Angewandte Chemie International Edition最新文献_第9页

Taxonomy of Chemical Bondings: Opportunities and Challenges 化学键的分类：机遇与挑战

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-22 DOI: 10.1002/anie.202506525

Andrea Pizzi, Giancarlo Terraneo, Cristina Lo Iacono, Roberta Beccaria, Arun Dhaka, Giuseppe Resnati

引用次数: 0

Tailoring Indolocarbazole‐Bridged Multiple Resonance Emitter through Steric Pre‐Substitution for Narrowband Electroluminescence with EQE over 40% 通过空间预取代裁剪吲哚咔唑桥接多共振发射极，窄带电致发光EQE超过40%

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-22 DOI: 10.1002/anie.202504628

Chuanqin Cheng, Senqiang Zhu, Hai Zhang, Tianyu Huang, Chenglong Li, Zhiyuan Chen, Peng Xu, Rui Liu, Xudong Cao, Lei Wang, Dongdong Zhang, Lian Duan

{"title":"Tailoring Indolocarbazole‐Bridged Multiple Resonance Emitter through Steric Pre‐Substitution for Narrowband Electroluminescence with EQE over 40%","authors":"Chuanqin Cheng, Senqiang Zhu, Hai Zhang, Tianyu Huang, Chenglong Li, Zhiyuan Chen, Peng Xu, Rui Liu, Xudong Cao, Lei Wang, Dongdong Zhang, Lian Duan","doi":"10.1002/anie.202504628","DOIUrl":"https://doi.org/10.1002/anie.202504628","url":null,"abstract":"Multiple resonance (MR) emitters bridged by multi‐nitrogen indolocarbazoles to extend molecule skeletons could modify emission maximums without scarifying narrow full width at half maximum (FWHM), which, however, face synthesis challenges of uncontrollable borylation regioselectivity and spectral broadening issue from intermolecular aggregation. Here, a steric pre‐substitution strategy is devised using tert‐butylphenyl‐functionalized indolo[3,2‐b]carbazole as a bridge to extend MR skeletons, not only steering regioselective Bora‐Friedel‐Crafts borylation but also suppressing intermolecular interactions in films. The targeted greenish emitter therefore achieves a small electroluminescence FWHM of only 22 nm in device, matching the intrinsic photoluminescence one of 21 nm in dilute toluene. The extended skeleton also enhances the horizontal orientation of emitting dipole moment with a ratio of 90%, leading to a remarkable high maximum external quantum efficiency (EQE) of 41.0% and power efficiency of 106.5 lm W‐1. The efficiency roll‐off remains remarkably low with EQEs sustaining at 35.0% and 30.6% at luminance of 1,000 cd m‐2 and 5,000 cd m‐2, respectively. This work establishes a pre‐substitution paradigm to concurrently optimize synthesis control and solid‐state emission for high‐performance MR emitters.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"127 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113368","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

Dual‐Responsive Ultrathin Polymersomes with Reversible Transitions on Acidochromism and Fluorochromism Performances for Multiple Information Encryption 具有可逆酸致变色和荧光致变色性能的双响应超薄聚合体用于多重信息加密

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-22 DOI: 10.1002/anie.202507852

Zichao Sun, Zejiang Xu, Pengchao Wu, Liquan Wang, Mingyu Ding, Lin Zhao, Yongli Zheng, Yongfeng Zhou, Shaoliang Lin, Haibao Jin

{"title":"Dual‐Responsive Ultrathin Polymersomes with Reversible Transitions on Acidochromism and Fluorochromism Performances for Multiple Information Encryption","authors":"Zichao Sun, Zejiang Xu, Pengchao Wu, Liquan Wang, Mingyu Ding, Lin Zhao, Yongli Zheng, Yongfeng Zhou, Shaoliang Lin, Haibao Jin","doi":"10.1002/anie.202507852","DOIUrl":"https://doi.org/10.1002/anie.202507852","url":null,"abstract":"Endowing dual‐responsive ultrathin polymersomes (UTPSs) with reversible stimuli‐chromic and fluorochromic performances offers a prospective yet challenging strategy for achieving high‐level information encryption and anti‐counterfeiting. Herein, starting from rational synthesis of visible light/pH‐responsive integrated azobenzene monomer, side‐chain‐type amphiphilic alternating azocopolymers was elaborately crafted using a moderate epoxy‐amino click‐polycondensation. Followed by subsequent solution self‐assembly, dual‐responsive UTPSs with a diameter of ~253 nm and a vesicular thickness of ~2.1 nm were subtly produced based on the pendant hydrophobic conjugate stacking mechanism. The photoisomerization of azobenzene units and protonation of tertiary amines within UTPSs were accountable for the visible light‐ or pH‐triggered reversible shape and physicochemical transitions (i.e., color, size, diameter, vesicular thickness, zeta potential, fluorescent intensity) as well as repeatable acidochromism from yellow to pink and recyclable fluorochromism, respectively. Benefiting from these attractive traits, the proof‐of‐concept 2D Quick Response code was meticulously crafted using the stimuli‐chromic UTPSs into patterning lithography, showcasing a multi‐level decryption, favorable reversibility, and preferable recyclability for advanced information security. Our work provides innovative guidelines for the development of dual‐responsive UTPSs with multiple stimuli‐chromism merits for the potential of complex information encryption.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"55 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113370","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

Molecularly woven artificial solid electrolyte interphase 分子编织人工固体电解质界面

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-22 DOI: 10.1002/anie.202505056

Tianyu Shan, Zhijin Ju, Ding Xiao, Ke Yue, Zhenxing Cui, Yifei Zhang, Xiaodong Chi, Xiulin Fan, Guangfeng Li, Tao Xinyong, Feihe Huang

引用次数: 0

A Neutral Single-Molecule Carrier for Delivery of Phosphonate Drugs 磷酸盐类药物的中性单分子载体

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-22 DOI: 10.1002/anie.202509002

Biao Wu, Qingling Nie, Juan Tang, Yongsheng Li, Ji Wang, Boyang Li, Hongwei Ma, Xiao-Juan Yang, Wei Zhao

{"title":"A Neutral Single-Molecule Carrier for Delivery of Phosphonate Drugs","authors":"Biao Wu, Qingling Nie, Juan Tang, Yongsheng Li, Ji Wang, Boyang Li, Hongwei Ma, Xiao-Juan Yang, Wei Zhao","doi":"10.1002/anie.202509002","DOIUrl":"https://doi.org/10.1002/anie.202509002","url":null,"abstract":"Phosphate/phosphonate-based drugs (PDs), as multi-negative, hydrophilic molecules, face the greatest difficulty in diffusion across biological membranes, leading to poor bioavailability. Conventional drug delivery strategies to overcome this issue, including utilizing small-molecule prodrugs or nanoparticle carriers, often suffer from case-specific modifications or uncertainties in drug loading. Inspired by the anion coordination chemistry of natural phosphate transporters and artificial anion receptors, here we present the first use of a neutral anion receptor, i.e., bis(tripodal hexaurea) cage 1, as a “single-molecule carrier” for the delivery of PDs into living cells. Cage 1 features advantages of molecular-level encapsulation, enhanced intracellular accumulation, subcellular targeting, responsive drug release, and broad adaptability. It enhances PD accumulation in tumor cells both in vitro and in vivo, enhancing the cellular uptake of mono-, di-, and tri-phosphate/phosphonate substrates by up to 45-fold via a macropinocytosis-mediated endocytosis pathway. This work demonstrates the potential of neutral anion receptors to serve as single-molecule carriers and offers a promising solution for improving PDs bioavailability, advancing the development of antitumor phosphate-based drugs.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"78 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114441","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

Delicate Control over Electron Distribution and Water Dissociation Kinetics in Strongly Coupled Ru@NMoC Hybrid Catalyst Realizes Efficient Seawater Electrolysis 强耦合Ru@NMoC杂化催化剂中电子分布和水解离动力学的精细控制实现了高效的海水电解

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-22 DOI: 10.1002/anie.202505031

Jintao Zhao, Jie Wang, Jixin Yao, Liang Li, Dongmeng Chen, Guang Li, Genqiang Zhang

{"title":"Delicate Control over Electron Distribution and Water Dissociation Kinetics in Strongly Coupled Ru@NMoC Hybrid Catalyst Realizes Efficient Seawater Electrolysis","authors":"Jintao Zhao, Jie Wang, Jixin Yao, Liang Li, Dongmeng Chen, Guang Li, Genqiang Zhang","doi":"10.1002/anie.202505031","DOIUrl":"https://doi.org/10.1002/anie.202505031","url":null,"abstract":"Delicate control over electron distribution in hybrid catalysts is crucial for improving hydrogen evolution catalysis, which remains an aspirational target in advancing efficient hydrogen production. Herein, we optimize the local electronic structures and balance the reaction steps by incorporating Ru clusters into nitrogen-doped molybdenum carbide (denoted as Ru@NMoC), addressing performance limitations in alkaline seawater. The Ru@NMoC catalyst demonstrates ultra-low overpotentials of 8, 17, and 20 mV at 10 mA cm⁻² in 1 M KOH, 1 M KOH + 0.5 M NaCl, and 1 M KOH seawater, respectively, significantly outperforming conventional HER catalysts. Operando spectroscopic techniques reveal strong ability for interface water dissociation and stable local charge structure in Ru@NMoC. Theoretical simulations demonstrate that N-doping of Ru clusters self-optimizes their electronic states and lowering the energy barrier for water dissociation. Self-powered H2 production system can be achieved using Zn-H₂O batteries to drive anion exchange membrane water electrolysis cell, demoinstrating its practicability.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"45 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144114458","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

Harmonizing Nanoparticle Exsolution from Ce‐Sm Oxide Matrix for Stable Methane Dry Reforming 甲烷稳定干重整中Ce - Sm氧化基纳米粒子的协调析出

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-22 DOI: 10.1002/anie.202503997

Yongjie Ye, Haofan Lei, Yuanbin Qin, Zhen Wang, Sunpei Hu, Tao Zhou, Lijun Zhang, Ruyang Wang, Zizhen Xiao, Xinhua Gao, Qingxiang Ma, Shucheng Shi, Hui Zhang, Han Yan, Shiming Zhou, Chao Ma, Zhi Liu, Jing Tao, Jie Zeng

{"title":"Harmonizing Nanoparticle Exsolution from Ce‐Sm Oxide Matrix for Stable Methane Dry Reforming","authors":"Yongjie Ye, Haofan Lei, Yuanbin Qin, Zhen Wang, Sunpei Hu, Tao Zhou, Lijun Zhang, Ruyang Wang, Zizhen Xiao, Xinhua Gao, Qingxiang Ma, Shucheng Shi, Hui Zhang, Han Yan, Shiming Zhou, Chao Ma, Zhi Liu, Jing Tao, Jie Zeng","doi":"10.1002/anie.202503997","DOIUrl":"https://doi.org/10.1002/anie.202503997","url":null,"abstract":"Catalyst deactivation hinders the application of high‐temperature catalysis such as methane dry reforming, where nanoparticle exsolution will likely clear the path. However, the harsh reaction conditions often easily unbalance the exsolution degree, leading to either sintering or insufficient exsolution of metal nanoparticles. Here, we achieve the fabrication of highly dispersed yet exposed Rh nanoparticles exsolved from the Ce‐Sm oxide matrix. Starting from examining the metal‐support interaction of Rh‐CeO2 and Rh‐Sm2O3, the exsolution dynamics of Rh nanoparticles are studied via multiple in‐situ techniques. Rapid exsolution from CeO2 induces Rh sintering and catalytic deactivation, while sluggish exsolution from Sm2O3 results in Rh encapsulation with poor activity. The balanced metal‐support interaction harmonizes the exsolution of Rh nanoparticles from the Ce‐Sm oxide matrix, fabricating an anti‐sintering and coke‐resistant catalyst for methane dry reforming. This work provides insights into the development of catalysts with structural robustness, where the essence lies in the engineering of nanoparticle exsolution.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"133 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144113917","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

Unlocking Durable and Sustainable Zinc-Iodine Batteries via Molecularly Engineered Polyiodide Reservoirs 通过分子工程聚碘化物储层解锁耐用和可持续的锌碘电池

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-21 DOI: 10.1002/anie.202506822

Leiqian Zhang, Ke Luo, Jiaming Gong, Yazhou Zhou, Hele Guo, Yi Yu, Guanjie He, Jean-François Gohy, Ivan P. Parkin, Johan Hofkens, Qing He, Tianxi Liu, Klaus Müllen, Feili Lai

{"title":"Unlocking Durable and Sustainable Zinc-Iodine Batteries via Molecularly Engineered Polyiodide Reservoirs","authors":"Leiqian Zhang, Ke Luo, Jiaming Gong, Yazhou Zhou, Hele Guo, Yi Yu, Guanjie He, Jean-François Gohy, Ivan P. Parkin, Johan Hofkens, Qing He, Tianxi Liu, Klaus Müllen, Feili Lai","doi":"10.1002/anie.202506822","DOIUrl":"https://doi.org/10.1002/anie.202506822","url":null,"abstract":"Zinc-iodine batteries (ZIBs) are promising candidates for safe and sustainable energy storage but are hindered by polyiodide shuttling, leading to rapid capacity decay and limited cyclability. In this work, we propose a “polyiodide reservoirs” concept, utilizing iodophilic covalent organic cages to confine polyiodide through multiple noncovalent interactions. By precisely engineering the nitrogen-active site densities around three-dimensional cavities, these cages evolve from open to near-enclosed structure, achieving molecular-level polyiodide entrapment. The optimized superphane cage (18 N-active sites) enables a ZIB with 90.1% capacity retention after 4000 cycles at 5 C, even under extreme conditions (58.9 wt% iodine content within the cage and an iodine area loading of 3.7 mg cm−2 in the cathode). Importantly, the cage’s solubility-driven regeneration capability retains 85.4% initial capacity over three reuse cycles without stability compromise. This work establishes covalent organic superphanes as a transformative platform for long-life ZIBs, offering a dual solution to shuttle suppression and electrode sustainability through structural confinement and dynamic recyclability.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"41 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104488","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

Substrate Preorganization within Photoactive Pt12L24 Nanospheres for Accelerated Decarboxylation Catalysis at Low Concentrations 光活性Pt12L24纳米球内底物预组织在低浓度下加速脱羧催化

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-21 DOI: 10.1002/anie.202508131

Rens Ham, Joost Reek, bettina baumgartner

引用次数: 0

Blocky Selective Post-Polymerization C–H Functionalization of Polyolefins 聚烯烃块状选择性聚合后C-H功能化

IF 16.6 1区化学

Angewandte Chemie International Edition Pub Date : 2025-05-21 DOI: 10.1002/anie.202507687

Frank Leibfarth, Eliza K. Neidhart, Michelle E. Pomatto, Chris Vasallo, Erin R. Crater, Jill W. Alty, Polyxeni P. Angelopoulou, Erik J. Alexanian, Logan T. Kearney, Robert B. Moore

{"title":"Blocky Selective Post-Polymerization C–H Functionalization of Polyolefins","authors":"Frank Leibfarth, Eliza K. Neidhart, Michelle E. Pomatto, Chris Vasallo, Erin R. Crater, Jill W. Alty, Polyxeni P. Angelopoulou, Erik J. Alexanian, Logan T. Kearney, Robert B. Moore","doi":"10.1002/anie.202507687","DOIUrl":"https://doi.org/10.1002/anie.202507687","url":null,"abstract":"C–H functionalization of commodity polyolefins affords functional materials derived from a high-volume, low-cost resource. However, current post-polymerization modification strategies result in randomly distributed functionalization along the length of the polymer backbone, which has a negative impact on the crystallinity of the resultant polymers, and thus the thermomechanical properties. Here, we demonstrate an amidyl radical mediated C–H functionalization of polyolefins to access blocky microstructures, which exhibit a higher crystalline fraction, larger crystallite size, and improved mechanical properties compared to their randomly functionalized analogues. Taking inspiration from the site-selective C–H functionalization of small molecules, we leverage the steric protection provided by crystallites and target polymer functionalization to amorphous domains in a semicrystalline polyolefin gel. The beneficial outcomes of blocky functionalization are independent of the identity of the pendant functional group that is installed through functionalization. The decoupling of functional group incorporation and crystallinity highlights the promise in accessing non-random microstructures through selective functionalization to circumvent traditional tradeoffs in post-polymerization modification, with potential impact in advanced materials and upcycling plastic waste.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"14 1","pages":""},"PeriodicalIF":16.6,"publicationDate":"2025-05-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144104496","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