Angewandte Chemie最新文献_第3页

Streamlined One-Step Dimerization of Small-Molecule Acceptors for High-Performance Organic Solar Cells 高效能有机太阳能电池中小分子受体的流线型一步二聚化

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-08-19 DOI: 10.1002/ange.1114374

Chen Zhang, Jiali Song, Haisheng Ma, Jiawei Deng, Cen Zhang, Jingyi Kong, Guangkuo Dai, Xuelin Wang, Min Gyu Kang, Zheng Tang, Han Young Woo, Yanming Sun

{"title":"Streamlined One-Step Dimerization of Small-Molecule Acceptors for High-Performance Organic Solar Cells","authors":"Chen Zhang, Jiali Song, Haisheng Ma, Jiawei Deng, Cen Zhang, Jingyi Kong, Guangkuo Dai, Xuelin Wang, Min Gyu Kang, Zheng Tang, Han Young Woo, Yanming Sun","doi":"10.1002/ange.1114374","DOIUrl":"https://doi.org/10.1002/ange.1114374","url":null,"abstract":"<div>\u0000 \u0000 Achieving both high power conversion efficiency (PCE) and long-term operational stability remains a formidable challenge for organic solar cells (OSCs). Dimeric small-molecule acceptors (DSMAs), constructed by linking small-molecule acceptor (SMA) subunits, have recently emerged as promising candidates. However, their conventional synthesis via Stille coupling necessitates multistep reactions, rendering large-scale, low-cost preparation impractical. Herein, we report a streamlined direct dimerization strategy that efficiently constructs core-linked DSMAs through the condensation of bromoacetyl groups with diamine subunits, obviating the need for expensive palladium catalysts and toxic organotin reagents. By systematically varying the linking units, we synthesized a series of DSMAs with precisely tunable optical and electronic properties, demonstrating the generality of the approach. Such a direct dimerization approach effectively resolves the long-standing trade-off between cost-effective synthesis and high photovoltaic performance. Consequently, the best-performing device delivers a record-high PCE of 20.15%, while maintaining outstanding photostability. Collectively, this work provides a versatile blueprint for the cost-effective synthesis of stable, high-performance DSMAs, effectively bridging the gap between molecular design and practical OSC scalability.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 42","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149163257","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

Inside Front Cover: In Silico to In Cerebro—Development of the Orexin Receptor Antagonist “Photorexant” for Photomodulation In Vitro and in Mouse Brains (Angew. Chem. 42/2026) 内页封面：从硅到脑——食欲素受体拮抗剂“光致光剂”在体外和小鼠大脑中用于光调节的发展（新）。化学42/2026)

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-09-21 DOI: 10.1002/ange.2026-m1709014100

Marcus Angermann, Marie H. Deventer, Vicente Ledesma-Martin, Nuno Filipe RodriguesMartinho, Alix Flake, Silvia Mori, Angel Nuñez, Jaime Pignatelli, Rita C. Guedes, Christophe P. Stove, Michael Decker

引用次数: 0

Directional Second Sphere Effect on CO2 Activation and Reduction by Iron Porphyrin in Aprotic and Protic Media 铁卟啉在非质子和质子介质中活化和还原CO2的定向第二球效应

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-07-23 DOI: 10.1002/ange.1490828

Ashutosh Vishwakarma, Sami Essid, Sarah Bouery, Régis Guillot, Bernard Boitrel, Philipp Gotico, Marie Sircoglou, Zakaria Halime

{"title":"Directional Second Sphere Effect on CO2 Activation and Reduction by Iron Porphyrin in Aprotic and Protic Media","authors":"Ashutosh Vishwakarma, Sami Essid, Sarah Bouery, Régis Guillot, Bernard Boitrel, Philipp Gotico, Marie Sircoglou, Zakaria Halime","doi":"10.1002/ange.1490828","DOIUrl":"https://doi.org/10.1002/ange.1490828","url":null,"abstract":"The topological directionality of functional groups in the secondary coordination sphere (SCS) plays a decisive role in enzymatic small-molecule activation but remains underexplored in synthetic systems. Here, we investigate how symmetry remodeling of a urea-based SCS modulates electrocatalytic CO2-to-CO reduction using two atropisomeric iron porphyrins, αβαβ-UrFe and α2β2-UrFe, which differ solely in the spatial arrangement of identical hydrogen-bond donor groups. Switching from a face-to-face to an adjacent urea-arms configuration enables unprecedented CO2-to-CO conversion under strictly aprotic conditions, in the absence of Brønsted or Lewis acids. Combined electrochemical, spectroscopic, kinetic, and DFT studies reveal that the adjacent positioning of the urea arms weakens the stabilization of the initial [Fe─CO2] intermediate but creates a more open and dynamically reorganizable SCS that permits insertion of a second CO2 molecule as an oxygen-atom acceptor, to yield CO and CO32ˉ. Under protic conditions, this improved active-site accessibility, combined with a dissymmetrization of the activated CO2 molecule, accelerates proton transfer, with CO2-to-CO reduction reaching turnover frequency of up to 2.72 × 107 s−1, among the highest reported for homogeneous catalysis. These results establish directional interactions within the SCS as powerful design strategy for boosting molecular catalysis.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 42","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.1490828","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149163279","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

Flavin Catalysts in Organic Synthesis 有机合成中的黄素催化剂

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-07-16 DOI: 10.1002/ange.6683110

Jan Freudenberg, Golo Storch

{"title":"Flavin Catalysts in Organic Synthesis","authors":"Jan Freudenberg, Golo Storch","doi":"10.1002/ange.6683110","DOIUrl":"https://doi.org/10.1002/ange.6683110","url":null,"abstract":"Flavin cofactors are nature's all-rounders with several essential roles in the active site of flavin-dependent enzymes. These flavoenzymes display an astonishingly broad activity spectrum, which also translates to the organic laboratory. In synthetic chemistry, flavin catalysis is now an integral part of several organocatalytic and photochemical methods with applications ranging from total synthesis to biocompatible photoproximity labeling. Flavins take a unique position in the field: they are easily accessible through synthesis or biochemical methods, while additionally exhibiting orthogonal reactivity compared to other (organo-)catalysts. Several flavin-mediated organic reactions were developed in a biomimetic fashion guided by extensive literature on enzymatic mechanisms. Additionally, flavin modification to tailored catalysts enabled desired non-natural transformations. This minireview gives an overview of and highlights the different key chemical transformations achieved with flavin catalysis in synthetic organic chemistry with a focus on photochemical oxidation and reduction, sensitization, oxygenation, and the activation of substrates by reversible covalent bond formation. The individual requirements for achieving specific flavin reactivity are illustrated based on example reactions. Finally, remaining challenges in the field of flavin catalysis are identified.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 42","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.6683110","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149163181","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

Rhenium-Based β-Galactosidase Probe Allows Senescence Profiling by Mass Cytometry 基于铼的β-半乳糖苷酶探针允许通过细胞计数法进行衰老分析

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-08-17 DOI: 10.1002/ange.5043520

Adam Tam, Kris Elbein, Aleida G. Gonzalez, Edgar A. Arriaga, Mark Nitz

{"title":"Rhenium-Based β-Galactosidase Probe Allows Senescence Profiling by Mass Cytometry","authors":"Adam Tam, Kris Elbein, Aleida G. Gonzalez, Edgar A. Arriaga, Mark Nitz","doi":"10.1002/ange.5043520","DOIUrl":"https://doi.org/10.1002/ange.5043520","url":null,"abstract":"Mass cytometry is an attractive analytical technique for the study of cellular senescence due to its ability to simultaneously interrogate the multiple biomarkers necessary to define senescent phenotypes. However, measuring senescence-associated β-Galactosidase (SA-β-Gal) activity, the gold standard biomarker for detection of senescent cells, requires a functional mass cytometry detectable probe compatible with an antibody-based panel. Herein, we report a small-molecule mass cytometry probe for SA-β-Gal, ReGal, that uses a piano-stool rhenium complex as a mass tag. We demonstrate that the probe measures β-Gal activity in vitro and in cellulo with minimal background signal. We further show that the probe improves the discrimination of senescence-induced mouse embryonic fibroblasts (MEFs) against untreated cells compared to using only antibody-based mass cytometry reagents. Finally, we demonstrate that the probe reveals a putatively senescent sub-population of mouse peripheral blood mononuclear cells (PBMCs), which is enriched in old vs. young mice, that could not be segmented by antibody-based reagents alone.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 42","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.5043520","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149163239","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

Inside Back Cover: Flavin Catalysts in Organic Synthesis (Angew. Chem. 42/2026) 内页后盖：有机合成中的黄素催化剂（新）。化学42/2026)

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-09-21 DOI: 10.1002/ange.2026-m1709012500

Jan Freudenberg, Golo Storch

引用次数: 0

Bright Ideas From Biology Transforming Synthesis: 59th Bürgenstock Conference 第59届生物转化合成大会

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-09-10 DOI: 10.1002/ange.8298635

Daniele Mazzarella, Jola Pospech

引用次数: 0

Tailoring Crystallization Modulators for the Facile Synthesis of One-Dimensional Covalent Organic Frameworks to Boost Ultrasound-Triggered Pyroptosis and Immunotherapy 为一维共价有机框架的简易合成量身定制结晶调节剂，以促进超声触发的焦亡和免疫治疗

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-08-19 DOI: 10.1002/ange.5056685

Jiwei Wang, Sainan Liu, Zhendong Liu, Jing Li, Di Han, Xinyu Ma, Yarui Hu, Binbin Ding, Kai Li, Yunling Liu, Ping'an Ma, Jun Lin

{"title":"Tailoring Crystallization Modulators for the Facile Synthesis of One-Dimensional Covalent Organic Frameworks to Boost Ultrasound-Triggered Pyroptosis and Immunotherapy","authors":"Jiwei Wang, Sainan Liu, Zhendong Liu, Jing Li, Di Han, Xinyu Ma, Yarui Hu, Binbin Ding, Kai Li, Yunling Liu, Ping'an Ma, Jun Lin","doi":"10.1002/ange.5056685","DOIUrl":"https://doi.org/10.1002/ange.5056685","url":null,"abstract":"<div>\u0000 \u0000 Ultrasound (US)-induced tumor cell pyroptosis holds great potential for cancer immunotherapy; however, its efficacy is often constrained by the inadequate reactive oxygen species (ROS) generation of conventional sonosensitizers. Herein, one-dimensional porphyrin-based covalent organic frameworks (designated as TD-aniline and TD-FeCl3) with well-defined structures were constructed under mild conditions via a novel synthesis strategy that employed aniline or FeCl3 as crystallization modulators, thereby achieving efficient ROS generation and controllable activation of tumor cell pyroptosis. Notably, FeCl3 not only promoted the ordered assembly of TD-FeCl3 but also introduced metal sites via coordination with porphyrin cores, resulting in superior sonodynamic performance compared to TD-aniline. Specifically, metal coordination in TD-FeCl3 reduced its band gap to promote electron-hole pair (e−–h+) generation under ultrasound. Meanwhile, the introduced Fe3+ diminished spatial e−–h+ overlap in the excited state, thereby suppressing charge recombination, and ultimately channeling more excited-state energy into a synergistic enhancement of superoxide anion and singlet oxygen production. Moreover, US irradiation enhanced the Fenton-like activity of TD-FeCl3. Based on its superior ROS generation capacity, TD-FeCl3 effectively promoted US-triggered pyroptosis in tumor cells, leading to robust antitumor immune responses. This work establishes a novel paradigm for the controlled synthesis of one-dimensional COFs and opens new avenues for pyroptosis-based immunotherapy.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 42","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149163258","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

Implanted Zn2+-Conducting Hydrogel Interphase Enables Highly Compacted Thick Iodine Electrodes for Ah-Level Aqueous Zinc–Iodine Pouch Batteries 植入的Zn2+导电水凝胶间相使高压实的厚碘电极用于ah级水锌-碘袋电池

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-08-19 DOI: 10.1002/ange.6865881

Huadong Jiang, Chenxi Sun, Hong Lin, Minghao Zhang, Fanxiang Meng, Jinbao Zhao, Yang Yang

{"title":"Implanted Zn2+-Conducting Hydrogel Interphase Enables Highly Compacted Thick Iodine Electrodes for Ah-Level Aqueous Zinc–Iodine Pouch Batteries","authors":"Huadong Jiang, Chenxi Sun, Hong Lin, Minghao Zhang, Fanxiang Meng, Jinbao Zhao, Yang Yang","doi":"10.1002/ange.6865881","DOIUrl":"https://doi.org/10.1002/ange.6865881","url":null,"abstract":"<div>\u0000 \u0000 Increasing the compaction density of dry-processed thick iodine cathodes is essential for enhancing energy density, yet remains hindered by sluggish reaction kinetics and aggravated polyiodide shuttling. Herein, we report an implanted Zn2+-conducting (PAMPS-Zn, poly(zinc 2-acrylamido-2-methylpropane sulfonate)) hydrogel interphase via in situ ultraviolet-induced polymerization, which enables local Zn2+ buffering, enhanced Zn2+ transport, and suppression of polyiodide migration in highly compacted dry-processed iodine cathodes. Abundant sulfonate groups in polymeric chains serve as immobilized anionic sites that coordinate Zn2+ and provide a local Zn2+ reservoir, which mitigates interfacial Zn2+ depletion. Meanwhile, the interconnected Zn2+-conducting hydrogel network facilitates Zn2+ transport through the thick electrode, reducing reliance on conventional electrolyte-permeation-mediated ion transport in dry-processed electrodes, which is intrinsically limited by the hydrophobic nature of the PTFE binder and high ionic tortuosity. Importantly, the negatively charged, water-regulated hydrogel interphase also suppresses polyiodide diffusion through electrostatic repulsion and reduced water-driven dissolution. Consequently, under high compaction conditions (∼0.5 g cm−3), Zn–I2 batteries incorporating PAMPS-Zn interphase achieve a high areal capacity of 9.6 mAh cm−2 at 0.5 C and an ultralong lifespan exceeding 4400 cycles at 5 C. Notably, Ah-level Zn-I2 pouch cells (∼1.2 Ah) achieve stable operation for 850 cycles, providing compelling proof-of-concept validation of this strategy.\u0000 </div>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"138 42","pages":""},"PeriodicalIF":0.0,"publicationDate":"2026-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"149163263","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

Jose B. Roque 何塞·b·罗克

Angewandte Chemie Pub Date : 2026-10-10 Epub Date: 2026-08-27 DOI: 10.1002/ange.3972904

Jose B. Roque

引用次数: 0