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Design of Multi-Shelled Hollow Cr2O3Spheres for Metabolic Fingerprinting

Angewandte Chemie 2021年第22期133卷

作者： Rongxin Li Dr. Yongjie Zhou Dr. Chao Liu Congcong Pei Weikang Shu Chaoqi Zhang Prof. Lianzhong Liu Prof. Liang Zhou Prof. Jingjing Wan School of Chemistry and Molecular Engineering East China Normal University Shanghai 200241 P. R. China Department of Psychiatric Rehabilitation Shenzhen Kangning Hospital Shenzhen Guangdong 518118 P. R. China Wuhan Mental Health Center Tongji Medical College of Huazhong University of Science and Technology Wuhan Hubei 430032 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China

Schizophrenia (SZ) detection enables effective treatment to improve the clinical outcome, but objective and reliable SZ diagnostics are still limited. An ideal diagnosis of SZ suited for robust clinical screening must address detection throughput, low invasiveness, and diagnosis accuracy. Herein, we built a multi-shelled hollow Cr 2 O 3 spheres (MHCSs) assisted laser desorption/ionization mass spectrometry (LDI MS) platform for the direct metabolic profiling of biofluids towards SZ diagnostics. The MHCSs displayed strong light absorption for enhanced ionization and microscale surface roughness with stability for the effective LDI of metabolites. We profiled urine and serum metabolites (≈1 μL) with the enhanced LDI efficacy in seconds. We discriminated SZ patients (SZs) from healthy controls (HCs) with the highest area under the curve (AUC) value of 1.000 for the blind test. We identified four compounds with optimal diagnostic power as a simplified metabolite panel for SZ and demonstrated the metabolite quantification for clinic use. Our approach accelerates the growth of new platforms toward a precision diagnosis in the near future.

关键词： in vitro diagnostics (IVD) mass spectrometry metabolites multi-shelled hollow spheres schizophrenia

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Dynamic Restructuring of Coordinatively Unsaturated Copper Paddle Wheel Clusters to Boost Electrochemical CO2Reduction to Hydrocarbons**

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Angewandte Chemie 2021年第3期134卷

作者： Dr. Wei Zhang Chuqiang Huang Jiexin Zhu Qiancheng Zhou Ruohan Yu Yali Wang Dr. Pengfei An Prof. Jing Zhang Prof. Ming Qiu Prof. Liang Zhou Prof. Liqiang Mai Prof. Zhiguo Yi Prof. Ying Yu Institute of Nanoscience and Nanotechnology College of Physical Science and Technology Central China Normal University Wuhan 430079 Hubei P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 Hubei P. R. China Beijing Synchrotron Radiation Facility Institute of High Energy Physics Chinese Academy of Science Beijing 100049 P. R. China State Key Laboratory of High Performance Ceramics and Superfine Microstructure Shanghai Institute of Ceramics Chinese Academy of Sciences Shanghai 200050 P. R. China

The electrochemical reduction of CO 2 to hydrocarbons involves a multistep proton-coupled electron transfer (PCET) reaction. Second coordination sphere engineering is reported to be effective in the PCET process; however, little is known about the actual catalytic active sites under realistic operating conditions. We have designed a defect-containing metal–organic framework, HKUST-1, through a facile “atomized trimesic acid” strategy, in which Cu atoms are modified by unsaturated carboxylate ligands, producing coordinatively unsaturated Cu paddle wheel (CU−CPW) clusters. We investigate the dynamic behavior of the CU−CPW during electrochemical reconstruction through the comprehensive analysis of in situ characterization results. It is demonstrated that Cu 2 (HCOO) 3 is maintained after electrochemical reconstruction and that is behaves as an active site. Mechanistic studies reveal that CU−CPW accelerates the proton-coupled multi-electron transfer (PCMET) reaction, resulting in a deep CO 2 reduction reaction.

关键词： catalytic active sites CO2 reduction Cu paddle wheel electrocatalysts

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NH4+Deprotonation at Interfaces Induced Reversible H3O+/NH4+Co-insertion/Extraction

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Angewandte Chemie 2023年第14期135卷

作者： Meng Huang Qiu He Junjun Wang Xiong Liu Fangyu Xiong Yu Liu Ruiting Guo Yan Zhao Jinlong Yang Liqiang Mai Guangdong Research Center for Interfacial Engineering of Functional Materials College of Materials Science and Engineering Shenzhen University Shenzhen 518060 China College of Physics and Optoelectronic Engineering Shenzhen University Shenzhen 518060 China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China College of Materials Science and Engineering Sichuan University Chengdu 610065 China School of Materials Science and Engineering Zhengzhou University Zhengzhou 450001 China Department of Physics City University of Hong Kong Tat Chee Avenue Kowloon 999077 Hong Kong China Department of Materials Science and Engineering National University of Singapore Singapore 117574 Singapore The Institute of Technological Sciences Wuhan University Hubei Wuhan 430072 China

Ion insertions always involve electrode-electrolyte interface process, desolvation for instance, which determines the electrochemical kinetics. However, it′s still a challenge to achieve fast ion insertion and investigate ion transformation at interface. Herein, the interface deprotonation of NH 4 + and the introduced dissociation of H 2 O molecules to provide sufficient H 3 O + to insert into materials′ structure for fast energy storages are revealed. Lewis acidic ion-NH 4 + can, on one hand provide H 3 O + itself via deprotonation, and on the other hand hydrolyze with H 2 O molecules to produce H 3 O + . In situ attenuated total reflection-Fourier transform infrared ray method probed the interface accumulation and deprotonation of NH 4 + , and density functional theory calculations manifested that NH 4 + tend to thermodynamically adsorb on the surface of monoclinic VO 2 , and deprotonate to provide H 3 O + . In addition, the inserted NH 4 + has a positive effect for stabilizing the VO 2 (B) structure. Therefore, high specific capacity (>300 mAh g −1 ) and fast ionic insertion/extraction (<20 s) can be realized in VO 2 (B) anode. This interface derivation proposes a new path for designing proton ion insertion/extraction in mild electrolyte.

关键词： Electrode-Electrolyte Interface Energy Storage Mechanism Proton Insertion Vanadium Dioxide In Situ Characterization

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Dual-Anionic Coordination Manipulation Induces Phosphorus and Boron-Rich Gradient Interphase Towards Stable and Safe Sodium Metal Batteries

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Angewandte Chemie 2024年第3期137卷

作者： Yi-Hu Feng Dr. Mengting Liu Wenli Qi Haoliang Liu Qiang Liu Dr. Chao Yang Yongwei Tang Xu Zhu Shuai Sun Yuan-Meng Li Tian-Ling Chen Bing Xiao Prof. Xiao Ji Prof. Ya You Prof. Peng-Fei Wang Center of Nanomaterials for Renewable Energy State Key Laboratory of Electrical Insulation and Power Equipment School of Electrical Engineering Xi'an Jiaotong University Xi'an Shaanxi 710049 P. R. China School of Optical and Electronic Information-Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan Hubei 430074 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan Hubei 430070 P. R. China Jiangsu Jufeng New Energy Technology Co. Ltd. Changzhou Jiangsu 213166 P. R. China

High-voltage sodium metal batteries (SMBs) present a viable pathway towards high-energy-density sodium-based batteries due to the competitive cost advantage and abundant supply of sodium resources. However, they still suffer from severe capacity decay induced by the notorious decomposition of the electrolyte under high voltage and unstable cathode/electrolyte interphase (CEI). In addition, the high reactivity of Na metal and flammable electrolytes push SMBs to their safety limits. Herein, a special dual-anion aggregated Na + solvation structure is designed in a nonflammable trimethyl phosphate-based localized high-concentration electrolyte, and a gradient CEI enriched with phosphorus and boron compounds is formed on the cathode. This thin and stable interphase effectively suppresses the parasitic reaction, improves the interfacial stability of the cathode, and facilitates Na + transport through the interface by the synergistic effect of multi-components, thus optimizing the cycling stability and safety of SMBs. The Na 0.95 Ni 0.4 Fe 0.15 Mn 0.3 Ti 0.15 O 2 //Na batteries employing such electrolyte provide a discharge capacity of 167.5 mAh g −1 and high retention in the capacity of 85.2 % after 800 cycles at 1 C. This approach offers a general strategy for the design of flame-retardant high-voltage electrolytes and the practical application of SMBs.

关键词： sodium metal batteries electrolyte non-flammable cathode/electrolyte interphase solvation structure

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Selective CO2Reduction to Ethylene Mediated by Adaptive Small-molecule Engineering of Copper-based Electrocatalysts

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Angewandte Chemie 2023年第50期135卷

作者： Dr. Shenghua Chen Dr. Chengliang Ye Dr. Ziwei Wang Dr. Peng Li Dr. Wenjun Jiang Dr. Zechao Zhuang Dr. Jiexin Zhu Dr. Xiaobo Zheng Dr. Shahid Zaman Dr. Honghui Ou Lei Lv Dr. Lin Tan Dr. Yaqiong Su Dr. Jiang Ouyang Prof. Dingsheng Wang National Innovation Platform (Center) for Industry-Education Integration of Energy Storage Technology School of Chemical Engineering and Technology Xi'an Jiaotong University Xi'an 710049 P. R. China Engineering Research Center of Advanced Rare Earth Materials Department of Chemistry Tsinghua University Beijing 100084 P. R. China School of Chemistry Xi'an Key Laboratory of Sustainable Energy Materials Chemistry State Key Laboratory of Electrical Insulation and Power Equipment Engineering Research Center of Energy Storage Materials and Devices Ministry of Education Xi'an Jiaotong University Xi'an 710049 P. R. China Qian Xuesen Laboratory of Space Technology China Academy of Space Technology Beijing 100094 P. R. China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing International School of Materials Science and Engineering Wuhan University of Technology Wuhan 430070 P. R China Key Laboratory of Energy Conversion and Storage Technologies Department of Mechanical and Energy Engineering Southern University of Science and Technology Shenzhen 518055 P. R. China School of Biomedical Engineering Guangzhou Medical University Guangzhou 511436 P. R. China

Electrochemical CO 2 reduction reaction (CO 2 RR) over Cu catalysts exhibits enormous potential for efficiently converting CO 2 to ethylene (C 2 H 4 ). However, achieving high C 2 H 4 selectivity remains a considerable challenge due to the propensity of Cu catalysts to undergo structural reconstruction during CO 2 RR. Herein, we report an in situ molecule modification strategy that involves tannic acid (TA) molecules adaptive regulating the reconstruction of a Cu-based material to a pathway that facilitates CO 2 reduction to C 2 H 4 products. An excellent Faraday efficiency (FE) of 63.6 % on C 2 H 4 with a current density of 497.2 mA cm −2 in flow cell was achieved, about 6.5 times higher than the pristine Cu catalyst which mainly produce CH 4 . The in situ X-ray absorption spectroscopy and Raman studies reveal that the hydroxyl group in TA stabilizes Cu δ+ during the CO 2 RR. Furthermore, theoretical calculations demonstrate that the Cu δ+ /Cu 0 interfaces lower the activation energy barrier for *CO dimerization, and hydroxyl species stabilize the *COH intermediate via hydrogen bonding, thereby promoting C 2 H 4 production. Such molecule engineering modulated electronic structure provides a promising strategy to achieve highly selective CO 2 reduction to value-added chemicals.

关键词： C2H4 CO2RR Cuδ+/Cu0 Hydrogen Bonding TA Molecule

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New Opportunities and Challenges of Smart Polymers in Post-Translational Modification Proteomics

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advanced materials (Deerfield Beach, Fla.) 2017年第20期29卷 2017 May;29(20)页

作者： Guangyan Qing Qi Lu Yuting Xiong Lei Zhang Hongxi Wang Xiuling Li Xinmiao Liang Taolei Sun State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China. Institute of Biomedical and Pharmaceutical Sciences College of Bioengineering Hubei University of Technology 28 Nanli Road Wuhan 430068 P. R. China. Key Laboratory of Separation Science for Analytical Chemistry Dalian Institute of Chemical Physics Chinese Academy of Sciences 457 Zhongshan Road Dalian 116023 P. R. China. International School of Materials Science and Engineering Wuhan University of Technology 122 Luoshi Road Wuhan 430070 P. R. China.

Protein post-translational modifications (PTMs), which denote covalent additions of various functional groups (e.g., phosphate, glycan, methyl, or ubiquitin) to proteins, significantly increase protein complexity and diversity. PTMs play crucial roles in the regulation of protein functions and numerous cellular processes. However, in a living organism, native PTM proteins are typically present at substoichiometric levels, considerably impeding mass-spectrometry-based analyses and identification. Over the past decade, the demand for in-depth PTM proteomics studies has spawned a variety of selective affinity materials capable of capturing trace amounts of PTM peptides from highly complex biosamples. However, novel design ideas or strategies are urgently required for fulfilling the increasingly complex and accurate requirements of PTM proteomics analysis, which can hardly be met by using conventional enrichment materials. Considering two typical types of protein PTMs, phosphorylation and glycosylation, an overview of polymeric enrichment materials is provided here, with an emphasis on the superiority of smart-polymer-based materials that can function in intelligent modes. Moreover, some smart separation materials are introduced to demonstrate the enticing prospects and the challenges of smart polymers applied in PTM proteomics.

关键词： enrichment interfaces post-translational modification proteomics smart polymers

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A facile spray-pressing synthesis approach for reusable photothermal masks

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iScience 2023年第8期26卷 107286页

作者： Yi Lu Yi-Xuan Liu Yong Wang Robert Oestreich Zi-Yan Xu Wen Zhang Philipp Hügenell Christoph Janiak Xiao-Yu Yang Hoffmann Institute of Advanced Materials Shenzhen Polytechnic 7098 Liuxian Boulevard Nanshan District Shenzhen 518055 China. Institut für Anorganische Chemie und Strukturchemie Heinrich-Heine-Universität Düsseldorf Universitätsstraße 1 40225 Düsseldorf Germany. School of Chemical Engineering and Technology Sun Yat-sen University Zhuhai 519082 China. State Key Laboratory of Advanced Technology for Materials Synthesis and Processing & Shenzhen Research Institute Wuhan University of Technology Wuhan 430070 China. Division Thermal Systems and Buildings Fraunhofer Institute for Solar Energy Systems ISE Heidenhofstraße 2 Freiburg 79110 Germany.

Certain types of face masks are highly efficient in protecting humans from bacterial and viral pathogens, and growing concerns with high safety, low cost, and wide market suitability have accelerated the replacement of reusable face masks with disposable ones during the last decades. However, wearing these masks creates countless problems associated with personnel comfort as well as more significant issues related to the cost of fabrication, the generation of medical waste, and environmental contaminants. In this work, we present a facile spray-pressing technique for the production of P-masks with a potential scale-up prospect by adding a graphene layer on one side of meltblown fabric and a functional layer on the other side. In principle, this technique could be easily integrated into the present automatic mask production process and the masks have self-cleaning and/or self-sterilizing properties when it is exposed to solar or simulated solar irradiation.

关键词： Applied sciences materials synthesis Nanotechnology fabrication

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bFGF and Poly‐RGD Cooperatively Establish Biointerface for Stem Cell Adhesion, Proliferation, and Differentiation

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advanced materials Interfaces 2018年第7期5卷

作者： Nan Jiang Yong Wang Yi‐Xia Yin Rui‐Peng Wei Guo‐Liang Ying Bin‐Bin Li Tong Qiu Patrick van Rijn Ge Tian Qiong‐Jiao Yan Hong‐Lian Dai Henk J. Busscher Shi‐Pu Li Ali K. Yetisen Xiao‐Yu Yang State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology Wuhan 430070 China School of Engineering and Applied Sciences Harvard University Cambridge MA 02138 USA Brigham and Women's Hospital Harvard Medical School Cambridge MA 02139 USA School of Materials Science and Engineering Wuhan Institute of Technology Wuhan 430205 China Department of Biomedical Engineering‐FB4 University of Groningen/University Medical Center Groningen Ant. Deusinglaan 1 9713 AV Groningen The Netherlands School of Chemical Engineering University of Birmingham Edgbaston Birmingham B15 2TT UK

Biointerface design is widely used to functionalize biomaterials with controllable physicochemical properties. Functionalized biointerface provides a versatile platform to connect biological entities and nonbiogenic materials. Existing nanofabrication approaches to create such a nanostructured biointerface involve in low stability of the functionalized nanolayer and simple functionalities that limit its applicability. Here, a stable nanolayered synthetic polypeptide (poly[LA‐ co ‐(Glc‐alt‐Lys)] and modified with arginine‐glycine‐aspartic acid, PRGD)/basic fibroblast growth factor (bFGF) biointerface is created via structural matching, charge interaction, and hydrogen bonding. The cooperative effect of the PRGD/bFGF biointerface shows multiple functionalities in promoting stem cell adhesion by 33% increase in cell adhesion to poly( d,l ‐lactic acid) substrate as compared to experiments on bare substrate as a control. Moreover, the biointerface enhances proliferation by 40% in cell density, potential differentiation by 62%, and gene expression by 40 and 80% respectively as compared to the control samples. The fabricated biointerface may have applications in nerve regeneration, tissue repair, and stem cell‐based therapy.

关键词： biointerface cell proliferation cooperative effect growth factors stem cell differentiation

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3D Ferroconcrete‐Like Aminated Carbon Nanotubes Network Anchoring Sulfur for advanced Lithium–Sulfur Battery

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advanced Energy materials 2018年第25期8卷

作者： Min Yan Hao Chen Yong Yu Heng Zhao Chao‐Fan Li Zhi‐Yi Hu Pan Wu Lihua Chen Hongen Wang Dongliang Peng Huanxin Gao Tawfique Hasan Yu Li Bao‐Lian Su State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of Technology 122 Luoshi Road 430070 Wuhan Hubei China Department of Materials Science and Engineering College of Materials Xiamen University 422 Siming South Road Xiamen 361005 China Fundamental Research Department SINOPEC Shanghai Research Institute of Petrochemical Technology 165 Pudong Bei Road Shanghai 201208 China Cambridge Graphene Centre University of Cambridge 9 JJ Thomson Avenue Cambridge CB3 0FA UK Laboratory of Inorganic Materials Chemistry (CMI) University of Namur 61 rue de Bruxelles B‐5000 Namur Belgium Clare Hall University of Cambridge Herschel Road Cambridge CB3 9AL UK

To address the serious capacity fading in lithium–sulfur batteries, a 3D ferroconcrete‐like aminated carbon nanotubes network with polyaniline coating as an effective sulfur host to contain polysulfide dissolution is presented here. In this composite, the cross‐linked aminated carbon nanotubes framework provides a fast charge transport pathway and enhancement in the reaction kinetics of the active material to greatly improve the rate capability and sulfur utilization. The ethylenediamine moieties provide strong adhesion of polar discharge products to nonpolar carbon surfaces and thus efficiently prevent polysulfide dissolution to improve the cycle stability, confirmed by density functional theory calculations. The outside polyaniline layers structurally restrain polysulfides to prevent the shuttle effect and active material loss. Benefiting from these advantages, the synthesized composite exhibits a high initial capacity of 1215 mAh g −1 and a capacity of 975 mAh g −1 after 200 cycles at 0.2 C. Even after 200 cycles at 0.5 C, a capacity of 735 mAh g −1 can be maintained, among the best performance reported. The strategy in this work can shed some light on modifying nonpolar carbon surfaces via the amination process to chemically attach sulfur species for high‐performance lithium–sulfur batteries.

关键词： carbon nanotubes density functional theory ethylenediamine modification Li–S battery polyaniline

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Precise Control of Selenium Functionalization in Non-Fullerene Acceptors Enabling High-Efficiency Organic Solar Cells

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Angewandte Chemie 2022年第46期134卷

作者： Dr. Jianquan Zhang Siwei Luo Heng Zhao Xiaoyun Xu Xinhui Zou Ao Shang Jiaen Liang Dr. Fujin Bai Dr. Yuzhong Chen Prof. Kam Sing Wong Prof. Zaifei Ma Prof. Wei Ma Prof. Huawei Hu Prof. Yiwang Chen Prof. He Yan State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and Engineering Donghua University Shanghai 201620 China Department of Chemistry Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials Energy Institute and Hong Kong Branch of Chinese National Engineering Research Center for Tissue Restoration and Reconstruction Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong 999077 China State Key Laboratory for Mechanical Behavior of Materials Xi'an Jiaotong University Xi'an 710049 Shannxi Province China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials Center for Advanced Low-dimension Materials College of Materials Science and Engineering Donghua University Shanghai 201620 China Department of Physics Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong 999077 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 China College of Chemistry/Institute of Polymers and Energy Chemistry (IPEC) Nanchang University 999 Xuefu Avenue Nanchang 330031 Jiangxi Province China Institute of Polymer Optoelectronic Materials and Devices State Key Laboratory of Luminescent Materials and Devices South China University of Technology Guangzhou 510640 Guangdong Province China

Central π-core engineering of non-fullerene small molecule acceptors (NF-SMAs) is effective in boosting the performance of organic solar cells (OSCs). Especially, selenium (Se) functionalization of NF-SMAs is considered a promising strategy but the structure-performance relationship remains unclear. Here, we synthesize two isomeric alkylphenyl-substituted selenopheno[3,2-b]thiophene-based NF-SMAs named mPh4F-TS and mPh4F-ST with different substitution positions, and contrast them with the thieno[3,2-b]thiophene-based analogue, mPh4F-TT. When placing Se atoms at the outer positions of the π-core, mPh4F-TS shows the most red-shifted absorption and compact molecular stacking. The PM6 : mPh4F-TS devices exhibit excellent absorption, high charge carrier mobility, and reduced energy loss. Consequently, PM6 : mPh4F-TS achieves more balanced photovoltaic parameters and yields an efficiency of 18.05 %, which highlights that precisely manipulating selenium functionalization is a practicable way toward high-efficiency OSCs.

关键词： Acceptor Core Engineering Non-Fullerene Selenium functionalization Solar Cell

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