Angewandte Chemie最新文献_第10页

Concise Total Syntheses of Leuconoxine-Type Alkaloids Enabled by Palladium/Norbornene-Catalyzed Pyrrole Difunctionalization 钯/降冰片烯催化吡咯双官能化合成白参醇类生物碱的简捷全合成

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202502736

Xin Liu, Yun Zhou, Yu Meng, Qi Zhu, Renhe Li, Guangbin Dong

引用次数: 0

Potassium Tetraiodatoiodate(III) Iodate(V): A Nonlinear Optical Crystal with Exceptional Second-Harmonic Generation and Full-Wavelength Phase Matching 四碘酸钾（III）碘酸钾(V)：一种具有特殊二次谐波产生和全波长相位匹配的非线性光学晶体

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202504673

Min-Quan Lin, Chun-Li Hu, Meng-Fan Duan, Bing-Xuan Li, Jiang-Gao Mao, Bing-Ping Yang

{"title":"Potassium Tetraiodatoiodate(III) Iodate(V): A Nonlinear Optical Crystal with Exceptional Second-Harmonic Generation and Full-Wavelength Phase Matching","authors":"Min-Quan Lin, Chun-Li Hu, Meng-Fan Duan, Bing-Xuan Li, Jiang-Gao Mao, Bing-Ping Yang","doi":"10.1002/ange.202504673","DOIUrl":"https://doi.org/10.1002/ange.202504673","url":null,"abstract":"The development of nonlinear optical materials with large nonlinear optical susceptibilities, wide transmission ranges, and comprehensive full-wavelength phase matching capabilities remains a significant challenge. In this study, we synthesized a novel potassium tetraiodatoiodate(III) iodate(V) via an in-situ reduction and complexation reaction. The resulting compound, K2[IIII(IVO3)4]IVO3, exhibits exceptional second-harmonic generation responses (21.6KH2PO4 at 1064 nm, 1.0KTiOPO4 at 2050 nm), a wide transparency range from the visible to the mid-infrared wavelengths (0.37–6.05 and 7.03–13.40 µm), and a high birefringence (0.358 at 543 nm) to achieve full-wavelength phase matching. These properties are primarily ascribed to the synergistic substantial hyperpolarizability and polarizability anisotropy exhibited by the [IIII(IVO3)4]− complex ions, which comprise square-planar coordinated trivalent iodine and optimally arranged iodate ligands. This study demonstrates the pivotal role of nonmetallic cation centered coordination entities in influencing linear and nonlinear optical properties, a discovery that has significant implications for the development of innovative inorganic functional materials.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179288","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

Regioselective Nickel-Catalyzed Hydroarylation of gem-Difluoroalkenes for the Synthesis of the Moiety 区域选择性镍催化的宝石-二氟烯烃氢芳基化合成

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202424714

Xiangyu Chen, Yaxing Wu, Ruitong Zhang, Fei Wang, Chao Chen

引用次数: 0

Removing α-H in Carboxylate-Based Electrolytes for Stable Lithium Metal Batteries 稳定锂金属电池羧酸基电解质中α-H的去除

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202503616

Yi Yang, Le-Geng Yu, Yu-Xin Huang, Xiao-Qing Ding, Zhou-Qing Xue, Zeheng Li, Yu-Xing Yao, Shuo Zhang, Lei Xu, Xue-Fei Wen, Jian Pei, Chong Yan, Jia-Qi Huang

{"title":"Removing α-H in Carboxylate-Based Electrolytes for Stable Lithium Metal Batteries","authors":"Yi Yang, Le-Geng Yu, Yu-Xin Huang, Xiao-Qing Ding, Zhou-Qing Xue, Zeheng Li, Yu-Xing Yao, Shuo Zhang, Lei Xu, Xue-Fei Wen, Jian Pei, Chong Yan, Jia-Qi Huang","doi":"10.1002/ange.202503616","DOIUrl":"https://doi.org/10.1002/ange.202503616","url":null,"abstract":"Although carboxylate esters greatly improve the cold weather performance of graphite-based lithium-ion batteries utilized in arctic expeditions, the underlying cause of the incompatibility between carboxylates and lithium (Li) anodes has not been sufficiently explained, resulting in the greatly restricted usage of carboxylate in lithium metal batteries (LMBs). Herein, we reveal the serious parasitic reactions between carboxylate α-H atoms and Li metal are the culprits that render carboxylate-based ineffectiveness for LMBs. By replacing all α-H atoms with fluorine atoms and methyl groups, we successfully construct inert carboxylates and find the ions/molecules distribution in electric-double-layer (EDL) can be manipulated at a molecular-level. The unique structure ensuring more anions are positioned closer to the Li surface in the EDL of the inert carboxylate-based electrolyte, the morphology of the deposited Li is significantly regulated and the chemical corrosion gets effectively inhibited, as a consequence of remarkable extending lifespan of carboxylate-based LMBs with routine salt concentration and few additives. More generally, using carboxylates lacking α-H atoms offer a realistic approach to increase the variety of solvents that can be used in LMBs electrolytes.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179344","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

Constructing Robust Electrode/Electrolyte Interphases for Highly Stable Lithium–Sulfurized Polyacrylonitrile Batteries 高稳定锂硫化聚丙烯腈电池电极/电解质界面的构建

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202503214

Siyuan Shao, Jinze Hou, Youxuan Ni, Chunyan Zhu, Shuang Wu, Xinyi Liu, Can Wang, Kai Zhang, Zhenhua Yan, Yong Lu, Jun Chen

{"title":"Constructing Robust Electrode/Electrolyte Interphases for Highly Stable Lithium–Sulfurized Polyacrylonitrile Batteries","authors":"Siyuan Shao, Jinze Hou, Youxuan Ni, Chunyan Zhu, Shuang Wu, Xinyi Liu, Can Wang, Kai Zhang, Zhenhua Yan, Yong Lu, Jun Chen","doi":"10.1002/ange.202503214","DOIUrl":"https://doi.org/10.1002/ange.202503214","url":null,"abstract":"Lithium–sulfurized polyacrylonitrile (SPAN) batteries show great promise for energy storage, but are plagued by poor cycling stability, which can be attributed to unfavorable electrode/electrolyte interphases for both anode and cathode. Here we design and achieve the anion-moderate solvation structure based interconnected clusters in electrolyte by regulating the interactions of solvent with Li+ and diluent to construct robust anode/electrolyte and cathode/electrolyte interphases simultaneously for high-performance Li–SPAN batteries. The optimal electrolyte endows Li plating/stripping with a high Coulombic efficiency of 99.47% at 1 mA cm−2 in Li||Cu cells. The Li–SPAN batteries show excellent cycling stability with a high capacity retention of 94.21% after 1215 cycles. Moreover, the assembled pouch-type Li–SPAN battery under limited electrolyte condition (2.40 g Ah−1) achieves a capacity of 3.75 Ah, corresponding to a high energy density of 180 Wh kg−1 based on the total mass of the battery. This work provides a good electrolyte design principle to construct robust anode/electrolyte and cathode/electrolyte interphases for batteries.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 22","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144140818","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

Controlling the Chirality of Metallo-Cages by Manipulating the Stereochemistry of the Metal Centers 通过操纵金属中心的立体化学来控制金属笼的手性

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202503833

Yu-Qing Li, Lei Fu, Zhiyuan Jiang, Ermeng Han, Tian Li, Qixia Bai, Ting-Zheng Xie, Zhe Zhang, Pingshan Wang, Tun Wu

{"title":"Controlling the Chirality of Metallo-Cages by Manipulating the Stereochemistry of the Metal Centers","authors":"Yu-Qing Li, Lei Fu, Zhiyuan Jiang, Ermeng Han, Tian Li, Qixia Bai, Ting-Zheng Xie, Zhe Zhang, Pingshan Wang, Tun Wu","doi":"10.1002/ange.202503833","DOIUrl":"https://doi.org/10.1002/ange.202503833","url":null,"abstract":"Precise control over the chirality of metallo-cages by manipulating the stereochemistry of metal centers is important in many practical applications, but is extremely challenging. In this study, two isostructural metallo-cuboctahedra (1-ZnII12L18 and 2-CdII12L18) have been assembled using ligand L1 and two kinds of metal ions (ZnII and CdII) with similar coordination lability. The chiral-induction by the same guests (D-/L-camphorsulfonate, D-/L-SCS) results in a completely opposing stereochemical output of 1 and 2: D-SCS induced host–guest complex of [D-SCS⊂Δ12–1] and [D-SCS⊂Λ12–2], respectively, with reverse handedness. The distinct stereochemical configuration of metallo-cuboctahedra can be manipulated by participant metal ions that exhibit similar dynamics. Furthermore, a subtle variation of the ligand peripheral substituent group facilitates spontaneous resolution of metallo-cuboctahedra 3-ZnII12L28 from a racemic mixture as (R24, Λ12)-3/(S24, Δ12)-3 enantiopure entities. The dynamic stereochemistry of MII12L8 cuboctahedra described in this work allows a chiral manipulation based on the nature of metal centers and ligands, enabling the design and control of the chirality of metallo-cages.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179271","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

Pressure-Induced Emission Luminogens Enable Optical Logic Gates Toward Lighting, Scintillators, and Anti-Counterfeiting 压力致发射发光源使光学逻辑门可用于照明、闪烁体和防伪

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202504913

Wenya Zhao, Guanjun Xiao, Shi Qiu, Yuchen Shang, Yue Qin, Jiayi Yang, Jingtian Wang, Jiajia Ning, Yanjun Fang, Qingfeng Dong, Zhaodong Liu, Shunxin Li, Junfeng Gao, Bo Zou

{"title":"Pressure-Induced Emission Luminogens Enable Optical Logic Gates Toward Lighting, Scintillators, and Anti-Counterfeiting","authors":"Wenya Zhao, Guanjun Xiao, Shi Qiu, Yuchen Shang, Yue Qin, Jiayi Yang, Jingtian Wang, Jiajia Ning, Yanjun Fang, Qingfeng Dong, Zhaodong Liu, Shunxin Li, Junfeng Gao, Bo Zou","doi":"10.1002/ange.202504913","DOIUrl":"https://doi.org/10.1002/ange.202504913","url":null,"abstract":"The pressure-induced emission luminogens (PIEgens) opened the door to highly emissive materials. However, the high-pressure phase with excellent optoelectrical properties is difficult to stabilize at ambient conditions, seriously limiting the practical applications. Here, we first lighted up non-emissive zero-dimensional (0D) metal halide (C25H22P)2SnCl6 via pressure engineering, ultimately yielding the bright emission. Note that the quenched (C25H22P)2SnCl6 after pressure treatment of 20.0 GPa exhibited very bright blue–white emission. This irreversible photoluminescence (PL) transition was associated with irreversible amorphization by increasing the potential barrier of phase transition through the steric hindrance effect. The increased distortion of inorganic octahedra and the enhanced hydrogen bond interaction within the amorphous (C25H22P)2SnCl6 after pressure treatment were responsible for the bright emission. Thus, pressure-triggered PL turn-on behavior can serve as a robust optical switchable logic gate from the initially dark state “0” to the bright state “1”. Furthermore, the pressure-treated (C25H22P)2SnCl6 exhibited an unexpected excitation-dependent emission. The unique characteristic of “PIE” with different colors can be decoded the Morse code encrypted with the pressure-treated (C25H22P)2SnCl6 and different excitations. The quenched (C25H22P)2SnCl6-based phosphor-converted light-emitting diodes (pc-LEDs), X-ray dose rate detection and centimeter-level patterns highlighted great potentials in lighting, display, scintillators, and anti-counterfeiting.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179289","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

Oxygen Atom Migration Dominates Anomalous Reversible Oxidation of Ru Nanosheets 氧原子迁移主导了钌纳米片的异常可逆氧化

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202502927

Xiong Xiao, Yongli Shen, Wei Xi, Lin Gu, Xiaogang Li, Baojuan Xi, Shenglin Xiong, Changhua An

{"title":"Oxygen Atom Migration Dominates Anomalous Reversible Oxidation of Ru Nanosheets","authors":"Xiong Xiao, Yongli Shen, Wei Xi, Lin Gu, Xiaogang Li, Baojuan Xi, Shenglin Xiong, Changhua An","doi":"10.1002/ange.202502927","DOIUrl":"https://doi.org/10.1002/ange.202502927","url":null,"abstract":"Oxidation is a ubiquitous reaction in nature. For most metals (especially metal nanoparticles [NPs]), they will be completely oxidized under suitable conditions, except ruthenium (Ru). In this work, in situ transmission electron microscopy (in situ TEM) and ex situ spectroscopy were employed to investigate the oxidation process of Ru nanosheets. Ex situ spectroscopic analysis demonstrates the incomplete oxidation of Ru nanosheets to RuO₂, while the in situ TEM observations uncover an anomalous reverse phase transformation from the oxidized to metallic phase during oxidation. Combined with theoretical calculations, the oxygen atom migration dominates the reversible oxidation process, strikingly distinct from the unidirectional oxidation pathways in conventional metallic systems. The as-generated abundant Ru─RuO2 heterointerfaces formed through reversible oxidation provide a wealth of active sites for electrochemical alkaline hydrogen evolution reaction (HER). Herein, the study not only lays a foundation for the understanding complex dynamic oxidation processes, but also offers new insights into the design of nanocatalysts.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179342","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

Harnessing Molecular Recognition for Small-Molecule-Mediated Reversible Photochemical Control Over mRNA Translation 利用分子识别对mRNA翻译进行小分子介导的可逆光化学控制

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202503078

Shaifaly Parmar, Logan Tenney, Xiao Liang, John T. Routzahn IV, Christopher D. Sibley, John S. Schneekloth Jr.

引用次数: 0

Cold-Optimized Zinc-Ion Batteries: Enhanced Stability at −5 °C 冷优化锌离子电池：在- 5°C下增强稳定性

Angewandte Chemie Pub Date : 2025-03-31 DOI: 10.1002/ange.202503435

Jianming Meng, Yulai Lin, Yuqing Wang, Peng Hei, Ya Sai, Jing Wang, Xiaoqi Sun, Xiao-Xia Liu, Yu Song

{"title":"Cold-Optimized Zinc-Ion Batteries: Enhanced Stability at −5 °C","authors":"Jianming Meng, Yulai Lin, Yuqing Wang, Peng Hei, Ya Sai, Jing Wang, Xiaoqi Sun, Xiao-Xia Liu, Yu Song","doi":"10.1002/ange.202503435","DOIUrl":"https://doi.org/10.1002/ange.202503435","url":null,"abstract":"Aqueous zinc-ion batteries (AZIBs) have been extensively studied under room and ultralow temperature conditions. However, mechanism studies at intermediate temperature ranges remain limited. In this work, we investigate the electrochemical performance of an AZIB using a commonly employed 3 M ZnSO4 electrolyte across the intermediate temperature range of 25 to −15 °C. Notably, we find that the battery with a double hydroxide cathode exhibits optimized performance at −5 °C, demonstrating significantly enhanced cycling stability compared to 25 °C. Mechanistic studies reveal that unfavorable H+-associated reactions at both the cathode and anode are effectively alleviated at −5 °C, contributing to improved cycling stability. Spectroscopic and theoretical analyzes show that changes in the electrolyte environment at −5 °C—such as reduced electrochemical activity of H2O, increased H-bond strength, and decreased total number of H bonds—impede H+ diffusion through H-bond network via the Grotthuss mechanism. These effects collectively suppress harmful H+-associated reactions, allowing Zn2+ insertion/deinsertion to dominate the charge storage process. This work provides valuable insights into the enhanced performance of AZIBs at sublow temperatures and presents opportunities for extending battery operation in near-freezing environments.","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 23","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144179343","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