Angewandte Chemie International Edition最新文献_第2页

Low-Solvent-Coordination Solvation Structure for Lithium-Metal Batteries via Electric Dipole-Dipole Interaction. 通过电偶极子-偶极子相互作用实现锂金属电池的低溶剂配位溶解结构

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-10-28 DOI: 10.1002/anie.202412703

Cong Kang, Jiaming Zhu, Fanpeng Kong, Xiangjun Xiao, Hua Huo, Yulin Ma, Yueping Xiong, Ying Luo, Taolin Lv, Jingying Xie, Geping Yin

{"title":"Low-Solvent-Coordination Solvation Structure for Lithium-Metal Batteries via Electric Dipole-Dipole Interaction.","authors":"Cong Kang, Jiaming Zhu, Fanpeng Kong, Xiangjun Xiao, Hua Huo, Yulin Ma, Yueping Xiong, Ying Luo, Taolin Lv, Jingying Xie, Geping Yin","doi":"10.1002/anie.202412703","DOIUrl":"10.1002/anie.202412703","url":null,"abstract":"Unveiling inherent interactions among solvents, Li+ ions, and anions are crucial in dictating solvation-desolvation kinetics at the electrode/electrolyte interface. Developing an electrolyte with a low ion-transport barrier and minimal solvent coordination in its interfacial solvation structure is essential for forming an anion-derived solid-electrolyte interface, a key component for high-performance Li-metal batteries. In this study, we harness electric dipole-dipole synergistic interactions to formulate an electrolyte with significantly reduced interfacial solvent coordination. Operando characterization and theoretical analysis reveal that 2-fluoropyridine (FPy) with high dipole preferentially adsorbs onto the Li metal surface. The adsorbed FPy molecule squeezes succinonitrile in the primary solvation sheath through steric hindrance, leading to the formation of an inorganic-rich interphase. Consequently, the introduction of FPy enhances the reversible capacity of the LiCoO2||Li cell, which maintains a capacity of 143 mAh g-1 after 500 cycles at a 1 C rate. Moreover, the cycle life of LiCoO2 batteries with a limited supply of lithium extends from 120 cycles to over 200 cycles. These findings offer a strategy that can be applied broadly to design interfacial solvation structures for various metal-ion/metal-based batteries.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202412703"},"PeriodicalIF":16.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142102495","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

Modifications of Prenyl Side Chains in Natural Product Biosynthesis. 天然产物生物合成过程中烯酰基侧链的修饰。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-11-11 DOI: 10.1002/anie.202415279

Huibin Wang, Yi Yang, Ikuro Abe

引用次数: 0

A High-capacity Benzoquinone Derivative Anode for All-organic Long-cycle Aqueous Proton Batteries. 用于全有机长周期水质子电池的高容量苯醌衍生物阳极

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-11-09 DOI: 10.1002/anie.202412455

Sicheng Wu, Mackenzie Taylor, Haocheng Guo, Shuhao Wang, Chen Han, Jitraporn Vongsvivut, Quentin Meyer, Qian Sun, Junming Ho, Chuan Zhao

{"title":"A High-capacity Benzoquinone Derivative Anode for All-organic Long-cycle Aqueous Proton Batteries.","authors":"Sicheng Wu, Mackenzie Taylor, Haocheng Guo, Shuhao Wang, Chen Han, Jitraporn Vongsvivut, Quentin Meyer, Qian Sun, Junming Ho, Chuan Zhao","doi":"10.1002/anie.202412455","DOIUrl":"10.1002/anie.202412455","url":null,"abstract":"Quinone compounds, with the ability to uptake protons, are promising electrodes for aqueous batteries. However, their applications are limited by the mediocre working potential range and inferior rate performance. Herein, we examined quinones bearing different substituents, and for the first time introduce tetraamino-1,4-benzoquinone (TABQ) as anode material for proton batteries. The strong electron-donating amino groups can effectively narrow the band gap and lower the redox potentials of quinone materials. The protonation of amino groups and the amorphization of structure result in the formation of an intermolecular hydrogen-bond network, supporting Grotthuss-type proton conduction in the electrode with a low activation energy of 192.7 meV. The energy storage mechanism revealed by operando FT-IR and ex situ XPS features a reversible quinone-hydroquinone conversion during cycling. TABQ demonstrates a remarkable specific capacity of 307 mAh g-1 at 1 A g-1, which is one of the highest among organic proton electrodes. An all-organic proton battery of TABQ//TCBQ has also been developed, achieving exceptional stability of 3500 cycles at room temperature and excellent performance at sub-zero temperature.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202412455"},"PeriodicalIF":16.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398790","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

Enhancing Hole Transport Uniformity for Efficient Inverted Perovskite Solar Cells through Optimizing Buried Interface Contacts and Suppressing Interface Recombination. 通过优化埋入式界面接触和抑制界面重组，提高高效反相包晶石太阳能电池的空穴传输均匀性。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-10-22 DOI: 10.1002/anie.202412601

Xilai He, Hui Chen, Jiabao Yang, Tong Wang, Xingyu Pu, Guangpeng Feng, Shiyao Jia, Yijun Bai, Zihao Zhou, Qi Cao, Xuanhua Li

{"title":"Enhancing Hole Transport Uniformity for Efficient Inverted Perovskite Solar Cells through Optimizing Buried Interface Contacts and Suppressing Interface Recombination.","authors":"Xilai He, Hui Chen, Jiabao Yang, Tong Wang, Xingyu Pu, Guangpeng Feng, Shiyao Jia, Yijun Bai, Zihao Zhou, Qi Cao, Xuanhua Li","doi":"10.1002/anie.202412601","DOIUrl":"10.1002/anie.202412601","url":null,"abstract":"[4-(3,6-dimethyl-9H-carbazol-9yl)butyl]phosphonic acid (Me-4PACz) self-assembly material has been recognized as a highly effective approach for mitigating nickel oxide (NiOx) surface-related challenges in inverted perovskite solar cells (IPSCs). However, its uneven film generation and failure to effectively passivate the buried interface defects limit the device's performance improvement potential. Herein, p-xylylenediphosphonic acid (p-XPA) containing bilateral phosphate groups (-PO3H2) is introduced as an interface layer between the NiOx/Me-4PACz and the perovskite layer. P-XPA can flatten the surface of hole transport layer and optimize interface contact. Meanwhile, p-XPA achieves better energy level alignment and promotes interfacial hole transport. In addition, the bilateral -PO3H2 of p-XPA can chelate with Pb2+ and form hydrogen bond with FA+ (formamidinium cation), thereby suppressing buried interface non-radiative recombination loss. Consequently, the IPSC with p-XPA buried interface modification achieves champion power conversion efficiency of 25.87 % (certified at 25.45 %) at laboratory scale (0.0448 cm2). The encapsulated target device exhibits better operational stability. Even after 1100 hours of maximum power point tracking at 50 °C, its efficiency remains at an impressive 82.7 % of the initial efficiency. Molecules featuring bilateral passivation groups optimize interfacial contact and inhibit interfacial recombination, providing an effective approach to enhancing the stability and efficiency of devices.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202412601"},"PeriodicalIF":16.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142078568","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

Experimental and Computational Evidence of a Stable RNA G-Triplex Structure at Physiological Temperature in the SARS-CoV-2 Genome. SARS-CoV-2 基因组中生理温度下稳定的 RNA G 三元结构的实验和计算证据

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-11-06 DOI: 10.1002/anie.202415448

Marco Campanile, Roberto Improta, Luciana Esposito, Chiara Platella, Rosario Oliva, Pompea Del Vecchio, Roland Winter, Luigi Petraccone

引用次数: 0

Hydrogenation Reactions with Heterobimetallic Complexes. 异二金属配合物的加氢反应。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-11-07 DOI: 10.1002/anie.202416100

Preshit C Abhyankar, Christine M Thomas

引用次数: 0

Dynamic Adaptation of Active Site Driven by Dual-side Adsorption in Single-Atomic Catalysts During CO₂ Electroreduction. 单原子催化剂在二氧化碳电还原过程中由双面吸附驱动的活性位点动态适应。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-11-06 DOI: 10.1002/anie.202411765

Nam Van Tran, Jiyuan Liu, Shuzhou Li

{"title":"Dynamic Adaptation of Active Site Driven by Dual-side Adsorption in Single-Atomic Catalysts During CO2 Electroreduction.","authors":"Nam Van Tran, Jiyuan Liu, Shuzhou Li","doi":"10.1002/anie.202411765","DOIUrl":"10.1002/anie.202411765","url":null,"abstract":"Single-atom iron embedded in N-doped carbon (Fe-N-C) is among the most representative single-atomic catalysts (SACs) for electrochemical CO2 reduction reaction (CO2RR). Despite the simplicity of the active site, the CO2-to-CO mechanism on Fe-N-C remains controversial. Firstly, there is a long debate regarding the rate-determining step (RDS) of the reactions. Secondly, recent computational and experimental studies are puzzled by the fact that the CO-poisoned Fe centers still remain highly active at high potentials. Thirdly, there are ongoing challenges in elucidating the high selectivity of hydrogen evolution reaction (HER) over CO2RR at high potentials. In this work, we introduce a novel CO2RR mechanism on Fe-N-C, which was inspired by the dynamic of active sites in biological systems. By employing grand-canonical density functional theory and kinetic Monte-Carlo, we found that the RDS is not fixed but changes with the applied potential. We demonstrated that our proposed dual-side mechanisms could clarify the reason behind the high catalytic activity of CO-poisoned metal centers, as well as the high selectivity of HER over CO2RR at high potential. This study provides a fundamental explanation for long-standing puzzles of an important catalyst and calls for the importance of considering the dynamic of active sites in reaction mechanisms.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202411765"},"PeriodicalIF":16.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142337690","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

Full-Spectrum Light-Harvesting Solar Thermal Electrocatalyst Boosts Oxygen Evolution. 全光谱光收集太阳热电催化剂促进氧气进化。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-10-30 DOI: 10.1002/anie.202412049

Mingxia Xu, Qiming Bing, Yunchuan Tu, Yunlong Zhang, Mo Zhang, Yafeng Cai, Jinlei Li, Xianguang Meng, Jia Zhu, Liang Yu, Dehui Deng

{"title":"Full-Spectrum Light-Harvesting Solar Thermal Electrocatalyst Boosts Oxygen Evolution.","authors":"Mingxia Xu, Qiming Bing, Yunchuan Tu, Yunlong Zhang, Mo Zhang, Yafeng Cai, Jinlei Li, Xianguang Meng, Jia Zhu, Liang Yu, Dehui Deng","doi":"10.1002/anie.202412049","DOIUrl":"10.1002/anie.202412049","url":null,"abstract":"Enabling high-efficiency solar thermal conversion (STC) at catalytic active site is critical but challenging for harnessing solar energy to boost catalytic reactions. Herein, we report the direct integration of full-spectrum STC and high electrocatalytic oxygen evolution activity by fabricating a hierarchical nanocage architecture composed of graphene-encapsulated CoNi nanoparticle. This catalyst exhibits a near-complete 98 % absorptivity of solar spectrum and a high STC efficiency of 97 %, which is superior than previous solar thermal catalytic materials. It delivers a remarkable potential decrease of over 240 mV at various current densities for electrocatalytic oxygen evolution under solar illumination, which is practically unachievable via traditionally heating the system. The high-efficiency STC is enabled by a synergy between the regulated electronic structure of graphene via CoNi-carbon interaction and the multiple absorption of lights by the light-trapping nanocage. Theoretical calculations suggest that high temperature-induced vibrational free energy gain promotes the potential-limiting *O to *OOH step, which decreases the overpotential for oxygen evolution.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202412049"},"PeriodicalIF":16.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142131336","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

6-Hydroxy Picolinohydrazides Promoted Cu(I)-Catalyzed Hydroxylation Reaction in Water: Machine-Learning Accelerated Ligands Design and Reaction Optimization. 6-Hydroxy Picolinohydrazides Promoted Cu(I)-Catalyzed Hydroxylation Reaction in Water：机器学习加速配体设计和反应优化。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-10-25 DOI: 10.1002/anie.202412552

Lanting Xu, Jiazhou Zhu, Xiaodong Shen, Jiashuang Chai, Lei Shi, Bin Wu, Wei Li, Dawei Ma

{"title":"6-Hydroxy Picolinohydrazides Promoted Cu(I)-Catalyzed Hydroxylation Reaction in Water: Machine-Learning Accelerated Ligands Design and Reaction Optimization.","authors":"Lanting Xu, Jiazhou Zhu, Xiaodong Shen, Jiashuang Chai, Lei Shi, Bin Wu, Wei Li, Dawei Ma","doi":"10.1002/anie.202412552","DOIUrl":"10.1002/anie.202412552","url":null,"abstract":"Hydroxylated (hetero)arenes are privileged motifs in natural products, materials, small-molecule pharmaceuticals and serve as versatile intermediates in synthetic organic chemistry. Herein, we report an efficient Cu(I)/6-hydroxy picolinohydrazide-catalyzed hydroxylation reaction of (hetero)aryl halides (Br, Cl) in water. By establishing machine learning (ML) models, the design of ligands and optimization of reaction conditions were effectively accelerated. The N-(1,3-dimethyl-9H- carbazol-9-yl)-6-hydroxypicolinamide (L32, 6-HPA-DMCA) demonstrated high efficiency for (hetero)aryl bromides, promoting hydroxylation reactions with a minimal catalyst loading of 0.01 mol % (100 ppm) at 80 °C to reach 10000 TON; for substrates containing sensitive functional groups, the catalyst loading needs to be increased to 3.0 mol % under near-room temperature conditions. N-(2,7-Di-tert-butyl-9H-carbazol-9-yl)-6-hydroxypicolinamide (L42, 6-HPA-DTBCA) displayed superior reaction activity for chloride substrates, enabling hydroxylation reactions at 100 °C with 2-3 mol % catalyst loading. These represent the state of art for both lowest catalyst loading and temperature in the copper-catalyzed hydroxylation reactions. Furthermore, this method features a sustainable and environmentally friendly solvent system, accommodates a wide range of substrates, and shows potential for developing robust and scalable synthesis processes for key pharmaceutical intermediates.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202412552"},"PeriodicalIF":16.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142071506","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

Highly Efficient Near-Infrared Luminescent Radicals with Emission Peaks over 750 nm. 具有 750 纳米以上发射峰的高效近红外发光自由基。

IF 16.1 1区化学

Angewandte Chemie International Edition Pub Date : 2024-12-20 Epub Date: 2024-10-24 DOI: 10.1002/anie.202412483

Chunxiao Wu, Chen Lu, Shilong Yu, Minzhe Zhang, Houyu Zhang, Ming Zhang, Feng Li

{"title":"Highly Efficient Near-Infrared Luminescent Radicals with Emission Peaks over 750 nm.","authors":"Chunxiao Wu, Chen Lu, Shilong Yu, Minzhe Zhang, Houyu Zhang, Ming Zhang, Feng Li","doi":"10.1002/anie.202412483","DOIUrl":"10.1002/anie.202412483","url":null,"abstract":"Purely organic molecules exhibiting near-infrared (NIR) emission possess considerable potential for applications in both biological and optoelectronic technological domains, owing to their inherent advantages such as cost-effectiveness, biocompatibility, and facile chemical modifiability. However, the repertoire of such molecules with emission peaks exceeding 750 nm and concurrently demonstrating high photoluminescence quantum efficiency (PLQE) remains relatively scarce due to the energy gap law. Herein, we report two open-shell NIR radical emitters, denoted as DMNA-Cz-BTM and DMNA-PyID-BTM, achieved through the strategic integration of a donor group (DMNA) onto the Cz-BTM and PyID-BTM frameworks, respectively. We found that the donor-acceptor molecular structure allows the two designed radical emitters to exhibit a charge-transfer excited state and spatially separated electron and hole levels with non-bonding characteristics. Thus, the high-frequency vibrations are effectively suppressed. Besides, the reduction of low-frequency vibrations is observed. Collectively, the non-radiative decay channel is significantly suppressed, leading to exceptional NIR PLQE values. Specifically, DMNA-Cz-BTM manifests an emission peak at 758 nm alongside a PLQE of 55 %, whereas DMNA-PyID-BTM exhibits an emission peak at 778 nm with a PLQE of 66 %. Notably, these represent the pinnacle of PLQE among metal-free organic NIR emitters with emission peaks surpassing 750 nm.","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":" ","pages":"e202412483"},"PeriodicalIF":16.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142102490","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