Angewandte Chemie International Edition最新文献_第3页

Fluorescence Modulation through the Inverted Energy Gap Law in Triply N-B←N-Containing Windmill-Shaped Triazines. 三重 N─B←N 含风车形三嗪中通过倒能隙定律实现的荧光调制。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-18 DOI: 10.1002/anie.202416425

Yi Feng, Liangxuan Wang, Hongcheng Gao, Jiadong Zhou, Matthias Stolte, Honglin Qiu, Linlin Liu, Victor Adebayo, Martial Boggio-Pasqua, Frank Würthner, Johannes Gierschner, Zengqi Xie

引用次数: 0

Localized High-Concentration Electrolyte for All-Carbon Rechargeable Dual-Ion Batteries with Durable Interfacial Chemistry. 用于全碳可充电双离子电池的局部高浓度电解质与持久的界面化学。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-18 DOI: 10.1002/anie.202416610

Rui Liu, Yan-Song Xu, Rui Zhou, Shuang-Jie Tan, Yun-Nuo Li, Si-Jie Jiang, Sen Xin, Yu-Guo Guo, Fei-Fei Cao

{"title":"Localized High-Concentration Electrolyte for All-Carbon Rechargeable Dual-Ion Batteries with Durable Interfacial Chemistry.","authors":"Rui Liu, Yan-Song Xu, Rui Zhou, Shuang-Jie Tan, Yun-Nuo Li, Si-Jie Jiang, Sen Xin, Yu-Guo Guo, Fei-Fei Cao","doi":"10.1002/anie.202416610","DOIUrl":"10.1002/anie.202416610","url":null,"abstract":"Lithium-based rechargeable dual-ion batteries (DIBs) based on graphite anode-cathode combinations have received much attention due to their high resource abundance and low cost. Currently, the practical realization of the batteries is hindered by easy oxidation of the electrolyte at the cathode interface, and solvent co-intercalation at the anode-electrolyte interface. Configuration of a \"solvent-in-salt\" electrolyte with a high concentration of Li salt is expected to stabilize the electrolyte chemistry versus both electrodes, yet inevitably reduces the mobility of the solvated working ions and increases the cost of the electrolyte. Herein, we propose to build a localized high-concentration electrolyte by adding hydrofluoroether as the diluent to reduce the salt content while improving the solvation structure, allowing more anions to enter the inner solvation sheath. The new electrolyte helps to form uniform and thin interfaces, with elevated contents of inorganic fluorides, on both electrodes, which effectively suppress electrolyte oxidation at the cathode and optimize electrolyte-electrode compatibility at the anode while facilitating charge transfer across the interface. Consequently, the DIBs with graphite as anode and cathode operate for 3000 cycles and retain a high-capacity retention of 95.7 %, highlighting the importance of stable interfacial chemistry in boosting the electrochemical performance of DIBs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416610"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542283","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

Regulating Interface Dipole Interaction between Ethers and Active Species Toward Highly Stable Li-SPAN Batteries. 调节醚和活性物质之间的界面偶极相互作用，实现高稳定性的锂-SPAN 电池。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-20 DOI: 10.1002/anie.202416731

Xinyi Liu, Shuang Wu, Zhimeng Hao, Long Shang, Mao Guo, Jinze Hou, Siyuan Shao, Haixia Li, Yixin Li, Yong Lu, Kai Zhang, Zhenhua Yan, Jun Chen

{"title":"Regulating Interface Dipole Interaction between Ethers and Active Species Toward Highly Stable Li-SPAN Batteries.","authors":"Xinyi Liu, Shuang Wu, Zhimeng Hao, Long Shang, Mao Guo, Jinze Hou, Siyuan Shao, Haixia Li, Yixin Li, Yong Lu, Kai Zhang, Zhenhua Yan, Jun Chen","doi":"10.1002/anie.202416731","DOIUrl":"10.1002/anie.202416731","url":null,"abstract":"Sulfurized polyacrylonitrile (SPAN) is recognized as a promising organic cathode for long-lifespan lithium metal batteries. Nevertheless, the irreversible cleavage/formation of multiple sulfur-sulfur (S-S) bonds of SPAN within conventional ether-based electrolytes results in loss of active S species, severe capacity fading and shuttle effects. Herein, we propose a new electrolyte based on dipropyl ether (PE) solvent for Li-SPAN batteries. Benefiting from the particular chain-coordination structure and weak dipole interactions with Li+ and active species, the resulting electrolyte not only achieves low desolvation energy barrier and high Li+ transference number, but also displays stable electrolyte-electrode interface (EEI). Consequently, the full cells utilizing this electrolyte exhibit good cyclability, outstanding capacity retention and superior extreme-temperature (-50 °C to 50 °C) performance. Furthermore, the Ah-scale pouch cell with lean electrolyte (2.5 g Ah-1) achieves record cycle stability with 96.5 % capacity retention after 75 cycles, which deliver an initial specific energy density of 150 Wh kg-1 (based on the weight of the entire cell). Impressively, this strategy demonstrates universality in a series of organic electrodes employing with PE-based electrolytes. This work highlights the strategy for modulating the dipole interaction at EEI for long-lifespan Li-organic batteries at extreme conditions.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416731"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581134","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

Terminal Fluorination Modulates Crystallinity and Aggregation of Fully Non-Fused Ring Electron Acceptors for High-Performance and Durable Near-Infrared Organic Photodetectors. 末端氟化调节完全无熔环电子受体的结晶度和聚集，以实现高性能和耐用的近红外有机光电探测器。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-18 DOI: 10.1002/anie.202416751

Wenxu Liu, Wenjing Guo, Lulu Fu, Yuxin Duan, Guoxin Han, Jiaxin Gao, Huayi Liu, Yuxing Wang, Zaifei Ma, Yao Liu

{"title":"Terminal Fluorination Modulates Crystallinity and Aggregation of Fully Non-Fused Ring Electron Acceptors for High-Performance and Durable Near-Infrared Organic Photodetectors.","authors":"Wenxu Liu, Wenjing Guo, Lulu Fu, Yuxin Duan, Guoxin Han, Jiaxin Gao, Huayi Liu, Yuxing Wang, Zaifei Ma, Yao Liu","doi":"10.1002/anie.202416751","DOIUrl":"10.1002/anie.202416751","url":null,"abstract":"High dark current density (Jd) severely hinders further advancement of near-infrared organic photodetectors (NIR OPDs). Herein, we tackle this grand challenge by regulating molecular crystallinity and aggregation of fully non-fused ring electron acceptors (FNREAs). TBT-V-F, which features fluorinated terminals, notably demonstrates crystalline intensification and a higher prevalence predominance of J-aggregation compared to its chlorinated counterpart (TBT-V-Cl). The amalgamation of advantages confers TBT-V-F-based OPDs with lower nonradiative energy loss, improved charge transport, decreased energetic disorder, and reduced trap density. Consequently, the corresponding self-powered OPDs exhibit a 40-fold decrease in Jd, a remarkable increase in detectivity (D*sh), faster response time, and superior thermal stability compared to TBT-V-Cl-based OPDs. Further interfacial optimization results in an ultra-low Jd of 7.30×10-12 A cm-2 with D*sh over 1013 Jones in 320-920 nm wavelength and a climax of 2.2×1014 Jones at 800 nm for the TBT-V-F-based OPDs, representing one of the best results reported to date. This work paves a compelling material-based strategy to suppress Jd for highly sensitive NIR OPDs, while also illustrates the viability of FNREAs in construction of stable and affordable NIR OPDs for real-world applications.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416751"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581138","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

Bead-Based DNA Synthesis and Sequencing for Integrated Data Storage Using Digital Microfluidics. 利用数字微流控技术进行基于微珠的 DNA 合成和测序，以实现集成数据存储。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-12-05 DOI: 10.1002/anie.202416004

Yuhao Piao, Yitong Fang, Bin Li, Tiantian Man, Jie Chen, Fulin Zhu, Weiqiang Wang, Ying Wan, Shengyuan Deng

{"title":"Bead-Based DNA Synthesis and Sequencing for Integrated Data Storage Using Digital Microfluidics.","authors":"Yuhao Piao, Yitong Fang, Bin Li, Tiantian Man, Jie Chen, Fulin Zhu, Weiqiang Wang, Ying Wan, Shengyuan Deng","doi":"10.1002/anie.202416004","DOIUrl":"10.1002/anie.202416004","url":null,"abstract":"DNA is considered as a prospective candidate for the next-generation data storage medium, due to its high coding density, long cold-storage lifespan, and low energy consumption. Despite these advantages, challenges remain in achieving high-fidelity, fully integrated, and cost-efficient DNA storage system. In this study, a homemade digital microfluidic (DMF)-based compact DNA data storing pipeline is orchestrated to complete the entire process from the synthesis to the sequencing. The synthetic half employs phosphoramidite chemistry on 200 nm magnetic beads (MBs), where the dimethyltrityl protecting group is removed by droplet manipulation of trichloroacetic acid. The sequencing counterpart relies on pyrophosphate releasing originated from polymerase-catalyzed primer extension, which leads to photon-countable chemiluminescence (CL) signal in 2.5-μL drops of trienzyme cascading reactions. Further by DNA denaturation, repeated pyrosequencing plus plurality voting can improve the nucleobase accuracy beyond 95 %. As a proof-of-concept trial, semantic information is saved in DNA via the Huffman coding algorithm plus the Reed-Solomon error-correction, and then robustly retrieved from this streamlined platform. As a result, it took a net total of approximately 6.5 h to writing and reading 8 bytes of data, that equal to a storaging speed of 49 min/byte, much quicker than the previously reported 2.8-4.2 h/byte. This bead-based miniaturized device promises an unattended protocol for achieving high-throughput, full-packaged, and above all, neatly precision DNA storage.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416004"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142738017","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

Dehydration-enhanced Ion Recognition of Triazine Covalent Organic Frameworks for High-resolution Li+/Mg2+ Separation

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 DOI: 10.1002/anie.202422423

Qinghua Zhang, Wentong Meng, Sifan Chen, Ming Wu, Feng Gao, Yang Hou, Xiaoli Zhan, Wei Hu, Lijun Liang

{"title":"Dehydration-enhanced Ion Recognition of Triazine Covalent Organic Frameworks for High-resolution Li+/Mg2+ Separation","authors":"Qinghua Zhang, Wentong Meng, Sifan Chen, Ming Wu, Feng Gao, Yang Hou, Xiaoli Zhan, Wei Hu, Lijun Liang","doi":"10.1002/anie.202422423","DOIUrl":"https://doi.org/10.1002/anie.202422423","url":null,"abstract":"The precise and rapid extraction of lithium from salt-lake brines is critical to meeting the global demand for lithium resources. However, it remains a major challenge to design ion-transport membranes with accurate recognition and fast transport path for the target ion. Here, we report a triazine covalent organic framework (COF) membrane with high resolution for Li+ and Mg2+ that enables fast Li+ transport while almost completely inhibiting Mg2+ permeation. The remarkably high rejection of Mg2+ by the COF membrane is achieved via imposed ion dehydration and the construction of the energy well. The proper hydrophilic environment of the COF channel promotes the dissociation of Li+ from the negatively charged functional groups, allowing Li+ for hopping transport supported by the sulfonate side-chains to shorten the diffusion path of Li+. Under high-salinity electrodialysis conditions, the COF membrane demonstrates robust Li+/Mg2+ separation performance (No Mg2+ were detected in the collected solution), achieving efficient lithium recovery and high product purity (Li2CO3: 99.3%). This membrane design strategy enables high energy efficiency and powerful lithium extraction in the electrodialysis lithium extraction process, and can be generalized to other energy and separation related membranes.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"74 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142991367","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

Amorphous Nanobelts for Efficient Electrocatalytic Ammonia Production. 用于高效电催化氨生产的非晶纳米颗粒。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-06 DOI: 10.1002/anie.202416878

Ziming Su, Xiangyu Chen, Mingke Sun, Xiuyi Yang, Jianxin Kang, Zhi Cai, Lin Guo

{"title":"Amorphous Nanobelts for Efficient Electrocatalytic Ammonia Production.","authors":"Ziming Su, Xiangyu Chen, Mingke Sun, Xiuyi Yang, Jianxin Kang, Zhi Cai, Lin Guo","doi":"10.1002/anie.202416878","DOIUrl":"10.1002/anie.202416878","url":null,"abstract":"One-dimensional (1D) amorphous nanomaterials combine the advantages of high active site concentration of amorphous structure, high specific surface area and efficient charge transfer of 1D materials, so they present promising opportunities for catalysis. However, how to achievie the balance between the high orientation of 1D morphology and the isotropy of amorphous structure is a significant challenge, which severely obstructs the controllable preparation of 1D amorphous materials. Guided by the hard-soft acids-bases theory, here we develop a general strategy for preparing 1D amorphous nanomaterials through the precise modulation of bond strength between metal ions and organic ligands for a moderated fastness. The soft base dodecanethiol (DT) is multifunctionally served as both structure-regulating agent and morphology-directing agent. Compared with the borderline acids (e.g. Fe2+, Co2+, Ni2+) to construct amorphous structure, soft acid of Cu+ which produced crystalline nanobelts can still be amorphized by reducing the hardness of Cu ions through redox reaction to weak Cu-SR bond. Due to the combined advantages of amorphous structure and one-dimensional morphology, amorphous CuDT nanobelts exhibited excellent electrocatalytic activity in electrochemical nitrate reduction, outperformed most of the reported Cu-based catalysts. This work will effectively bridge the gap between traditional 1D crystalline nanomaterials synthesis and their amorphization preparation.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416878"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370337","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

Catalytically Active Site Mapping Realized through Energy Transfer Modeling. 通过能量转移建模实现催化活性位点映射

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-09 DOI: 10.1002/anie.202416695

William J Thompson, Buddhima K P Maldeni Kankanamalage, Grace C Thaggard, Kyoung Chul Park, Corey R Martin, Jia Niu, Jeffery A Byers, Natalia B Shustova

{"title":"Catalytically Active Site Mapping Realized through Energy Transfer Modeling.","authors":"William J Thompson, Buddhima K P Maldeni Kankanamalage, Grace C Thaggard, Kyoung Chul Park, Corey R Martin, Jia Niu, Jeffery A Byers, Natalia B Shustova","doi":"10.1002/anie.202416695","DOIUrl":"10.1002/anie.202416695","url":null,"abstract":"The demands of a sustainable chemical industry are a driving force for the development of heterogeneous catalytic platforms exhibiting facile catalyst recovery, recycling, and resilience to diverse reaction conditions. Homogeneous-to-heterogeneous catalyst transitions can be realized through the integration of efficient homogeneous catalysts within porous matrices. Herein, we offer a versatile approach to understanding how guest distribution and evolution impact the catalytic performance of heterogeneous host-guest catalytic platforms by implementing the resonance energy transfer (RET) concept using fluorescent model systems mimicking the steric constraints of targeted catalysts. Using the RET-based methodology, we mapped condition-dependent guest (re)distribution within a porous support on the example of modular matrices such as metal-organic frameworks (MOFs). Furthermore, we correlate RET results performed on the model systems with the catalytic performance of two MOF-encapsulated catalysts used to promote CO2 hydrogenation and ring-closing metathesis. Guests are incorporated using aperture-opening encapsulation, and catalyst redistribution is not observed under practical reaction conditions, showcasing a pathway to advance catalyst recyclability in the case of host-guest platforms. These studies represent the first generalizable approach for mapping the guest distribution in heterogeneous host-guest catalytic systems, providing a foundation for predicting and tailoring the performance of catalysts integrated into various porous supports.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202416695"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142370339","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

Planar Pentacoordinate Halogens. 平面五配位卤素。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-25 DOI: 10.1002/anie.202416057

Li-Juan Cui, Lin-Hong Miao, Mesías Orozco-Ic, Lu Li, Sudip Pan, Gabriel Merino, Zhong-Hua Cui

引用次数: 0

Aptamer and DNAzyme Based Colorimetric Biosensors for Pathogen Detection. 用于病原体检测的基于 Aptamer 和 DNA 酶的比色生物传感器。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2025-01-21 Epub Date: 2024-11-25 DOI: 10.1002/anie.202418725

Rudi Liu, Jiuxing Li, Bruno J Salena, Yingfu Li

{"title":"Aptamer and DNAzyme Based Colorimetric Biosensors for Pathogen Detection.","authors":"Rudi Liu, Jiuxing Li, Bruno J Salena, Yingfu Li","doi":"10.1002/anie.202418725","DOIUrl":"10.1002/anie.202418725","url":null,"abstract":"The detection of pathogens is critical for preventing and controlling health hazards across clinical, environmental, and food safety sectors. Functional nucleic acids (FNAs), such as aptamers and DNAzymes, have emerged as versatile molecular tools for pathogen detection due to their high specificity and affinity. This review focuses on the in vitro selection of FNAs for pathogens, with emphasis on the selection of aptamers for specific biomarkers and intact pathogens, including bacteria and viruses. Additionally, the selection of DNAzymes for bacterial detection is discussed. The integration of these FNAs into colorimetric biosensors has enabled the development of simple, cost-effective diagnostic platforms. Both non-catalytic and catalytic colorimetric biosensors are explored, including those based on gold nanoparticles, polydiacetylenes, protein enzymes, G-quadruplexes, and nanozymes. These biosensors offer visible detection through color changes, making them ideal for point-of-care diagnostics. The review concludes by highlighting current challenges and future perspectives for advancing FNA-based colorimetric biosensing technologies for pathogen detection.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202418725"},"PeriodicalIF":16.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646449","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