Angewandte Chemie (International ed. in English)最新文献_第3页

Conformation-Locking in Thiazole-Rich Mixed-Linkage Covalent Organic Frameworks for Spontaneous Exciton Dissociation and Efficient Photocatalysis. 富噻唑混合键共价有机框架中自发激子解离和高效光催化的构象锁定。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-08-29 DOI: 10.1002/anie.4914496

Liujun Yang, Xu Zhang, Chenfan Xie, Long Zhang, Jiangyue Wang, Qiang Cao, Junwei Yuan, Chen Yu, Liren Gu, Zhigang Ren, Hua Li, Jianmei Lu

{"title":"Conformation-Locking in Thiazole-Rich Mixed-Linkage Covalent Organic Frameworks for Spontaneous Exciton Dissociation and Efficient Photocatalysis.","authors":"Liujun Yang, Xu Zhang, Chenfan Xie, Long Zhang, Jiangyue Wang, Qiang Cao, Junwei Yuan, Chen Yu, Liren Gu, Zhigang Ren, Hua Li, Jianmei Lu","doi":"10.1002/anie.4914496","DOIUrl":"10.1002/anie.4914496","url":null,"abstract":"The formidable exciton effect inherent in organic semiconductors fundamentally restricts free charge carrier generation, thereby impeding photocatalytic redox efficiency. Facilitating spontaneous exciton dissociation and lowering exciton binding energy are essential for maximizing charge utilization. Herein, we report a conformation-locking strategy to engineer a thiazole-rich mixed-linkage donor-acceptor conjugated covalent organic framework (SBt-Tapt) via post-synthetic cyclization. The seamless integration of sulfur heteroatoms into a rigid, thiazole-bridged framework significantly enhances π-conjugated and electronic polarizability. Crucially, this structural reinforcement lowers the exciton activation energy below to 25 meV, triggering spontaneous exciton dissociation, extending carrier lifetimes, and yielding a proliferation of free charge carriers at room temperature. Mechanistic insights elucidate that the thiazole moieties synergistically activate adjacent phenyl units for O2 reduction while simultaneously lowering the energy barrier for H2O oxidation at benzothiophene sites. This dual-pathway mechanism drives efficient H2O2 photosynthesis with robust operational stability exceeding 100 h. Notably, utilizing phenolic pollutants as proton donors, SBt-Tapt delivers an exceptional H2O2 evolution rate of 8.99 mmol gcat -1 h-1 alongside effective pollutant mineralization. This study elucidates a profound structure-activity relationship (SAR) and establishes conformation locking as a potent excitonic engineering paradigm for developing high performance organic photocatalysts.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e4914496"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148852218","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 Regulation of Crystallization via Volatile Additives to Obtain High-Quality Perovskite Films. 挥发性添加剂对高质量钙钛矿薄膜结晶的瞬态调控。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-09-02 DOI: 10.1002/anie.7089275

Aiqing Sun, Wangda Li, Changshan Bu, Yang Huang, Li-Min Liu, Linhua Hu

{"title":"Transient Regulation of Crystallization via Volatile Additives to Obtain High-Quality Perovskite Films.","authors":"Aiqing Sun, Wangda Li, Changshan Bu, Yang Huang, Li-Min Liu, Linhua Hu","doi":"10.1002/anie.7089275","DOIUrl":"10.1002/anie.7089275","url":null,"abstract":"Exact regulation of nucleation and crystallization kinetics is essential for fabricating high-performance perovskite solar cells (PSCs). However, regulating the fast assembly of precursors without incorporating residual impurities presents a significant difficulty. We present an approach of a \"transient kinetic modulation\" strategy employing octafluorotoluene (OCF) to control the crystallization of formamidinium (FA)-based perovskites. Distinct from conventional additives that focus on cations or lead centers, OCF utilizes its electron-deficient perfluorinated aromatic ring to form robust anion-π interactions with iodide ions (I-). This interaction effectively sequesters iodide species in the precursor solution, kinetically inhibiting the formation of PbI3 - intermediates and reducing the disordered precipitation of phases. The resultant delayed nucleation and synchronized crystal growth provide perovskite films characterized by markedly increased grain size, alleviated lattice strain, and reduced defect density. Significantly, OCF totally volatilizes during annealing, guaranteeing a pure, residue-free film. Consequently, the optimized devices achieve a champion power conversion efficiency (PCE) of 25.44% with a high fill factor of 85.27%, alongside exceptional long-term stability, retaining 93% of the initial PCE after 1800 h of ambient aging. This study establishes volatile additive modulation as an effective, non-invasive method for crystallization management.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e7089275"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877230","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

Symmetry Reconstruction Breaks the Trade-Off Between Spectral Redshift and Broadening in Long-Wavelength Multiple Resonance Emitters. 对称重构打破了长波多共振发射体中光谱红移与展宽之间的权衡。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-09-04 DOI: 10.1002/anie.2435246

Yue Zhang, Panpan Ling, Yu Liu, Chenglong Li, Yincai Xu

{"title":"Symmetry Reconstruction Breaks the Trade-Off Between Spectral Redshift and Broadening in Long-Wavelength Multiple Resonance Emitters.","authors":"Yue Zhang, Panpan Ling, Yu Liu, Chenglong Li, Yincai Xu","doi":"10.1002/anie.2435246","DOIUrl":"10.1002/anie.2435246","url":null,"abstract":"Long-wavelength multiple resonance (MR) emitters are desirable for high-color-purity organic light-emitting diodes (OLEDs), yet conventional redshifting strategies often enhance excited-state delocalization and vibronic coupling, leading to spectral broadening. In this study, we present a symmetry reconstruction strategy to break the trade-off between spectral redshift and broadening in MR emitters. Unilateral and bilateral naphthalene-fused π-extension afford SN-BN and DN-BN, respectively, providing a direct platform for correlating excited-state symmetry, vibronic coupling, and emission bandwidth. SN-BN lowers the excited-state energy but disrupts the balanced excited-state hole-electron distribution, inducing partial charge-transfer character and enhanced vibronic coupling. In contrast, DN-BN expands the π-conjugated framework and reconstructs excited-state symmetry, thereby preserving short-range charge-transfer character while suppressing structural relaxation and vibronic coupling. Consequently, DN-BN exhibits yellow emission at 545 nm with an ultranarrow full-width at half-maximum (FWHM) of 16 nm/0.07 eV and a photoluminescence quantum yield of 90% in toluene. The corresponding OLED achieves yellow electroluminescence at 560 nm with an FWHM of 24 nm, a maximum external quantum efficiency of 23.3%, and efficiency roll-offs of 33.5% and 43.8% at 1000 and 100 000 cd m-2, respectively. This work establishes symmetry-reconstructive π-extension as a promising design strategy for high-color-purity, long-wavelength MR emitters.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e2435246"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148893324","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 Bidentate Chelation Strategy for Breaking the Thermodynamic Hydrophobicity-Activity Trade-Off to Boost the Electroreduction of CO₂ to Formate. 一种双齿螯合策略：打破热力学疏水-活性平衡，促进CO2电还原成甲酸盐。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-08-28 DOI: 10.1002/anie.9439653

Kang Liu, Zheng Lin, Zhengyi Qian, Xiaoyan Zhang, Mengyu Guo, Longren Wang, Mingzi Sun, Yue Wang, Bolong Huang, Shaojun Guo, Lixue Zhang

{"title":"A Bidentate Chelation Strategy for Breaking the Thermodynamic Hydrophobicity-Activity Trade-Off to Boost the Electroreduction of CO2 to Formate.","authors":"Kang Liu, Zheng Lin, Zhengyi Qian, Xiaoyan Zhang, Mengyu Guo, Longren Wang, Mingzi Sun, Yue Wang, Bolong Huang, Shaojun Guo, Lixue Zhang","doi":"10.1002/anie.9439653","DOIUrl":"10.1002/anie.9439653","url":null,"abstract":"Achieving industrially relevant electrochemical CO2 reduction (CO2RR) to formic acid requires catalyst that simultaneously exhibits high intrinsic activity and surface hydrophobicity. However, high intrinsic activity is considered thermodynamically contradictory on a hydrophobic surface since high hydrophobicity corresponds to low surface energy, thereby leading to low intrinsic activity. Here we overcome this hydrophobicity-activity trade-off via a bidentate chelation strategy that grafts carboxylic acid molecules with tunable alkyl chain lengths on Bi2O2CO3 (XC-BOC, where X denotes the carbon number). The obtained 10C-BOC sustains high hydrophobicity without sacrificing activity. This hydrophobicity-activity balance is achieved by restructuring the interfacial hydrogen-bond (HB) network to suppress the undesired hydrogen evolution reaction (HER) and ensure the timely hydrogenation rate for the key *OCHO intermediate, in conjunction with modulating the Bi site electronic structure via the carboxyl-O/Bi bidentate chelation to guarantee the high intrinsic activity. Consequently, 10C-BOC achieves ampere-level performance with FEHCOO- > 90% from 100-1000 mA cm-2, with an optimal FEHCOO- of 97.7% at 600 mA cm-2 (vs. 83.2% for bare BOC), and maintains FEHCOO- > 93% at 200 mA cm-2 for 200 h. This work offers a general strategy to decouple hydrophobicity from intrinsic activity for advanced CO2RR electrocatalysts.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e9439653"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148851856","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

2D Covalent Organic Frameworks as Robust n-Type Organic Mixed Ionic-Electronic Conductors for Electrochemical Transistors. 二维共价有机框架作为电化学晶体管中坚固的n型有机混合离子电子导体。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-09-02 DOI: 10.1002/anie.5032409

Wenkai Zhao, Junyi Han, Guangen Fu, Yiming Wang, Quanxing Yao, Ling Yin, Yuxiang Zhao, Shengxu Li, Qiang Ma, Guohui Gao, Wan Yue, Xiaojian Zhu, Paolo Samorì, Tao Zhang

{"title":"2D Covalent Organic Frameworks as Robust n-Type Organic Mixed Ionic-Electronic Conductors for Electrochemical Transistors.","authors":"Wenkai Zhao, Junyi Han, Guangen Fu, Yiming Wang, Quanxing Yao, Ling Yin, Yuxiang Zhao, Shengxu Li, Qiang Ma, Guohui Gao, Wan Yue, Xiaojian Zhu, Paolo Samorì, Tao Zhang","doi":"10.1002/anie.5032409","DOIUrl":"10.1002/anie.5032409","url":null,"abstract":"Organic mixed ionic-electronic conductors (OMIECs) with exclusive electrochemical modulation and coupling between ions and electrons have exhibited intriguing efficiencies in bioelectronics, logic circuits, and wearable devices. However, OMIECs are typically linear polymers whose excessive structural swelling and morphological disorder during electrochemical doping led to low performance and instability. Here, we report n-type 2D covalent organic frameworks (2D COFs) as novel OMIECs (BTID-BFDO COF and BTDD-BFDO COF). The rigid π-conjugated scaffold functions as both a charge transport pathway and an ion-electron coupling plane, whilst the nanochannels serve as directional conduits for rapid ion transport. 2D OMIECs-based OECTs exhibit favorable threshold voltages (< 0.5 V), Ion/Ioff ratios (103) and high stability (modulation current retention rate of 91.3% during continuous operation) compared with the linear counterpart (< 10%). More importantly, we elucidate the mechanism underlying in situ ion transport and doping within the rigid porous architectures of 2D OMIECs, establishing a novel design paradigm for robust n-type organic semiconductors.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e74084"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148877106","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 Triple-Site Engineered Heterojunction Photocatalyst for Full-Spectrum NH₃ Synthesis via Synergistic Promotion of Water Oxidation and Nitrate Reduction. 三位点工程异质结光催化剂协同促进水氧化和硝酸盐还原全光谱合成NH3。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-08-28 DOI: 10.1002/anie.9657393

Yamin Xi, Shunqiong Long, Jing Wang, Chaoqi Zhang, Tianxiang Wang, Tong Bao, Suzhao Liu, Yingying Zou, Yuye Zhao, Chengzhong Yu, Chao Liu

{"title":"A Triple-Site Engineered Heterojunction Photocatalyst for Full-Spectrum NH3 Synthesis via Synergistic Promotion of Water Oxidation and Nitrate Reduction.","authors":"Yamin Xi, Shunqiong Long, Jing Wang, Chaoqi Zhang, Tianxiang Wang, Tong Bao, Suzhao Liu, Yingying Zou, Yuye Zhao, Chengzhong Yu, Chao Liu","doi":"10.1002/anie.9657393","DOIUrl":"10.1002/anie.9657393","url":null,"abstract":"Photocatalytic nitrate reduction reaction (NitRR) represents a sustainable approach to convert nitrate pollutants to valuable NH3. However, the performance of state-of-the-art photocatalysts is hampered by insufficient near-infrared (NIR) light utilization and sluggish kinetics of hydrogenation steps and coupled water-oxygen reaction (WOR). Herein, we report a NIR-response S-scheme heterojunction photocatalyst with engineered triple-active sites for NH3 production. The integration of narrow-bandgap CuS and Co-based metal-organic framework (Co-MOF) into an S-scheme heterojunction enhances the NIR light harvesting and charge separation. At the heterointerface, the Cu and Co sites drive WOR and NitRR, respectively. Acting as a dynamic proton relay, the bridging S sites capture protons from H2O to facilitate its dissociation at Cu sites and sequentially transport the protons to Co sites to promote the hydrogenation steps. The synergy of Cu, S, and Co sites thereby induces an interfacial dynamic proton transfer mechanism for balancing the kinetics of the two coupled reactions. Taken together, an NH3 production rate of 5750.06 µmol g-1 h-1 is achieved with an apparent quantum yield of 13.27% at 600 nm and 11.63% at 1000 nm, and a solar-to-chemical conversion efficiency of 0.11%. This work provides valuable perspectives into the design principles of advanced nitrate reduction photocatalysts.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e9657393"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148852127","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

Carbonyl-Enriched Nonionic Covalent Organic Framework Nanochannels for High-Salinity Ionic Thermoelectrics. 高盐离子热电材料的富羰基非离子共价有机框架纳米通道。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-08-28 DOI: 10.1002/anie.4046032

Huixia Lv, Zhiwei Xing, Zhuozhi Lai, Qing Guo, Kunkun Ren, Haitao Su, Jiaming Yi, Sai Wang, Qi Sun

{"title":"Carbonyl-Enriched Nonionic Covalent Organic Framework Nanochannels for High-Salinity Ionic Thermoelectrics.","authors":"Huixia Lv, Zhiwei Xing, Zhuozhi Lai, Qing Guo, Kunkun Ren, Haitao Su, Jiaming Yi, Sai Wang, Qi Sun","doi":"10.1002/anie.4046032","DOIUrl":"10.1002/anie.4046032","url":null,"abstract":"High-salinity electrolytes coupled with low-grade heat offer an attractive opportunity for ionic thermoelectric conversion, yet conventional fixed-charge membranes rapidly lose ion permselectivity in concentrated media because Donnan exclusion is strongly screened. Here, we report an isoreticular series of nonionic covalent organic framework membranes with comparable one-dimensional nanochannels but systematically varied pore-wall oxygen chemistry. Hydroxyl-substitution-regulated hydrazone-to-β-ketoenamine tautomerism generates carbonyl-enriched BthTb-3OH nanochannels, which preferentially partition and transport cations while suppressing anion migration without relying on covalently anchored charges. Across diverse electrolytes, BthTb-3OH exhibits broadly cation-favored transport, with particularly strong cation/anion mobility contrasts in sulfate- and phosphate-containing media. Experiments and molecular dynamics simulations further reveal that the carbonyl-rich channels couple high K+ permselectivity with rapid K+ conduction under concentrated-salt conditions. K3PO4 preconditioning reorganizes the confined transport landscape through retained phosphate/K+ species within the carbonyl-rich nanochannels, facilitating K+ transport and amplifying thermodiffusive cation/anion contrast in sulfate media. Consequently, the conditioned membrane delivers a peak power density of 224.2 W m-2 in saturated K2SO4 under a 50 K temperature difference, establishing nonionic COF nanochannels as a charge-screening-resistant platform for high-salinity ionic thermoelectrics.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e4046032"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148852255","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

Orthogonal Photochemistry-Confined Crystallization Enables Mechanically Robust, Printable Shape-Programmable Polymers. 正交光化学限制结晶使机械坚固，可打印的形状可编程聚合物。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-08-28 DOI: 10.1002/anie.7052006

Beijia Yuan, Tong Yang, Yanpei Tian, Yulin Xiong, Zhe Lu, Ming Lei, Zijian Zheng, Xinjun Luan, You Yu, Hongqiu Wei

{"title":"Orthogonal Photochemistry-Confined Crystallization Enables Mechanically Robust, Printable Shape-Programmable Polymers.","authors":"Beijia Yuan, Tong Yang, Yanpei Tian, Yulin Xiong, Zhe Lu, Ming Lei, Zijian Zheng, Xinjun Luan, You Yu, Hongqiu Wei","doi":"10.1002/anie.7052006","DOIUrl":"10.1002/anie.7052006","url":null,"abstract":"Shape-programmable polymers are promising for soft robotics, minimally invasive medicine, and deployable structures. However, integrating high mechanical robustness, versatile shape programmability, and excellent printability into a single material system remains challenging. Here, an orthogonal photochemistry-confined crystallization strategy is developed to fabricate mechanically robust, printable shape-programmable polymers. This approach utilizes a rationally designed photochemical process to trigger radical polymerization and phenol coupling synchronously yet orthogonally, enabling one-step formation of a covalent double-network that efficiently confines polymer crystallization during solvent evaporation. The resulting homogeneous, refined crystalline domains greatly enhance stretchability (1891%) and toughness (41 MJ m- 3) by up to 63- and 103-fold, respectively, compared to counterparts lacking network confinement, while also maintaining fatigue resistance over 1500 stretching cycles. The synergy between confined crystallization and double-network confinement further confers shape reconfiguration and shape‑memory morphing, affording robust shape programmability under thermal stimuli. Moreover, the efficient photo‑mediated gelation, coupled with solvent evaporation, enables rapid and controllable solidification fully compatible with additive manufacturing. Leveraging these capabilities, and as a proof-of-concept, the developed polymers are printed and assembled into bioinspired soft actuators capable of integrated active actuation and precise sensing. This work provides new insight into the photochemical design of high-performance shape-programmable polymers and advanced soft devices.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e7052006"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148852307","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

Conjugation-Controlled Ion Response in One-Dimensional Covalent Organic Frameworks for Seawater Photocatalysis. 海水光催化一维共价有机框架中共轭控制离子响应。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-08-28 DOI: 10.1002/anie.7279758

Jie-Yu Yue, Yan Guo, Zi-Shuo Xu, Jing Lin, Peng Yang, Bo Tang

{"title":"Conjugation-Controlled Ion Response in One-Dimensional Covalent Organic Frameworks for Seawater Photocatalysis.","authors":"Jie-Yu Yue, Yan Guo, Zi-Shuo Xu, Jing Lin, Peng Yang, Bo Tang","doi":"10.1002/anie.7279758","DOIUrl":"10.1002/anie.7279758","url":null,"abstract":"Photocatalytic hydrogen evolution from seawater offers a sustainable route for energy production, yet the role of dissolved ions in modulating carrier dynamics remains poorly understood. Herein, we demonstrate conjugation-controlled ion responses that regulate charge separation in one-dimensional covalent organic frameworks (1D COFs) through ion-induced polarization for seawater photocatalysis. Two COFs featuring localized (DHP-COF) and extended (DHPD-COF) conjugation are constructed. In natural seawater, DHP-COF achieves 246.9 mmol g-1 h-1 for hydrogen evolution, 5.03-fold higher than in pure water (49.1 mmol g-1 h-1), whereas DHPD-COF shows only 2.48-fold enhancement (from 38.9 to 96.5 mmol g-1 h-1), revealing markedly stronger ion-responsive sensitivity in the locally conjugated framework. Mechanistic investigations reveal that localized conjugation preserves spatially inhomogeneous polar domains arising from segmented π-electron distribution, enabling strong coupling with seawater ions and thereby amplifying local dipoles to generate enhanced internal electric fields for efficient charge separation. In contrast, extended π-delocalization leads to electronic homogenization that attenuates ion-induced polarization. Beyond hydrogen production, this system simultaneously achieves chemoselective hydrogenation of α,β-unsaturated carbonyl compounds to high-value pharmaceutical intermediates in natural seawater/CH3OH. These findings establish conjugation-controlled ion response as a key design principle for charge separation in saline photocatalysis and provide general guidelines for environment-adaptive catalysts.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e7279758"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148852219","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

Evolving an Aptameric Nose for Synthetic Cannabinoids Through Modular Reprogramming of Specificity. 通过特异性模块重编程进化合成大麻素的适体鼻。

IF 16.9

Angewandte Chemie (International ed. in English) Pub Date : 2026-10-19 Epub Date: 2026-08-28 DOI: 10.1002/anie.6031066

Yijing He, Fan Zhang, Huixi Wang, Yue Yang, Keyu Shao, Kai-Bo Wang, Xiaoyi Chen, Haixiang Yu, Bin Di

{"title":"Evolving an Aptameric Nose for Synthetic Cannabinoids Through Modular Reprogramming of Specificity.","authors":"Yijing He, Fan Zhang, Huixi Wang, Yue Yang, Keyu Shao, Kai-Bo Wang, Xiaoyi Chen, Haixiang Yu, Bin Di","doi":"10.1002/anie.6031066","DOIUrl":"10.1002/anie.6031066","url":null,"abstract":"Discerning subtle structural differences among highly similar small molecules remains a major challenge for synthetic receptors. Natural olfactory systems solve this problem using cross-reactive receptor families that combine a conserved docking core with hypervariable specificity domains. Despite the modular nature of nucleic acid aptamers, the variable supporting domains have largely been viewed as inert scaffolds, whereas the conserved regions have been the main focus of functional studies. Here, we demonstrate that these supporting domains actively govern fine-structural selectivity, thereby decoupling specificity from core binding affinity and enabling modular reprogramming of recognition. Guided by this insight, we emulated natural receptor evolution by screening a structure-biased library with randomized peripheral domains, thus building a family of structurally homologous, cross-reactive aptamers against synthetic cannabinoids. When assembled into a machine-learning-guided sensor array, termed an \"aptameric nose\", this repertoire produces distinct yet correlative response patterns for closely related analogs. The array robustly discriminates these compounds and adaptively identifies emerging new variants. Through modular reprogramming, we engineer artificial receptor families that keep pace with continuously diversifying chemical threats, offering a powerful analytical tool for forensic, clinical, and environmental monitoring.","PeriodicalId":520556,"journal":{"name":"Angewandte Chemie (International ed. in English)","volume":" ","pages":"e6031066"},"PeriodicalIF":16.9,"publicationDate":"2026-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148852226","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