Data curation (equal) Methodology (supporting) Contribution: Data curation (equal) Contribution: Data curation (supporting) Funding acquisition (supporting) National Engineering Research Center for Colloidal Materials School of Chemistry & Chemical Engineering Shandong University Jinan Shandong 250100 China Contribution: Data curation (equal) Funding acquisition (supporting) Contribution: Data curation (equal) Funding acquisition (supporting) Writing - review & editing (supporting) Contribution: Data curation (equal) Fu

The determination of molecular conformations of oligomeric acceptors (OAs) and their impact on molecular packing are crucial for understanding the photovoltaic performance of their resulting polymer solar cells (PSCs) but have not been well studied yet. Herein, we synthesized two dimeric acceptor materials, DIBP3F-Se and DIBP3F-S, which bridged two segments of Y6-derivatives by selenophene and thiophene, respectively. Theoretical simulation and experimental 1D and 2D NMR spectroscopic studies prove that both dimers exhibit O -shaped conformations other than S - or U -shaped counter-ones. Notably, this O -shaped conformation is likely governed by a distinctive “conformational lock” mechanism, arising from the intensified intramolecular π–π interactions among their two terminal groups within the dimers. PSCs based on DIBP3F-Se deliver a maximum efficiency of 18.09 %, outperforming DIBP3F-S-based cells (16.11 %) and ranking among the highest efficiencies for OA-based PSCs. This work demonstrates a facile method to obtain OA conformations and highlights the potential of dimeric acceptors for high-performance PSCs.

关键词： Acceptor Molecular Conformation Oligomer Selenophene Solar Cells

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A Dislocated Twin-Locking Acceptor-Donor-Acceptor Configuration for Efficient Delayed Fluorescence with Multiple Through-Space Charge Transfer

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Angewandte Chemie 2022年第49期134卷

作者： Dr. Feng-Ming Xie Hao-Ze Li Kai Zhang Yang Shen Prof. Xin Zhao Prof. Yan-Qing Li Prof. Jian-Xin Tang Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices Institute of Functional Nano & Soft Materials (FUNSOM) Soochow University Suzhou Jiangsu 215123 P. R. China Contribution: Conceptualization (equal) Investigation (lead) Methodology (lead) Writing - original draft (lead) School of Physics and Electronic Science Ministry of Education Nanophotonics & Advanced Instrument Engineering Research Center East China Normal University Shanghai 200062 P. R. China Contribution: Investigation (supporting) Methodology (supporting) Macau Institute of Materials Science and Engineering (MIMSE) Faculty of Innovation Engineering Macau University of Science and Technology Taipa Macau SAR 999078 P. R. China Contribution: Formal analysis (equal) Methodology (equal) Contribution: Data curation (supporting) Formal analysis (supporting) School of Chemistry and Life Sciences Suzhou University of Science and Technology Suzhou Jiangsu 215009 P. R. China Contribution: Data curation (supporting) Methodology (supporting) Contribution: Supervision (supporting) Writing - original draft (equal) Writing - review & editing (equal) Contribution: Conceptualization (equal) Resources (lead) Supervision (lead) Writing - review & editing (lead)

Organic materials featuring intramolecular through-space charge transfer (TSCT) excited states are advantageous for efficient thermally activated delayed fluorescence (TADF), although the realization of multiple TSCT systems remains challenging. Herein, a rigid molecule with a three-dimensional dislocated sandwich acceptor-donor-acceptor configuration has been developed by a linking biphenazine (2PXZ) donor and 2,4,6-triphenyl-1,3,5-triazine (TRZ) acceptor through the twin-locking of two spiro-fluorene bridges. The twin-locking construction with multiple TSCT effects suppresses the intramolecular rotations of various segments in 2PXZ-2TRZ, leading to a small singlet-triplet energy difference, a fast reverse intersystem crossing process, and high photoluminescence quantum yield. This material simultaneously possesses the capabilities of TADF and aggregation-induced emission. The device employing 2PXZ-2TRZ as a dopant displays an optimal external quantum efficiency of 27.1 % and a low efficiency roll-off.

关键词： Multiple Through-Space Charge Transfer Organic Light-Emitting Diodes Polycyclic Aromatic Hydrocarbons Thermally Activated Delayed Fluorescence Twin-Locking Configuration

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