Angewandte Chemie最新文献_第7页

Fine-Tuned Charge Density of Pt Single-Atom Sites for Controllable Hydrodeoxygenation of Lignin 木质素可控氢脱氧Pt单原子位电荷密度的微调

Angewandte Chemie Pub Date : 2025-05-16 DOI: 10.1002/ange.202504347

Qiqi Dai, Zechuan Xu, Dr. Shibin Wang, Dr. Xu Zeng, Fan He, Prof. Fengxia Yue, Dr. Zedong Zhang, Dr. Chenliang Ye, Prof. Yu Wang, Prof. Chuanfu Liu, Peng Wang, Minjie Hou, Asso. Prof. Ge Meng, Asso. Prof. Wu Lan, Prof. Dingsheng Wang

{"title":"Fine-Tuned Charge Density of Pt Single-Atom Sites for Controllable Hydrodeoxygenation of Lignin","authors":"Qiqi Dai, Zechuan Xu, Dr. Shibin Wang, Dr. Xu Zeng, Fan He, Prof. Fengxia Yue, Dr. Zedong Zhang, Dr. Chenliang Ye, Prof. Yu Wang, Prof. Chuanfu Liu, Peng Wang, Minjie Hou, Asso. Prof. Ge Meng, Asso. Prof. Wu Lan, Prof. Dingsheng Wang","doi":"10.1002/ange.202504347","DOIUrl":"https://doi.org/10.1002/ange.202504347","url":null,"abstract":"Achieving high-selectivity conversion of lignin to value-added chemicals and biofuels remains a desirable but challenging target due to its complex structure with multiple reaction paths. Herein, we designed the robust Pt single-atom sites supported on NiAl layered double hydroxide (Pt1/NiAl-LDH) and intermetallic compound (Pt1/NiAl-IMC) with distinct local charge density for selectivity-controllable hydrodeoxygenation of lignin. The Pt1/NiAl-LDH with electron-deficient Pt sites hydrogenated 4-propylguaiacol into 4-propylcyclohexanol with 100% conversion and over 90% selectivity, while Pt1/NiAl-IMC with electron-rich Pt sites favored complete deoxygenation, yielding almost equivalent of propylcyclohexane. Similar results were achieved using lignin samples. Density functional theory calculations revealed that the deoxygenation capacity of Pt1/NiAl-IMC stems from the high electronic density of Pt single atoms, which injects electrons into the C─O bond and weakens its bonding energy. This study demonstrates that the catalytic performance of single-atom catalysts in biopolymers hydrodeoxygenation can be optimized toward different products by well-controlled electronic structures.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624825","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

A Nonfused Ring Electron Acceptor with Aggregation-Induced Emission Assistance Achieving Over 20% Efficiency in Organic Solar Cells 具有聚集诱导发射辅助的非熔合环电子受体在有机太阳能电池中实现了超过20%的效率

Angewandte Chemie Pub Date : 2025-05-16 DOI: 10.1002/ange.202506415

Kun Li, Qian Xie, Prof. Cunbin An, Jianbin Zhong, Yuan Yao, Chuangcheng Hong, Prof. Yu Chen, Prof. Hua Geng, Prof. Yishi Wu, Prof. Wei Zhang, Prof. Qing Liao, Prof. Hongbing Fu

{"title":"A Nonfused Ring Electron Acceptor with Aggregation-Induced Emission Assistance Achieving Over 20% Efficiency in Organic Solar Cells","authors":"Kun Li, Qian Xie, Prof. Cunbin An, Jianbin Zhong, Yuan Yao, Chuangcheng Hong, Prof. Yu Chen, Prof. Hua Geng, Prof. Yishi Wu, Prof. Wei Zhang, Prof. Qing Liao, Prof. Hongbing Fu","doi":"10.1002/ange.202506415","DOIUrl":"https://doi.org/10.1002/ange.202506415","url":null,"abstract":"The development of nonfused ring electron acceptors (NFREAs) with high electroluminescence quantum efficiency (EQEEL) is essential for advancing the commercialization of organic solar cells (OSCs), due to their low-cost and minimal energy losses (Eloss). However, designing such NFREAs remains a significant challenge. Herein, we present a medium-bandgap NFREA, TT-TCBr, which exhibits a high EQEEL of 1.0 × 10−3 and an excellent electron mobility of 1.5 × 10−4 cm2 V−1 s−1. Interestingly, TT-TCBr shows enhanced photoluminescence quantum yield from solution (9.24%) to film (20.7%). In OSCs, the D18:TT-TCBr-based OSC achieves a good power conversion efficiency (PCE) of 13.20% with a high open-circuit voltage of 1.09 V and a low nonradiative energy loss of 0.177 eV. Importantly, TT-TCBr shows good miscibility with L8-BO, leading to an increased exciton diffusion length and EQEEL in the L8-BO: TT-TCBr blend. When TT-TCBr is introduced as a guest molecule into the D18:L8-BO-based OSC, Eloss is reduced from 0.543 to 0.530 eV, resulting in a significantly increased PCE from 19.16% to 20.10%, which represents one of the highest PCEs reported for OSCs. This research will significantly contribute to the advancement of high-performance guest materials for the rapid development of single-junction OSCs.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624823","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

Transient Supramolecular Polymers by pH-Gated Conformational Control of a Self-Assembling Cyclodextrin ph门控自组装环糊精的瞬态超分子聚合物构象控制

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202507069

Dr. Wenting Hu, Valérian Libérioux, Dr. Julien Rossignol, Dr. Gaëlle Pembouong, Dr. Etienne Derat, Dr. Mickaël Ménand, Dr. Laurent Bouteiller, Prof. Matthieu Sollogoub

{"title":"Transient Supramolecular Polymers by pH-Gated Conformational Control of a Self-Assembling Cyclodextrin","authors":"Dr. Wenting Hu, Valérian Libérioux, Dr. Julien Rossignol, Dr. Gaëlle Pembouong, Dr. Etienne Derat, Dr. Mickaël Ménand, Dr. Laurent Bouteiller, Prof. Matthieu Sollogoub","doi":"10.1002/ange.202507069","DOIUrl":"https://doi.org/10.1002/ange.202507069","url":null,"abstract":"Linking a cyclodextrin (CD) host to a hydrophobic guest can result in two distinct conformations: an introverted form (in), in which the guest is self-included within the CD cavity, and an extraverted form (out), which enables intermolecular interactions and thus the formation of a supramolecular polymer. In this study, we demonstrate that a subtle variation of the linker enables interconversion between these two conformations, the in conformer being thermodynamically the most stable in water. At basic pH (>8) the out conformer is instantly converted into the in. In contrast, at acidic pH (<2), the out monomer can be kinetically trapped and can self-assemble into a supramolecular polymer. DFT calculations reveal that the interconversion mechanism is governed by a key hydrogen bond that locks the conformational states. Furthermore, we show that pH provides fine kinetic control over the interconversion rate and, consequently, the polymerization process. The system can then be reset toward the out conformation by using DMSO. This system stands in contrast to known transient supramolecular polymerization processes, which rely on metastable (non-assembled) monomers. Here, it is the kinetic trapping of the assembling monomer that allows control over the lifetime of the transient supramolecular polymer via a pH-responsive mechanism.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202507069","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624838","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

Defect-Driven Stepwise Activation of Metal–Organic Frameworks Toward Industrial-Level Anion Exchange Membrane Water Electrolysis 缺陷驱动的金属-有机框架在工业阴离子交换膜水电解中的逐步活化

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202503787

Jian Zhou, Shuai Qiu, Xianbiao Hou, Tengjia Ni, Canhui Zhang, Dr. Shuixing Dai, Dr. Xingkun Wang, Dr. Guanghui Wang, Dr. Heqing Jiang, Dr. Minghua Huang

{"title":"Defect-Driven Stepwise Activation of Metal–Organic Frameworks Toward Industrial-Level Anion Exchange Membrane Water Electrolysis","authors":"Jian Zhou, Shuai Qiu, Xianbiao Hou, Tengjia Ni, Canhui Zhang, Dr. Shuixing Dai, Dr. Xingkun Wang, Dr. Guanghui Wang, Dr. Heqing Jiang, Dr. Minghua Huang","doi":"10.1002/ange.202503787","DOIUrl":"https://doi.org/10.1002/ange.202503787","url":null,"abstract":"Metal-organic frameworks (MOFs), featuring well-defined metal active sites and unique coordination environment, have recently emerged as ideal model catalysts for establishing precise structure-activity relationships in oxygen evolution reaction (OER). However, elucidating essential catalytic mechanisms responsible for dynamic reaction conditions remain challenging, primarily due to the complicated adsorption behavior and cross-step transfer of key adsorbates during OER. Herein, we propose a defect-driven stepwise activation strategy to meticulously control the adsorption behavior for defective Co-based MOF (termed D/CoFc-MOF) through tailoring the interplay between local coordination geometry and electronic configuration. Operando characterizations reveal that D/CoFc-MOF undergoes a unique stepwise activation during OER, progressing from pristine MOF state to intermediate α-FeOOH state, and ultimately to active CoFeOOH phase, which markedly differs from conventional single-step surface phase conversion. Theoretical calculations demonstrate that the electronic interaction between the active Co sites and OOH* intermediates of MOF-derived defective CoFeOOH can be effectively strengthened, thereby overcoming the high reaction barrier and enhancing OER activity. The D/CoFc-MOF anode, deployed in anion exchange membrane water electrolysis, achieves industrial-scale current densities of 1 A cm−2 at 1.69 V and operates stably for 300 h. This approach provides a fundamental insight into designing catalysts prone to dynamic phase transitions.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624872","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

Outside Back Cover: Benzotrifuran-based Covalent Organic Frameworks for Artificial Photosynthesis of H2O2 from H2O, O2 and Sunlight (Angew. Chem. 27/2025) 外封底：基于苯三氟醚的H2O2人工光合作用的共价有机框架（英文）化学27/2025)

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202510011

Zhenwei Zhang, Yuxin Hou, Shanshan Zhu, Liuliu Yang, Yinghui Wang, Huijuan Yue, Hong Xia, Gang Wu, Shuo-Wang Yang, Xiaoming Liu

引用次数: 0

Ammonia Hydration in a Cu(II)-Pyrazolate Framework for Efficient Trace Capture 氨水合Cu(II)-吡唑酸酯框架高效痕量捕获

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202507356

Dr. Guang-Rui Si, Dr. Xiang-Jing Kong, Prof. Tao He, Jia-Teng Zhao, Prof. Lin-Hua Xie, Prof. Jian-Rong Li

{"title":"Ammonia Hydration in a Cu(II)-Pyrazolate Framework for Efficient Trace Capture","authors":"Dr. Guang-Rui Si, Dr. Xiang-Jing Kong, Prof. Tao He, Jia-Teng Zhao, Prof. Lin-Hua Xie, Prof. Jian-Rong Li","doi":"10.1002/ange.202507356","DOIUrl":"https://doi.org/10.1002/ange.202507356","url":null,"abstract":"Ammonia (NH3) emissions from industrial and agricultural activities pose severe environmental and health issues. Trace NH3 capture typically relies on chemisorption at Lewis acid sites or physisorption on porous adsorbents but usually suffers from irreversible binding, energy-intensive regeneration, and structural degradation. In this work, for the first time, we demonstrate a new hydration pathway as a promising solution. In a Cu(II)-pyrazolate framework, BUT-64(H2O), the bridging water molecules between adjacent Cu(II) ions serve as Brønsted acid sites to hydrate ammonia, achieving a remarkable NH3 packing density of 0.27 g cm−3 at 0.1 kPa and an adsorption capacity of 1.51 mmol g−1 for 1000 ppm NH3 under 80% relative humidity, among the leading adsorbents. The reversible hydration mechanism combines enhanced NH3 affinity with facile regeneration and mitigated moisture co-adsorption, overcoming the inherent trade-off. The remarkable alkaline stability of this material also highlights its potential as an energy-efficient sorbent for trace NH3 capture.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624839","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

Outside Front Cover: Biomimetic Hierarchical Construction of Anti-Tumor Polyoxopalladates for Cancer Therapy (Angew. Chem. 23/2025) 外封面：用于癌症治疗的抗肿瘤多氧藻酸盐的仿生分层结构。化学23/2025)

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202510019

Yue Zhao, Zheran Liu, Zijian Qin, Qinlong Wen, Jing Du, Xiang-Yu Ren, Chao-Qin Chen, Xingchen Peng, Ulrich Kortz, Peng Yang

引用次数: 0

Highly Efficient Circularly Polarized Luminescence Based on Center-Chiral Frustrated Lewis Pairs 基于中心-手性受挫刘易斯对的高效圆偏振发光

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202504057

Fan Zheng, Xiao-Long Liu, Longjiang Xing, Jia-Ming Jin, Prof. Shaomin Ji, Prof. Yanping Huo, Prof. Wen-Cheng Chen

{"title":"Highly Efficient Circularly Polarized Luminescence Based on Center-Chiral Frustrated Lewis Pairs","authors":"Fan Zheng, Xiao-Long Liu, Longjiang Xing, Jia-Ming Jin, Prof. Shaomin Ji, Prof. Yanping Huo, Prof. Wen-Cheng Chen","doi":"10.1002/ange.202504057","DOIUrl":"https://doi.org/10.1002/ange.202504057","url":null,"abstract":"Achieving high-efficiency circularly polarized luminescence (CPL) in organic light-emitting diodes (OLEDs) presents a significant challenge, particularly for center-chiral systems, due to the inherent trade-off between high luminescence efficiency and large luminescence dissymmetry factors. In this work, we introduce a center-chiral frustrated Lewis pair (FLP) design to overcome this limitation. By integrating a stereogenic carbon center into a fluorene scaffold, we create a unique interaction between a boron-based multi-resonance (MR) thermally activated delayed fluorescence (TADF) Lewis acid and an arylamine Lewis base. This sterically hindered design prevents strong charge transfer while optimizing the alignment between electric and magnetic dipole moments for amplified CPL signals. Our OLEDs achieve impressive electroluminescence (EL) dissymmetry factors (|gEL|) of 6.64 × 10−3, external quantum efficiencies (EQEs) of up to 30.4%, and sub-30 nm spectral linewidths. These improvements yield a Figure of Merit (FoM = EQE × |gEL|) of 1.91 × 10−3, the highest reported for center-chiral CPL devices. These findings demonstrate the effectiveness of the center-chiral FLP design in overcoming the long-standing trade-off between polarization and efficiency in CPL devices.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624840","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

Peter A. Korevaar Peter A. Korevaar

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202509726

Peter A. Korevaar

引用次数: 0

Molecular Ordering in Low-Dimensional Hybrid Perovskites for Improved X-Ray Detection 用于改进x射线探测的低维杂化钙钛矿分子排序

Angewandte Chemie Pub Date : 2025-05-15 DOI: 10.1002/ange.202506973

Sihan Zeng, Xinyuan Sui, Dr. Da Liu, Dr. Yu Peng, Dr. Qing Li, Mengyao Song, Junjie Qian, Dr. Haiyang Yuan, Prof. Dr. Shuang Yang, Prof. Dr. Hua Gui Yang, Prof. Dr. Yu Hou

{"title":"Molecular Ordering in Low-Dimensional Hybrid Perovskites for Improved X-Ray Detection","authors":"Sihan Zeng, Xinyuan Sui, Dr. Da Liu, Dr. Yu Peng, Dr. Qing Li, Mengyao Song, Junjie Qian, Dr. Haiyang Yuan, Prof. Dr. Shuang Yang, Prof. Dr. Hua Gui Yang, Prof. Dr. Yu Hou","doi":"10.1002/ange.202506973","DOIUrl":"https://doi.org/10.1002/ange.202506973","url":null,"abstract":"Low-dimensional hybrid perovskites are emerging semiconductors with excellent photophysical property, chemical stability, and structural diversity and have shown prominence in the fields of solar cells, light-emitting diodes, and X-ray detectors. To date, the inorganic framework structure in perovskites has been intensively studied, but the molecular arrangement of organic counterparts and its impact on physical properties remains largely unexplored. Herein, we engineer the coordination geometry of inorganic and organic building units to implement molecular ordering and π–π stacking in low-dimensional perovskites. We observe a positive dependence of carrier transport capacity and environmental stability on the molecular regularity in hybrid perovskites. Furthermore, 5-aminoquinoline lead iodide single crystal with the highest regularity exhibit nearly 5-fold increased carrier mobility-lifetime product and 20-fold decreased ionic conductivity along [011] than [100] orientation, enabling a high sensitivity of 8.25 × 105 µC Gyair−1 cm−2 under 8 keV X-ray radiation for radiation detection application. This work sheds light on the design and synthesis of next-generation perovskite-based semiconductors with enhanced performance and stability for optoelectronic applications.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 29","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-05-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144624837","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