Angewandte Chemie最新文献_第8页

Decavanadate-Catalyzed Oxidative Cross-Dehydrogenative Coupling: an Efficient and Sustainable Approach toward P(O)─S Bond Formation 十碳酸盐催化氧化交叉脱氢偶联：一种高效、可持续的P(O)─S键形成方法

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202507245

Dr. Jian Lei, Zhenliang Yu, Dr. Shi Ru, Dr. Zixiu Wang, Shan Li, Dr. Nianhua Luo, Dr. Jiuzhong Huang, Dr. Xiaopeng Peng, Prof. Feng Jiang, Prof. Yongge Wei

引用次数: 0

Crystallization of L-Cysteine in Heavy Water Induces Intrinsic Fluorescence l -半胱氨酸在重水中的结晶诱导本征荧光

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202505331

Debarshi Banerjee, Sonika Chibh, Om Shanker Tiwari, Gonzalo Díaz Mirón, Marta Monti, Hadar R. Yakir, Shweta Pawar, Dror Fixler, Linda J. W. Shimon, Ehud Gazit, Ali Hassanali

{"title":"Crystallization of L-Cysteine in Heavy Water Induces Intrinsic Fluorescence","authors":"Debarshi Banerjee, Sonika Chibh, Om Shanker Tiwari, Gonzalo Díaz Mirón, Marta Monti, Hadar R. Yakir, Shweta Pawar, Dror Fixler, Linda J. W. Shimon, Ehud Gazit, Ali Hassanali","doi":"10.1002/ange.202505331","DOIUrl":"https://doi.org/10.1002/ange.202505331","url":null,"abstract":"Developing noninvasive techniques that can probe how solvents modulate the nucleation pathways of bioorganic molecules in solution remains an active and open area of research. Herein, we investigate the crystallization of the amino acid L-Cysteine and show that both the structure of the crystal and its intrinsic fluorescence can be drastically altered by the solvent. Crystals formed in heavy water exhibit markedly different intermolecular packing as well as strikingly different monomer conformations compared to those in light water. Remarkably, these differences in the supramolecular packing result in significantly elevated intrinsic fluorescence in the crystal that is formed in heavy water. Using a combination of experimental techniques and advanced electronic structure approaches, we elucidate the molecular interactions within the crystals that govern both the electronic origins and the intensity of their emission. These findings demonstrate how tuning the solvent by changing its isotope leads to the emergence of design principles for new intrinsic fluorophores that could serve as novel sensing probes for biomedical applications.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202505331","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624637","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Hydroenergy Inspiring Large-Scale Piezoelectric Catalysis for Seawater Hydrogen Evolution 水能激发大规模压电催化海水析氢

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202504749

Dr. Wenyuan Liu, Dr. Shu Zhu, Dr. Maoxi Ran, Zhihao Fu, Mengke Zhang, Prof. Dr. Yayun Zhang, Prof. Dr. Hualin Wang, Prof. Dr. Mingyang Xing, Prof. Dr. Pengbo Fu

{"title":"Hydroenergy Inspiring Large-Scale Piezoelectric Catalysis for Seawater Hydrogen Evolution","authors":"Dr. Wenyuan Liu, Dr. Shu Zhu, Dr. Maoxi Ran, Zhihao Fu, Mengke Zhang, Prof. Dr. Yayun Zhang, Prof. Dr. Hualin Wang, Prof. Dr. Mingyang Xing, Prof. Dr. Pengbo Fu","doi":"10.1002/ange.202504749","DOIUrl":"https://doi.org/10.1002/ange.202504749","url":null,"abstract":"The piezoelectric effect presents a promising avenue for harvesting and utilizing low-grade mechanical energy. However, challenges from lacking matched industrial equipment and maintaining catalytic performance during scaling up impede the engineering of piezo-catalysis. Here, utilizing mechanical energy of water to inspire piezoelectricity, a successful attempt at large-scale piezo-catalysis seawater H2 evolution was reported for the first time, exhibiting an efficiency of 36.82% for converting mechanical energy to hydrogen energy. A scaling-up test with 20 L of seawater was conducted, yielding an H2 production rate of 0.73 L h−1, which just occupied 0.7 m2. This performance (1.04 L h−1 m−2) exceeds the large-scale photocatalytic pure water H2 production by panel reactor array (0.18∼0.25 L h−1 m−2) reported in 2021. Additionally, the H2 evolution activity of the 20 L system showed no obvious decline compared with the 50 mL system before scaling-up, owing to the utilization of ternary piezo-catalysts system, which capitalized on the synergistic coupling effect of kinetics and thermodynamics. This attempt provides a prototype for pursuing large-scale piezo-catalysis and practical engineering application.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624636","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Epitaxially Grown Lattice-Coherent Surface Enabling Superior Mechanical Integrity for High-Voltage LiCoO2 Cathode 外延生长的晶格相干表面使高压LiCoO2阴极具有优异的机械完整性

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202504221

Xiang Li, Kexin Wang, Miao Tian, Xu Zhang, Xingyang Wu, Haotian Song, Shuo-Wang Yang, Junwei Zheng, Fanghui Du, Jing Lyu, Zhongkai Hao, Guo Qin Xu

{"title":"Epitaxially Grown Lattice-Coherent Surface Enabling Superior Mechanical Integrity for High-Voltage LiCoO2 Cathode","authors":"Xiang Li, Kexin Wang, Miao Tian, Xu Zhang, Xingyang Wu, Haotian Song, Shuo-Wang Yang, Junwei Zheng, Fanghui Du, Jing Lyu, Zhongkai Hao, Guo Qin Xu","doi":"10.1002/ange.202504221","DOIUrl":"https://doi.org/10.1002/ange.202504221","url":null,"abstract":"The growing demand for high-energy-density cathode is pushing LiCoO2 towards 4.6 V operation. However, the structural and interfacial instability of high-voltage LiCoO2 is exacerbated when the charging cut-off voltage exceeds 4.55 V, resulting in severe mechanical failure and subsequent dramatic capacity decay. Herein, through thermally driven element interdiffusion, a highly durable Co-containing Li-rich phase with the lattice coherence has been epitaxially grown along LiCoO2 surface, which enhances the intrinsic mechanical integrity of high-voltage LiCoO2. Through establishing the lattice-coherent Li-rich surface, adverse side reactions, irreversible phase transition and lattice oxygen loss are significantly inhibited in high-voltage LiCoO2, thereby alleviating cracks formation and maintaining the structural integrity. The presence of the Li-rich phase endows LiCoO2 with the additional capacity and the excellent cycling stability at 4.6 V and even at 4.7 V. This work taps into a new avenue of surface engineering on high-voltage LiCoO2.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624530","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Surface Work Function-Induced High-Entropy Solid Electrolyte Interphase Formation for Highly Stable Potassium Metal Anodes 高稳定金属钾阳极表面功函数诱导的高熵固体电解质界面形成

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202509252

Dr. Lili Song, Qiaoxi Yang, Dr. Yu Yao, Mengran Tan, Renke Li, Dr. Jiaying Liao, Prof. Xiaosi Zhou, Prof. Yan Yu

{"title":"Surface Work Function-Induced High-Entropy Solid Electrolyte Interphase Formation for Highly Stable Potassium Metal Anodes","authors":"Dr. Lili Song, Qiaoxi Yang, Dr. Yu Yao, Mengran Tan, Renke Li, Dr. Jiaying Liao, Prof. Xiaosi Zhou, Prof. Yan Yu","doi":"10.1002/ange.202509252","DOIUrl":"https://doi.org/10.1002/ange.202509252","url":null,"abstract":"The failure of the solid electrolyte interphase (SEI) layer is a key issue limiting the practical application of potassium metal batteries. Herein, a novel high-entropy SEI layer rich in inorganic components is designed and constructed via in situ electrochemical conversion of the Sn3O4/Sn2S3 interfacial layer on a porous scaffold. Theoretical studies and experimental techniques reveal that the Sn3O4/Sn2S3 heterostructure, with its low work function and weak Sn─O/S bond, significantly enhances reactivity with the electrolyte, thereby facilitating the in situ formation of the high-entropy SEI layer. The in situ generated high-entropy SEI exhibits low surface roughness, low surface potential, fast potassium ion transport characteristics, and excellent mechanical properties (Young's modulus of 20.08 GPa). Leveraging these advantageous properties of the high-entropy SEI, the resulting potassium metal anode achieves an excellent rate performance up to 10 mA cm−2 in symmetric cells and demonstrates outstanding cycling stability for 2500 h at 0.5 mA cm−2. When paired with a perylene-3,4,9,10-tetracarboxylic dianhydride cathode, the potassium metal full battery retains 81.6% of its capacity over 1650 cycles at 10 C. This work underscores a straightforward and effective approach for the establishment of a stable interphase on metallic potassium anodes.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Exploring the Interplay of Lattice Dynamics and Charge Transport in Organic Semiconductors: Progress Toward Rational Phonon Engineering 探索有机半导体中晶格动力学与电荷输运的相互作用：理性声子工程的进展

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202507566

Barbara M. T. C. Peluzo, Rahul Meena, Luca Catalano, Guillaume Schweicher, Michael T. Ruggiero

{"title":"Exploring the Interplay of Lattice Dynamics and Charge Transport in Organic Semiconductors: Progress Toward Rational Phonon Engineering","authors":"Barbara M. T. C. Peluzo, Rahul Meena, Luca Catalano, Guillaume Schweicher, Michael T. Ruggiero","doi":"10.1002/ange.202507566","DOIUrl":"https://doi.org/10.1002/ange.202507566","url":null,"abstract":"Organic semiconductors (OSCs) have garnered significant attention due to their potential use in flexible, lightweight, and cost-effective electronic devices. Despite their promise, the assembly of organic molecules into the condensed phase promotes a diverse set of lattice dynamics that introduce a detrimental modulation in the intermolecular electronic structure—termed dynamic disorder—that results in charge carrier mobilities that are orders of magnitude lower than inorganic semiconductors. This dynamic disorder is generally associated with low-frequency phonons, yet whether a small subset of modes or a broad range of phonons drives dynamic disorder remains contested. Resolving this debate is critical for defining how targeted phonon engineering could practically improve OSC performance. In this review, we explore progress toward uncovering the interplay between lattice dynamics and charge transport in OSCs, focusing on the critical role of thermally activated phonons. We describe the powerful insight that mode-resolved analyses of electron–phonon interactions lends toward the rational design of new materials. We highlight recent efforts to achieve this, showcasing proposed strategies to mitigate dynamic disorder through molecular and crystal design. This work offers an overview of the insight gained toward understanding the fundamental mechanisms governing charge transport in OSCs and outlines pathways for enhancing performance via targeted manipulation of interatomic/intermolecular interactions and resulting phonon modes.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 26","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202507566","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144339305","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Phase Engineering for Achieving Full-Color Tunable Emission from Blue to Red and Multi-Level Information Security in Isomeric Hybrid Copper Halides 实现从蓝到红全彩色可调发射的相位工程和异构杂化卤化铜的多层次信息安全

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202506748

Dr. Jiajing Wu, Qiao-Feng Huang, Yi-Fan Fu, Jing-Li Qi, Li-Xiang Chen, Shu-Fang Yan, Prof. Wenlong Liu, Prof. Sheng-Ping Guo

{"title":"Phase Engineering for Achieving Full-Color Tunable Emission from Blue to Red and Multi-Level Information Security in Isomeric Hybrid Copper Halides","authors":"Dr. Jiajing Wu, Qiao-Feng Huang, Yi-Fan Fu, Jing-Li Qi, Li-Xiang Chen, Shu-Fang Yan, Prof. Wenlong Liu, Prof. Sheng-Ping Guo","doi":"10.1002/ange.202506748","DOIUrl":"https://doi.org/10.1002/ange.202506748","url":null,"abstract":"The design and synthesis of novel hybrid metal halides polymorphs with full-color tunable emission are critical for the advancement of solid-state lighting and display technologies. However, it remains challenging and rarely reported. Herein, we successfully synthesized three new zero-dimensional (0D) hybrid isomeric copper (I) halides, namely α-/β-/γ-(BuPh3P)2Cu2I4 (where BuPh3P+ = butyltriphenylphosphonium, C22H24P+), featuring the same edge-sharing [Cu2I4]2− units. Notably, the monoclinic α-(BuPh3P)2Cu2I4 and β-(BuPh3P)2Cu2I4, both belonging to the P21/n space group, exhibit bright blue and orange emission, respectively. The orthorhombic-phase γ-(BuPh3P)2Cu2I4 with space group Pbca and larger lattice volume shows vivid red emission, thus achieving tunable full-color emission wavelength spanning from blue (445 nm) to red (667 nm), representing the first instance of such broad tunability through adjusting the spatial arrangement of the organic and inorganic parts. Interestingly, α-(BuPh3P)2Cu2I4 undergoes a reversible photo-induced fluorochromism, transitioning from blue to green. Furthermore, a reversible phase transformation between α- and β-(BuPh3P)2Cu2I4 can be triggered by dichloromethane and ethyl acetate. As such, a photo-responsive switchable system and a multistage information encryption/decryption system are successfully devised through leveraging unique multi-stimuli-responsive properties.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624479","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dual-Interface Nanopipette Sensor for Electrochemical Interferent Shielding 电化学干扰屏蔽双界面纳米吸管传感器

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202504520

Si-Yu Tian, Rui-Xue Gao, Zi-Qiang Du, Yu-Ting Qi, Ying Chen, Prof. Dr. Fan Xia, Prof. Dr. Xin-Wei Zhang, Prof. Dr. Wei-Hua Huang

{"title":"Dual-Interface Nanopipette Sensor for Electrochemical Interferent Shielding","authors":"Si-Yu Tian, Rui-Xue Gao, Zi-Qiang Du, Yu-Ting Qi, Ying Chen, Prof. Dr. Fan Xia, Prof. Dr. Xin-Wei Zhang, Prof. Dr. Wei-Hua Huang","doi":"10.1002/ange.202504520","DOIUrl":"https://doi.org/10.1002/ange.202504520","url":null,"abstract":"Enzyme-based sensors have been widely utilized for their superior selectivity. However, they cannot distinguish the same kind of redox mediators from different sources. Typically, both the H2O2 produced in glucose (analyte) oxidation by glucose oxidase (GOD) and the endogenous H2O2 (interferent) existing in the detection system can be simultaneously measured, causing inaccurate results in glucose detection. To address this long-standing and inevitable obstacle, we proposed a new sensor design strategy, a dual-interface nanopipette sensor (DINS), to shield against the interferent electrochemically. The DINS comprised an anti-interference interface at the orifice of the nanopipette, and a sensing interface located at the inner wall with a certain distance from the orifice. Anti-interference interface, functioning as an “electrochemical Faraday cage”, electrochemically eliminated the interferents with high efficiency while allowed the target species to pass through and be detected at the sensing interface. With the synergy of these two independent interfaces, the GOD-modified DINS (GOD-DINS) allowed the accurate detection of intracellular glucose with effectively eliminating endogenous H2O2, facilitating the quantitative study on the glucose metabolism inside single cells. Furthermore, this DINS configuration is expected to accurately quantify more substances, and reveal complex crosstalk interactions between multiple species in the physiological, pathological and pharmacological research.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Cooperative Photometallobiocatalysis: Nonheme Fe Enzyme-Catalyzed Enantioconvergent Radical Decarboxylative Azidation, Thiocyanation, and Isocyanation of Redox-Active Esters 协同光金属生物催化：非血红素铁酶催化的对映收敛自由基脱羧叠氮化、硫氰化和氧化还原活性酯的异氰化

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202506361

Liu-Peng Zhao, Ken Lin, Pei-Pei Xie, Huichong Liu, Hengye Xiang, Xin Liu, Yunlong Zhao, Peng Liu, Yang Yang

{"title":"Cooperative Photometallobiocatalysis: Nonheme Fe Enzyme-Catalyzed Enantioconvergent Radical Decarboxylative Azidation, Thiocyanation, and Isocyanation of Redox-Active Esters","authors":"Liu-Peng Zhao, Ken Lin, Pei-Pei Xie, Huichong Liu, Hengye Xiang, Xin Liu, Yunlong Zhao, Peng Liu, Yang Yang","doi":"10.1002/ange.202506361","DOIUrl":"https://doi.org/10.1002/ange.202506361","url":null,"abstract":"Cooperative catalysis with an enzyme and a small-molecule photocatalyst has recently emerged as a potentially general activation mode to advance novel biocatalytic reactions with synthetic utility. Herein, we report cooperative photobiocatalysis involving an engineered nonheme Fe enzyme and a tailored photoredox catalyst to achieve enantioconvergent decarboxylative azidation, thiocyanation, and isocyanation of redox-active esters via a radical mechanism. We repurposed and further evolved metapyrocatechase (MPC), a nonheme Fe extradiol dioxygenase not previously studied in new-to-nature biocatalysis, for the enantioselective C─N3, C─SCN, and C─NCO bond formation via an enzymatic Fe─X intermediate (X═N3, NCS, and NCO). A range of primary, secondary, and tertiary alkyl radical precursors were effectively converted by our engineered MPC, allowing the syntheses of organic azides, thiocyanates, and isocyanates with good to excellent enantiocontrol. Further derivatization of these products furnished valuable compounds including enantioenriched amines, triazoles, ureas, and SCF3-containing products. DFT and MD simulations shed light on the mechanism as well as the binding poses of the alkyl radical intermediate in the enzyme active site and the π-facial selectivity in the enantiodetermining radical rebound. Overall, cooperative photometallobiocatalysis with nonheme Fe enzymes provides a means to develop challenging asymmetric radical transformations eluding small-molecule catalysis.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202506361","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624529","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Asymmetric B←N Functionalized Benzothiadiazoles for High-Performance n-Type Semiconducting Polymers 不对称B←N功能化苯并噻二唑高性能N型半导体聚合物

Angewandte Chemie Pub Date : 2025-05-14 DOI: 10.1002/ange.202507528

Kewei Jiao, Dr. Wei Song, Dr. Di Liu, Zhen Jiang, Dongsheng Yan, Zhiwei Zhao, Prof. Dr. Ziyi Ge, Prof. Dr. Yunqi Liu, Prof. Dr. Yang Wang

{"title":"Asymmetric B←N Functionalized Benzothiadiazoles for High-Performance n-Type Semiconducting Polymers","authors":"Kewei Jiao, Dr. Wei Song, Dr. Di Liu, Zhen Jiang, Dongsheng Yan, Zhiwei Zhao, Prof. Dr. Ziyi Ge, Prof. Dr. Yunqi Liu, Prof. Dr. Yang Wang","doi":"10.1002/ange.202507528","DOIUrl":"https://doi.org/10.1002/ange.202507528","url":null,"abstract":"B←N containing polymers have emerged in organic electronics due to their fascinating optical and electronic properties. Despite these advantages, the development of B←N-based n-type polymers for high-performance organic transistors remains a significant challenge, primarily due to the scarcity of effective B←N containing acceptor units. In this work, we address this challenge through the rational design and synthesis of two asymmetric half-fused B←N functionalized benzothiadiazole derivatives, BTBN and FBTBN. These compounds leverage the unique electronic properties of the B←N motif, enabling the development of two new n-type polymers, PBTBN and PFBTBN. Notably, the lowest unoccupied molecular orbital (LUMO) levels of PBTBN and PFBTBN are significantly lowered by 0.2–0.3 eV compared to their counterparts without B←N functionalization, with PFBTBN achieving a LUMO of ∼ −4.0 eV. Importantly, PFBTBN exhibits exceptional unipolar n-type transistor performance with a high electron mobility (µe) of 3.85 cm2 V−1 s−1. The asymmetric half-fused B←N molecular backbone not only stabilizes the electronic structure but also induces a near-amorphous morphology, thereby enabling PFBTBN-based flexible transistors to retain a high µe of 3.16 cm2 V−1 s−1 even after 1000 bending cycles. This work demonstrates the transformative potential of incorporating asymmetric B←N functionalized acceptors for high-performance n-type semiconducting polymers.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0