Angewandte Chemie International Edition最新文献_第2页

Mark C. Lipke 马克·c·利普克

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-03 DOI: 10.1002/anie.202508938

Mark C. Lipke

引用次数: 0

Phenacetin[3]arenes: Mannich-type Macrocyclization, Unique Structure, Versatile Functionalization, and Strong Allosteric Binding 非那西丁芳烃：曼尼型大环化、独特结构、多功能功能化和强变构结合

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202504211

Yanling Shen, Xiaotong Liang, Tianning Ma, Dayang Zhou, Wenjia Liu, Jingyu Ma, Wanhua Wu, Zhipeng Yu, Cheng Yang

{"title":"Phenacetin[3]arenes: Mannich-type Macrocyclization, Unique Structure, Versatile Functionalization, and Strong Allosteric Binding","authors":"Yanling Shen, Xiaotong Liang, Tianning Ma, Dayang Zhou, Wenjia Liu, Jingyu Ma, Wanhua Wu, Zhipeng Yu, Cheng Yang","doi":"10.1002/anie.202504211","DOIUrl":"https://doi.org/10.1002/anie.202504211","url":null,"abstract":"This work introduces a novel NAm-CH₂-CAr macrocyclization pathway, diverging from the conventional CAr-CH₂-CAr linkages prevalent in macrocyclic arenes. This approach involves a one-pot condensation of readily available Phenacetin and its homologs with formaldehyde, yielding phenacetin[3]arenes (Ph[3]) in yields up to 25.9%. Ph[3] exhibits an unsymmetrical hourglass-shaped architecture, featuring an upper rim adorned with amide groups and a lower rim comprising an alkoxylbenzene cavity. This unique structure facilitates reversible equilibrium between conformers via benzene ring flipping, which simultaneously reverses the orientation of the amide groups, establishing equilibrium between C3 and F conformers. Increasing concentrations of organic ammonium guests lead to a transition from a predominantly 1:1 to a 1:2 host–guest complexation. The estimated binding constants for the 1:1 complexes are in the order of 104-105 M-1, the overall binding constants for the 1:2 complexes are greater than 106 M-2. This stepwise complexation triggers a conformational shift from the C3 to the F conformer, demonstrating intriguing allosteric behavior. Furthermore, interactions with chiral guests selectively influence the equilibrium of planar chiral conformers, generating chiroptical responses suitable for chirality sensing applications. The distinct functional groups on the two rims—amides and alkoxyl groups—facilitate diverse chemical modifications, including reduction, deprotection, and condensation, …","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"39 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897733","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Synthesis and Modification of Formate Zr-MOF (ZrFA) toward Scalable and Cost-Cutting Gas Separation 甲酸Zr-MOF （ZrFA）的合成与改性及其在气体分离中的应用

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202505978

Xiao-Hong Xiong, Liang Song, Wei Wang, Xiao-Yan Zhu, Liu-Li Meng, Hui-Ting Zheng, Zhang-Wen Wei, Li-Lin Tan, Xiao-Chun Huang, Cheng-Yong Su

{"title":"Synthesis and Modification of Formate Zr-MOF (ZrFA) toward Scalable and Cost-Cutting Gas Separation","authors":"Xiao-Hong Xiong, Liang Song, Wei Wang, Xiao-Yan Zhu, Liu-Li Meng, Hui-Ting Zheng, Zhang-Wen Wei, Li-Lin Tan, Xiao-Chun Huang, Cheng-Yong Su","doi":"10.1002/anie.202505978","DOIUrl":"https://doi.org/10.1002/anie.202505978","url":null,"abstract":"The mass production of metal-organic frameworks (MOFs) with affordable cost is highly demanding yet limited for commercial applications, e.g., purification of polymer-grade ethylene (C2H4) via acetylene (C2H2) and carbon dioxide (CO2) removal faces the challenge of developing low-cost and large-scale physisorbents with efficiency and recyclability. Herein, we developed a viable synthetic protocol to scale-up a series of ultramicroporous Zr-MOFs (ZrFA/ZrFA-D/ZrFA-D-Cu(I)) with the simplest monocarboxylate, formate (FA), through consecutive production by recycling solvent/modulator. Besides a size-exclusion effect disfavoring C2H4 adsorption, introduction of defective and Cu(I) sites was found to enhance gas affinity and uptake capacity. A comprehensive evaluation of C2H4 separation and economic efficiency has been proposed, suggesting the improvement of C2H2 uptake capacity is effective for the binary C2H2/C2H4 separation, while the separation process of the ternary C2H2/CO2/C2H4 mixtures depends on subtle tradeoff of complex factors and limited by challenging CO2/C2H4 separating. Notably, the large-scale separation has been testified to significantly improve separation efficiency, and the low-cost preparation benefits high economic efficiency. The distinct C2H2/C2H4/CO2 adsorption mechanism in ZrFA/ZrFA-D/ZrFA-D-Cu(I) has been elucidated by the theoretical calculations. This work may shed a light on the future C2H4 purification technology by pushing MOF-syntheses towards low-cost, scale-up, and recyclable production.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"9 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

P-type Cathode Material Design Guided by Material Descriptors for High-energy Density Sodium Batteries 基于材料描述符的高密度钠电池p型正极材料设计

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202505831

Weijia Zhang, Tianjiang Sun, Weichao Cheng, Mengyao Shi, Min Cheng, Qiong Sun, Jianfei Su, Xiulan Li, Zhanliang Tao

{"title":"P-type Cathode Material Design Guided by Material Descriptors for High-energy Density Sodium Batteries","authors":"Weijia Zhang, Tianjiang Sun, Weichao Cheng, Mengyao Shi, Min Cheng, Qiong Sun, Jianfei Su, Xiulan Li, Zhanliang Tao","doi":"10.1002/anie.202505831","DOIUrl":"https://doi.org/10.1002/anie.202505831","url":null,"abstract":"P-type organic electrode materials (OEMs) face considerable challenges in constructing high-energy density sodium metal batteries (SMBs) due to the low capacity. To preserve their voltage advantage, developing effective structural design strategies is essential. However, the lack of material descriptors hampers the efficiency of material design and screening. Herein, two material descriptors: the benzene ring/active nitrogen (R/N) ratio and energy density factor (Ef) are established to guide high-energy density SMB design. As proof of concept, triphenylamine (TPA, 3 R/N ratio and 573.6 Ef value) and a porous organic polymer condensation of triiodotriphenylamine and dihydrophenazine named p-PZA POP (1.5 R/N ratio and 907.5 Ef value) are chosen. As a result, the p-PZA POP achieves a high energy density of 524.6 Wh kg-1 at 1 A g-1, nearly double that of TPA (273.3 Wh kg-1). Remarkably, p-PZA POP demonstrates excellent wide-temperature electrochemical performance from 50 °C (166.2 mAh g-1 at 1 A g-1) to -20 °C (141.6 mAh g-1 at 0.1 A g-1). This work establishes a theoretical framework for the rational design and screening of high-performance p-type OEMs through predictive material descriptors.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"42 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143901794","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Chen Wang 陈王

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202508077

Chen Wang

引用次数: 0

Spatially Engineering the Internal Microstructure of a Single Crystal via Nanoparticle Occlusion 利用纳米粒子遮挡技术实现单晶内部微观结构的空间工程

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202505637

Bing Yu, Pei Liu, Jingjing He, Xiaojie Li, Xia Sun, Boxiang Peng, Jiahao Zhang, Yin Ning

{"title":"Spatially Engineering the Internal Microstructure of a Single Crystal via Nanoparticle Occlusion","authors":"Bing Yu, Pei Liu, Jingjing He, Xiaojie Li, Xia Sun, Boxiang Peng, Jiahao Zhang, Yin Ning","doi":"10.1002/anie.202505637","DOIUrl":"https://doi.org/10.1002/anie.202505637","url":null,"abstract":"Single crystals are characterized by their continuous, highly ordered atomic lattices. Therefore, introducing impurities or structural defects into their matrices presents a major challenge, particularly in spatially-controlled manner. Herein, we demonstrate a nanoparticle occlusion approach that enables the microstructure of cuprous oxide (Cu2O) single crystals to be engineered in a tunable way. This is achieved by directly incorporating poly(glycerol monomethacrylate)51-block-poly(benzyl methacrylate)100 [G51-B100] diblock copolymer nanoparticles into growing Cu2O crystals, leading to the formation of G51-B100@Cu2O composite crystals with structural defects localized at the G51-B100/Cu2O interfaces. The spatial distribution of these defects can be systematically engineered, ranging from surface region to the entire crystal. Remarkably, the G51-B100 occlusion endows the resulting composite crystals with excellent catalytic performance in dye degradation under dark conditions, with activity correlated to the extent of nanoparticle occlusion. This study offers a unique strategy to create interfacial defects in single crystals, imparting emerging functionalities to the resulting composites.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"111 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897731","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

p-π Conjugation-Promoted Electrochemiluminescence of Halogenated Covalent Organic Framework Nanoemitters p-π共轭促进卤代共价有机骨架纳米发光材料的电化学发光

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202506309

Jianping Lei, Hanlin Hou, Yuting Wu, Jiacheng Wan, Rengan Luo, Lina Wu, Yanli Zhao, Xiaojun Wu

{"title":"p-π Conjugation-Promoted Electrochemiluminescence of Halogenated Covalent Organic Framework Nanoemitters","authors":"Jianping Lei, Hanlin Hou, Yuting Wu, Jiacheng Wan, Rengan Luo, Lina Wu, Yanli Zhao, Xiaojun Wu","doi":"10.1002/anie.202506309","DOIUrl":"https://doi.org/10.1002/anie.202506309","url":null,"abstract":"Covalent organic frameworks (COFs) are a kind of promising electrochemiluminescence (ECL) crystalline nanoemitters due to their rapid intrareticular charge transfer and predesigned structures. However, the high polarization of heteroatom-containing linkages impedes the charge transfer within reticular structures. In this study, we construct a series of halogenated COFs nanoemitters composed of terephthalaldehyde ortho-substitutions and 1,3,6,8-tetrakis(4-aminophenyl)pyrene ligands via a covalent halogenation predesign strategy. The incorporation of covalently bonded halogen atoms promotes a dense electron population in carbon-carbon antibonding molecular orbitals, thereby facilitating efficient p-π conjugation within the COF structure. Based on the improved intrareticular charge transfer along carbon skeleton, as evidenced by the Hall effect and terahertz spectroscopy, the brominated COF demonstrates a 49-fold enhancement in ECL intensity compared to non-halogenated COF. Furthermore, the performance of four partially brominated COFs establishes a positive correlation between the degree of Br doping and ECL intensity. Beyond the corresponding model compounds, the conjugated frameworks of COFs significantly amplify the halogenation-induced enhancement effect. This halogenation-promoted p-π conjugation in reticular skeleton provides a universal strategy to sensitize crystalline nanoemitters for decoding ECL enhancement mechanism.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"10 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143901796","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Harnessing Negative Photochromism in Styryl Cyanines for Light-Modulated Proton Transport 利用苯乙烯菁中的负光致变色进行光调制质子输运

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202506532

Gianni Pacella, Maria Nabatova, Yuxuan Zhang, David Picconi, Roza R. Weber, Shirin Faraji, Giuseppe Portale

{"title":"Harnessing Negative Photochromism in Styryl Cyanines for Light-Modulated Proton Transport","authors":"Gianni Pacella, Maria Nabatova, Yuxuan Zhang, David Picconi, Roza R. Weber, Shirin Faraji, Giuseppe Portale","doi":"10.1002/anie.202506532","DOIUrl":"https://doi.org/10.1002/anie.202506532","url":null,"abstract":"Efficient photoswitches capable of complete conversion to their metastable isomer are not so common, yet highly desirable for applications in smart materials and devices. Here, we report the photochromic behavior of a series of styryl cyanine photoswitches, all demonstrating high switching efficiency, with some achieving full conversion to the metastable form. Despite structural similarities to spiropyran photoswitches, we demonstrate that the photochemistry of styryl cyanines is fundamentally different. Unlike classical photoswitches that rely on double-bond rotation, these molecules undergo substantial geometric changes via the formation of a spiro carbon. This transformation disrupts conjugation, causing a desirable blue shift in absorbance ideal for creating responsive materials and devices. We further show that the switching kinetics can be finely tuned through electronic effects of various substituents or the choice of surrounding medium. These photoswitches exhibit excellent fatigue resistance and can be easily shifted into the visible region via their acidochromic properties. Taking advantage of their high switching efficiency and affinity for acidic polymers, we finally propose their use as smart dopants to develop light-responsive materials with tunable proton transport properties under visible light irradiation.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"14 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143897985","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Solar-Blind Ultraviolet Organic Mechanoluminescent Materials 太阳盲紫外有机机械发光材料

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202506461

Hailan Wang, Yuxin Xiao, Shuting Kong, Yuanda Luo, Tao Yu, Wei Huang

{"title":"Solar-Blind Ultraviolet Organic Mechanoluminescent Materials","authors":"Hailan Wang, Yuxin Xiao, Shuting Kong, Yuanda Luo, Tao Yu, Wei Huang","doi":"10.1002/anie.202506461","DOIUrl":"https://doi.org/10.1002/anie.202506461","url":null,"abstract":"Organic mechanoluminescent (ML) materials have attracted intensive attention for their potential applications in real-time stress sensing and structural damage monitoring. To avoid interference from daylight or artificial lighting sources, the ML-based sensors can be only used in dark-field scenarios, which becomes the most serious limitation for their development. Herein, we proposed a new strategy that adjusts the ML spectra to the solar-blind ultraviolet region to address this challenge. By strategically breaking the molecular conjugation and adjusting the packing mode, a series of diphenylphosphine oxide derivatives were successfully designed. To our delight, the shortest ML emission, among all reported organic ML materials, with the maxima at ca. 293 nm (in solar-blind UV region) was achieved. Photophysical studies, single crystal analysis and theoretical calculations were performed to investigate the solar-blind UV ML properties. Furthermore, wide-range color-tunable ML emissions spanning from 293 nm to 741 nm were achieved. Under various external stimuli such as stretching, folding, and vehicle impact in daylight, obvious ML signals could be directly recorded, and the quantitative relationship between the mechanical stimuli and the ML intensities was also studied. This work suggests a feasible strategy to realize solar-blind UV ML materials and makes bright-field environment ML sensors possible.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"8 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143901795","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Gang Li

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-02 DOI: 10.1002/anie.202508663

Gang Li

引用次数: 0