Journal of the American Chemical Society最新文献_第8页

Poly(Ionic Liquid) Electrolytes at an Extreme Salt Concentration for Solid-State Batteries. 用于固态电池的极端盐浓度聚（离子液体）电解质。

IF 14.4 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-18 DOI: 10.1021/jacs.4c12616

Shinji Kondou, Mohanad Abdullah, Ivan Popov, Murillo L Martins, Luke A O'Dell, Hiroyuki Ueda, Faezeh Makhlooghiazad, Azusa Nakanishi, Taku Sudoh, Kazuhide Ueno, Masayoshi Watanabe, Patrick Howlett, Heng Zhang, Michel Armand, Alexei P Sokolov, Maria Forsyth, Fangfang Chen

{"title":"Poly(Ionic Liquid) Electrolytes at an Extreme Salt Concentration for Solid-State Batteries.","authors":"Shinji Kondou, Mohanad Abdullah, Ivan Popov, Murillo L Martins, Luke A O'Dell, Hiroyuki Ueda, Faezeh Makhlooghiazad, Azusa Nakanishi, Taku Sudoh, Kazuhide Ueno, Masayoshi Watanabe, Patrick Howlett, Heng Zhang, Michel Armand, Alexei P Sokolov, Maria Forsyth, Fangfang Chen","doi":"10.1021/jacs.4c12616","DOIUrl":"10.1021/jacs.4c12616","url":null,"abstract":"Polymer-in-salt electrolytes were introduced three decades ago as an innovative solution to the challenge of low Li-ion conductivity in solvent-free solid polymer electrolytes. Despite significant progress, the approach still faces considerable challenges, ranging from a fundamental understanding to the development of suitable polymers and salts. A critical issue is maintaining both the stability and high conductivity of molten salts within a polymer matrix, which has constrained their further exploration. This research offers a promising solution by integrating cationic poly(ionic liquids) (polyIL) with a crystallization-resistive salt consisting of asymmetric anions. A stable polymer-in-salt electrolyte with an exceptionally high Li-salt content of up to 90 mol % was achieved, providing a valuable opportunity for the in-depth understanding of these electrolytes at an extremely high salt concentration. This work explicates how increased salt concentration affects coordination structures, glass transitions, ionic conductivity, and the decoupling and coupling of ion transport from structural dynamics in a polymer electrolyte, ultimately enhancing electrolyte performance. These findings provide significant knowledge advancement in the field, guiding the future design of polymer-in-salt electrolytes.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":""},"PeriodicalIF":14.4,"publicationDate":"2024-11-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142666193","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

Solvent-Directed Social Chiral Self-Sorting in Pd₂L₄ Coordination Cages. Pd2L4 配位笼中溶剂引导的社会手性自分类。

IF 14.4 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-17 DOI: 10.1021/jacs.4c12525

Alexandre Walther, Gers Tusha, Björn Schmidt, Julian J Holstein, Lars V Schäfer, Guido H Clever

{"title":"Solvent-Directed Social Chiral Self-Sorting in Pd2L4 Coordination Cages.","authors":"Alexandre Walther, Gers Tusha, Björn Schmidt, Julian J Holstein, Lars V Schäfer, Guido H Clever","doi":"10.1021/jacs.4c12525","DOIUrl":"10.1021/jacs.4c12525","url":null,"abstract":"A family of Pd2L4 cages prepared from ligands based on an axially chiral diamino-[1,1'-biazulene] motif (serving as a unique azulene-based surrogate of the ubiquitous BINOL moiety) is reported. We show that preparing a cage starting from the racemate of a shorter bis-monodentate ligand derivative, equipped with pyridine donor groups, leads to integrative (\"social\") chiral self-sorting, exclusively yielding the meso-trans product, but only in a selection of solvents. This phenomenon is driven by individual solvent molecules acting as hydrogen bonding tethers between the amino groups of neighboring ligands, thereby locking the final coordination cage in a single isomeric form. The experimental (solvent-dependent NMR, single-crystal X-ray diffraction) observations of this cooperative interaction could be explained by computational analyses only when explicit solvation was considered. Furthermore, we prepared a larger chiral ligand with isoquinoline donors, which, unlike the first one, does not undergo social self-sorting from its racemic mixture, further highlighting the importance of solvents bridging short distances between the amino groups. Homochiral cages formed from this larger ligand, however, furnish a cavity that can bind anionic and neutral metal complexes such as [Pt(CN)6]2- and Cr(CO)6 and discriminate between the two enantiomers of chiral guest camphor sulfonate.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":""},"PeriodicalIF":14.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643401","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

Manganese Oxide-Incorporated Hybrid Lipid Nanoparticles Amplify the Potency of mRNA Vaccine via Oxygen Generation and STING Activation. 氧化锰掺杂混合脂质纳米颗粒通过氧气生成和 STING 激活增强 mRNA 疫苗的效力

IF 14.4 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-17 DOI: 10.1021/jacs.4c12166

Jinqun Gan, Jiaqi Lei, Yongcan Li, Meixin Lu, Xinyang Yu, Guocan Yu

{"title":"Manganese Oxide-Incorporated Hybrid Lipid Nanoparticles Amplify the Potency of mRNA Vaccine via Oxygen Generation and STING Activation.","authors":"Jinqun Gan, Jiaqi Lei, Yongcan Li, Meixin Lu, Xinyang Yu, Guocan Yu","doi":"10.1021/jacs.4c12166","DOIUrl":"https://doi.org/10.1021/jacs.4c12166","url":null,"abstract":"Messenger RNA (mRNA) vaccines have exhibited enormous potential in the treatment of human diseases; however, their widespread applications are curtailed by the induction of reactive oxygen species during mRNA translation, which greatly compromises the translation efficiency. Herein, we present a robust strategy with the capability to substantially enhance the efficacy of the mRNA vaccine through promoting mRNA translation and stimulator of interferon genes (STING) activation. The strategy entails the coassembly of small-sized manganese oxide nanoparticles (Mn3O4 NPs) with lipid nanoparticles (LNPs) as the hybrid delivery vehicle (MnLNPs) for the fabrication of mRNA vaccine. The acquired MnLNPs proficiently scavenge reactive oxygen species (ROS) produced during mRNA translation and facilitate oxygen production, thereby boosting adenosine triphosphate (ATP) synthesis and augmenting mRNA translation. Furthermore, MnLNPs effectively bolster the antigen presentation and maturation of dendritic cells by activating the cGAS-STING pathway. In vivo studies demonstrate that mRNA vaccine prepared from MnLNPs markedly enhances the translation of antigen-encoding mRNA compared to LNPs, leading to superior antitumor efficacy. The tumor-suppressive capabilities of MnLNPs@mRNA are further promoted by synergizing with immune checkpoint blockade, underscoring MnLNPs-based mRNA vaccine as an exceptionally promising avenue in cancer immunotherapy.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":""},"PeriodicalIF":14.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646407","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

Excited State Dynamics of Geometrical Evolution of α-Substituted Dibenzoylmethanatoboron Difluoride Complex with Aggregation-Induced Emission Property. 具有聚集诱导发射特性的α-取代二苯甲酰甲硼二氟化物配合物几何演化的激发态动力学。

IF 14.4 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-17 DOI: 10.1021/jacs.4c10277

Yushi Fujimoto, Yoshifumi Mochiduki, Hikaru Sotome, Rintaro Shimada, Hajime Okajima, Yasunori Toda, Akira Sakamoto, Hiroshi Miyasaka, Fuyuki Ito

{"title":"Excited State Dynamics of Geometrical Evolution of α-Substituted Dibenzoylmethanatoboron Difluoride Complex with Aggregation-Induced Emission Property.","authors":"Yushi Fujimoto, Yoshifumi Mochiduki, Hikaru Sotome, Rintaro Shimada, Hajime Okajima, Yasunori Toda, Akira Sakamoto, Hiroshi Miyasaka, Fuyuki Ito","doi":"10.1021/jacs.4c10277","DOIUrl":"https://doi.org/10.1021/jacs.4c10277","url":null,"abstract":"Organic molecules with an aggregation-induced emission (AIE) property have been attracting much attention from the viewpoint of application to solid state emissive materials. For the AIE mechanism, quantum mechanical studies proposed the restriction of the intramolecular motion (RIM) model with the contribution of the conical intersection (CI) and deduced the importance of the restricted access to a conical intersection (RACI) in the potential energy surface (PES). Although these theoretical studies have contributed to the elucidation of AIE phenomena, direct detection of the reaction dynamics is indispensable to clarify the actual PES and the deactivation mechanism. Along this line, we investigated excited state dynamics of the AIE molecule with dibenzoylmethanatoboron difluoride complexes using time-resolved absorption spectroscopies in both visible and infrared (IR) regions. While the reference system of 1,3-bis(4-methoxyphenyl)methanatoboron difluoride (2aBF2) showed strong emission in solution, the methyl-substituted derivative at the α-position of the dioxaborine ring (2amBF2) led to the very weak fluorescence in solution but strong emission in the solid state. Time-resolved visible absorption measurements revealed a peak shift and broadening of the stimulated emission in the solution of 2amBF2, owing to the rapid change of the molecular geometry. With the temporal evolution of time-resolved IR absorption signals and density functional theory (DFT) calculation of these systems, it was deduced that 2amBF2 has two stable geometries, namely, planar and bending, in the S1 state and the bending geometry in the S1 state led to rapid conversion to the S0 state. These results support the RACI model in the aggregated states, leading to the AIE properties.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":""},"PeriodicalIF":14.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142643291","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

Ammonia Synthesis with Visible Light and Quantum Dots. 利用可见光和量子点合成氨。

IF 14.4 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-17 DOI: 10.1021/jacs.4c06713

Vanshika Jain, Shreya Tyagi, Pradyut Roy, Pramod P Pillai

{"title":"Ammonia Synthesis with Visible Light and Quantum Dots.","authors":"Vanshika Jain, Shreya Tyagi, Pradyut Roy, Pramod P Pillai","doi":"10.1021/jacs.4c06713","DOIUrl":"https://doi.org/10.1021/jacs.4c06713","url":null,"abstract":"Light-assisted synthesis of ammonia from nitrate and nitrite sources is a sustainable approach to reduce the burden of the energy-intensive Haber-Bosch process. However, poor selectivity and the need for UV-active photocatalysts are the current bottlenecks in the synthesis of ammonia from nitrate and nitrite sources. Herein, we introduce selective visible-light-driven ammonia production from nitrate and nitrite ions with indium phosphide quantum dots (InP QDs) as the photocatalyst. The presence of catalytic indium sites and microenvironment modulation through an interplay of catalyst-reactant interactions resulted in efficient and selective ammonia formation under visible light. Ammonia was produced in an attractive yield of ∼94% in both aqueous and gaseous phases within 2 h of visible-light irradiation at room temperature. A decent formation of ammonia was observed under sunlight as well, strengthening the translational prospects of InP QD photocatalysts. Mechanistic investigations ascertained a negligible role of competing hydrogen evolution in direct nitrate reduction, confirming the active participation of photoexcited charge carriers from InP QDs in the ammonia synthesis. Kinetic studies revealed the energetically challenging nitrate-to-nitrite conversion as the rate-determining step, with subsequent reactions proceeding with ∼100% conversion to yield ammonia. A series of experiments concluded that water is the proton source in the InP QD-photocatalyzed synthesis of ammonia. Our study shows the impact of the rationally designed core and surface of InP QD-based photocatalysts in developing sustainable routes to produce ammonia beyond the Haber-Bosch process.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":" ","pages":""},"PeriodicalIF":14.4,"publicationDate":"2024-11-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142646405","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

Length and Sequence-Selective Polymer Synthesis Templated by a Combination of Covalent and Noncovalent Base-Pairing Interactions 以共价和非共价碱基配对相互作用组合为模板的长度和序列选择性聚合物合成

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-16 DOI: 10.1021/jacs.4c13452

Federica Balduzzi, Vihanga Munasinghe, Oliver N. Evans, Agustin Lorusso Notaro Francesco, Cecilia J. Anderson, Salvatore Nigrelli, Luis Escobar, Rafel Cabot, Joseph T. Smith, Christopher A. Hunter

{"title":"Length and Sequence-Selective Polymer Synthesis Templated by a Combination of Covalent and Noncovalent Base-Pairing Interactions","authors":"Federica Balduzzi, Vihanga Munasinghe, Oliver N. Evans, Agustin Lorusso Notaro Francesco, Cecilia J. Anderson, Salvatore Nigrelli, Luis Escobar, Rafel Cabot, Joseph T. Smith, Christopher A. Hunter","doi":"10.1021/jacs.4c13452","DOIUrl":"https://doi.org/10.1021/jacs.4c13452","url":null,"abstract":"Information can be encoded and stored in sequences of monomer units organized in linear synthetic polymers. Replication of sequence information is of fundamental importance in biology; however, it represents a challenge for synthetic polymer chemistry. A combination of covalent and noncovalent base pairs has been used to achieve high-fidelity templated synthesis of synthetic polymers that encode information as a sequence of different side-chain recognition units. Dialkyne building blocks were attached to the template by using ester base pairs, and diazide building blocks were attached to the template by using H-bond base pairs. Copper-catalyzed azide–alkyne cycloaddition reactions were used to zip up the copy strand on the template, and the resulting duplex was cleaved by hydrolyzing the covalent ester base pairs. By using recognition-encoded melamine oligomers with either three phosphine oxide or three 4-nitrophenol recognition units to form the noncovalent base pairs, exceptionally high affinities of the diazides for the template were achieved, allowing the templated polymerization step to be carried out at low concentrations, which promoted on-template intramolecular reactions relative to competing intermolecular processes. Two different templates, a 7-mer and an 11-mer, were used in the three-step reaction sequence to obtain the sequence-complementary copy strands with minimal amounts of side reaction.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"12 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642839","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

A Universal Interfacial Reconstruction Strategy Based on Converting Residual Alkali for Sodium Layered Oxide Cathodes: Marvelous Air Stability, Reversible Anion Redox, and Practical Full Cell 基于钠层状氧化物阴极残碱转化的通用界面重构策略：神奇的空气稳定性、可逆的阴离子氧化还原和实用的全电池

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-16 DOI: 10.1021/jacs.4c04766

Ling-Yi Kong, Jia-Yang Li, Han-Xiao Liu, Yan-Fang Zhu, Jingqiang Wang, Yifeng Liu, Xin-Yu Zhang, Hai-Yan Hu, Hanghang Dong, Zhuang-Chun Jian, Chen Cheng, Shuangqiang Chen, Liang Zhang, Jia-Zhao Wang, Shulei Chou, Yao Xiao

{"title":"A Universal Interfacial Reconstruction Strategy Based on Converting Residual Alkali for Sodium Layered Oxide Cathodes: Marvelous Air Stability, Reversible Anion Redox, and Practical Full Cell","authors":"Ling-Yi Kong, Jia-Yang Li, Han-Xiao Liu, Yan-Fang Zhu, Jingqiang Wang, Yifeng Liu, Xin-Yu Zhang, Hai-Yan Hu, Hanghang Dong, Zhuang-Chun Jian, Chen Cheng, Shuangqiang Chen, Liang Zhang, Jia-Zhao Wang, Shulei Chou, Yao Xiao","doi":"10.1021/jacs.4c04766","DOIUrl":"https://doi.org/10.1021/jacs.4c04766","url":null,"abstract":"Mn-based layered oxide cathodes have attracted widespread attention due to high capacity and low cost, however, poor air stability, irreversible phase transitions, and slow kinetics inhibit their practical application. Here, we propose a universal interfacial reconstruction strategy based on converting residual alkali to tunnel phase Na0.44MnO2 for addressing the above mentioned issue simultaneously, using O3 NaNi0.4Fe0.2Mn0.4O2@2 mol % Na0.44MnO2 (NaNFM@NMO) as the prototype material. The optimized material exhibits an initial capacity and energy density comparable with lithium-ion batteries. The reversible anionic redox behavior and charge compensation mechanism of NaNFM@NMO were analyzed and verified by soft X-ray absorption spectrum and in situ X-ray absorption spectrum. Due to the intrinsic stability of the tunnel structure, excellent air stability and highly reversible structure evolution of the NaNFM@NMO cathode material are achieved, which are confirmed by contact angle test, rigorous aging test, and in situ X-ray diffraction. More importantly, the NaNFM@NMO cathode demonstrates a great match with the nonpresodiated hard carbon anode and shows excellent electrochemical performance of the full cell. Additionally, such a strategy could be also applied to modify P2-type cathodes, showing superior universality and good prospects in industrialized production. Overall, the proposed strategy could improve air stability while remaining interfacial and bulk stable simultaneously and will open up a whole new field for the optimization of other electrode materials.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"166 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642841","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

Non-Innocent Role of Sacrificial Anodes in Electrochemical Nickel-Catalyzed C(sp2)–C(sp3) Cross-Electrophile Coupling 电化学镍催化 C（sp2）-C（sp3）交叉亲电偶联中牺牲阳极的非无辜作用

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-15 DOI: 10.1021/jacs.4c10979

Luana Cardinale, Gregory L. Beutner, Christopher Y. Bemis, Daniel J. Weix, Shannon S. Stahl

引用次数: 0

C–OH Bond Activation for Stereoselective Radical C-Glycosylation of Native Saccharides C-OH 键活化用于原生糖的立体选择性 Radical C-Glycosylation

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-15 DOI: 10.1021/jacs.4c11857

Hao Xie, Sheng Wang, Xing-Zhong Shu

引用次数: 0

Diameter-Controlled Synthesis of Carbon Nanotubes Using [2n]Collarenes as Rigid Organic Templates. 以 [2n]Collarenes 为刚性有机模板合成直径可控的碳纳米管。

IF 14.4 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-15 DOI: 10.1021/jacs.4c08536

Ting Liu, Linxi Zhu, Ke Liu, Zhe Liu, Yang Liu, Yifei Zhang, Yue Hu, Qing-Hui Guo, Feihe Huang

引用次数: 0