Journal of the American Chemical Society最新文献_第4页

Structural Disorder of a Layered Lithium Manganese Oxide Cathode Paving a Reversible Phase Transition Route toward Its Theoretical Capacity 层状氧化锰锂阴极的结构紊乱为实现理论容量铺平了一条可逆相变之路

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c12248

Suwon Lee, Seongkoo Kang, Youngju Choi, Jihyun Kim, Junghoon Yang, Daseul Han, Kyung-Wan Nam, Olaf J. Borkiewicz, Jiliang Zhang, Yong-Mook Kang

{"title":"Structural Disorder of a Layered Lithium Manganese Oxide Cathode Paving a Reversible Phase Transition Route toward Its Theoretical Capacity","authors":"Suwon Lee, Seongkoo Kang, Youngju Choi, Jihyun Kim, Junghoon Yang, Daseul Han, Kyung-Wan Nam, Olaf J. Borkiewicz, Jiliang Zhang, Yong-Mook Kang","doi":"10.1021/jacs.4c12248","DOIUrl":"https://doi.org/10.1021/jacs.4c12248","url":null,"abstract":"Layered lithium manganese oxides suffer from irreversible phase transitions induced by Mn migration and/or dissolution associated with the Jahn–Teller effect (JTE) of Mn3+, leading to inevitable capacity fading during cycling. The popular doping strategy of oxidizing Mn3+ to Mn4+ to relieve the JTE cannot completely eliminate the detrimental structural collapse from the cooperative JTE. Therefore, they are considered to be impractical for commercial use as cathode materials. Here, we demonstrate a layered lithium manganese oxide that can be charged and discharged without any serious structural collapse using metastable Li-birnessite with controlled structural disorder. Although Li-birnessite is thermodynamically unstable under ambient conditions, Li ion exchange into Na-birnessite followed by an optimal dehydration resulted in a disordered Li-birnessite. The control over crystal water in the interlayer provides intriguing short-range order therein, which can help to suppress parasitic Mn migration and dissolution, thereby ensuring a reversible electrochemical cycling. The Mn redox behavior and local structure change of the Li-birnessite were investigated by ex situ soft X-ray absorption spectroscopy (sXAS) and X-ray pair distribution function (PDF) analysis. The combined sXAS and PDF with electrochemical analyses disclosed that the reversible Mn redox and suppressed phase transitions in Dh Li-birnessite contribute to dramatically improving its electrochemical reversiblity during cycling. Our findings underscore the substantial effects of controlled static disorder on the structural stability and electrochemical reversibility of a layered lithium manganese oxide, Li-birnessite, which extends the practical capacity of layered oxides close to their theoretical limit.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"35 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685118","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

Enantioselective Synthesis of vic-Aminoalcohol Derivatives by Nickel-Catalyzed Reductive Coupling of Aldehydes with Protected Amino-pentadienoates 通过镍催化醛与受保护氨基戊二烯酸酯的还原偶联，对映选择性合成vic-氨基乙醇衍生物

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c12002

Thilo Bender, Alois Fürstner

引用次数: 0

Molecular Design of Phthalocyanine-Based Drug Coassembly with Tailored Function 具有定制功能的酞菁类药物共聚物的分子设计

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c10070

Dong Li, Siyong Huang, Jianlin Ge, Ziqi Zhuang, Longyi Zheng, Lai Jiang, Yulun Chen, Chengchao Chu, Yang Zhang, Jie Pan, Bingwei Cheng, Jian-Dong Huang, Huirong Lin, Wei Han, Gang Liu

{"title":"Molecular Design of Phthalocyanine-Based Drug Coassembly with Tailored Function","authors":"Dong Li, Siyong Huang, Jianlin Ge, Ziqi Zhuang, Longyi Zheng, Lai Jiang, Yulun Chen, Chengchao Chu, Yang Zhang, Jie Pan, Bingwei Cheng, Jian-Dong Huang, Huirong Lin, Wei Han, Gang Liu","doi":"10.1021/jacs.4c10070","DOIUrl":"https://doi.org/10.1021/jacs.4c10070","url":null,"abstract":"Coassemblies with tailored functions, such as drug loading, tissue targeting and releasing, therapeutic and/or imaging purposes, and so on, have been widely studied and applied in biomedicine. De novo design of these coassemblies hinges on an integrated approach involving synergy between various design strategies, ranging from structure screening of combinations of “phthalocyanine-chemotherapeutic drug” molecules for molecular scaffolds, exploration of related fabrication principles to verification of intended activity of specific designs. Here, we propose an integrated approach combining computation and experiments to design from scratch coassembled nanoparticles. This nanocoassembly, termed NanoPC here, consists of phthalocyanine-based scaffolds hosting chemotherapeutic drugs, aimed at hypersensitive chemotherapy guided by photoimaging for targeting tumors. Our design starts from the selection of phthalocyanine derivatives that are not aggregation-prone, followed by computational screening of coassembled molecules covering various categories of chemotherapy drugs. To facilitate an efficient and accurate assessment of coassembly capabilities, we utilize small systems as surrogates to enable free-energy calculations at all-atom levels facilitated with enhanced sampling and statistical mechanics for efficient and accurate evaluation of coassembly ability. The final top NanoPC candidate, comprised of phthalocyanine PcL and cytarabine (CYT), can greatly increase the fluorescence intensity ratio of tumor/liver by 21.5 times and achieve higher antitumor efficiency in a pH-dependent manner. Therefore, the designing approach proposed here has a potential pattern, which can provide ideas and references for the design and development of coassembled nanodrugs with tailored functions and applications in biomedicine.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"110 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685111","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

Spotlights on Recent JACS Publications, Volume 146, Issue 48 聚焦最近的 JACS 出版物，第 146 卷第 48 期

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c16058

ACS Contributing Correspondents

引用次数: 0

Generative Pretrained Transformer for Heterogeneous Catalysts 用于异质催化剂的生成式预训练变换器

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c11504

Dong Hyeon Mok, Seoin Back

引用次数: 0

Covalent DNA-Encoded Library Workflow Drives Discovery of SARS-CoV-2 Nonstructural Protein Inhibitors 共价 DNA 编码库工作流程推动了 SARS-CoV-2 非结构蛋白抑制剂的发现

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c12992

Xudong Wang, Liwei Xiong, Ying Zhu, Sixiu Liu, Wenfeng Zhao, Xinyuan Wu, Mengnisa Seydimemet, Linjie Li, Peiqi Ding, Xian Lin, Jiaxiang Liu, Xuan Wang, Zhiqiang Duan, Weiwei Lu, Yanrui Suo, Mengqing Cui, Jinfeng Yue, Rui Jin, Mingyue Zheng, Yechun Xu, Lianghe Mei, Hangchen Hu, Xiaojie Lu

{"title":"Covalent DNA-Encoded Library Workflow Drives Discovery of SARS-CoV-2 Nonstructural Protein Inhibitors","authors":"Xudong Wang, Liwei Xiong, Ying Zhu, Sixiu Liu, Wenfeng Zhao, Xinyuan Wu, Mengnisa Seydimemet, Linjie Li, Peiqi Ding, Xian Lin, Jiaxiang Liu, Xuan Wang, Zhiqiang Duan, Weiwei Lu, Yanrui Suo, Mengqing Cui, Jinfeng Yue, Rui Jin, Mingyue Zheng, Yechun Xu, Lianghe Mei, Hangchen Hu, Xiaojie Lu","doi":"10.1021/jacs.4c12992","DOIUrl":"https://doi.org/10.1021/jacs.4c12992","url":null,"abstract":"The COVID-19 pandemic, exacerbated by persistent viral mutations, underscored the urgent need for diverse inhibitors targeting multiple viral proteins. In this study, we utilized covalent DNA-encoded libraries to discover innovative triazine-based covalent inhibitors for the 3-chymotrypsin-like protease (3CLpro, Nsp5) and the papain-like protease (PLpro) domains of Nsp3, as well as novel non-nucleoside covalent inhibitors for the nonstructural protein 12 (Nsp12, RdRp). Optimization through molecular docking and medicinal chemistry led to the development of LU9, a nonpeptide 3CLpro inhibitor with an IC50 of 0.34 μM, and LU10, whose crystal structure showed a distinct binding mode within the 3CLpro active site. The X-ray cocrystal structure of SARS-CoV-2 PLpro in complex with XD5 uncovered a previously unexplored binding site adjacent to the catalytic pocket. Additionally, a non-nucleoside covalent Nsp12 inhibitor XJ5 achieved a potency of 0.12 μM following comprehensive structure–activity relationship analysis and optimization. Molecular dynamics revealed a potential binding mode. These compounds offer valuable chemical probes for target validation and represent promising candidates for the development of SARS-CoV-2 antiviral therapies.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"23 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685120","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

Charge Transfer Dynamics in Supramolecular Tessellations Composed of Aromatic Donors and Chiral Tris(naphthalenediimide) Triangular Acceptors 由芳香族供体和手性三(萘二亚胺)三角受体组成的超分子网状结构中的电荷转移动力学

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c13800

Malik L. Williams, Jonathan R. Palmer, Ryan M. Young, Michael R. Wasielewski

{"title":"Charge Transfer Dynamics in Supramolecular Tessellations Composed of Aromatic Donors and Chiral Tris(naphthalenediimide) Triangular Acceptors","authors":"Malik L. Williams, Jonathan R. Palmer, Ryan M. Young, Michael R. Wasielewski","doi":"10.1021/jacs.4c13800","DOIUrl":"https://doi.org/10.1021/jacs.4c13800","url":null,"abstract":"Understanding charge transfer (CT) dynamics in donor–acceptor (D–A) cocrystals is important for the development of efficient organic photovoltaic and electronic materials. This study explores the photogenerated CT states of supramolecular tessellations formed by cocrystallizing a chiral tris(naphthalenediimide) triangular prism (−)-NDI-Δ with pyrene, perylene, and peri-xanthenoxanthene electron donors. By manipulating crystallization conditions, one-dimensional (1D) and two-dimensional (2D) cocrystals with distinct structural motifs and morphologies are achieved. Femtosecond and nanosecond transient absorption microscopies and time-resolved electron paramagnetic resonance spectroscopy were employed to elucidate the CT state dynamics. Our findings reveal that the CT state lifetimes are lengthened in the 2D cocrystals relative to the 1D cocrystals, which is attributable to the symmetry and molecular packing differences between them that modulate the CT interactions. This work highlights the potential of using preorganized covalent multisite charge carriers as donors or acceptors in cocrystals as a strategy for engineering structures for advanced multifunctional materials with tunable CT properties.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"24 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142690921","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

Exclusive Generation of Single-Atom Sulfur for Ultrahigh Quality Monolayer MoS2 Growth 为超高质量单层 MoS2 生长独家生成单原子硫

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c10810

Yunhao Zhang, Jingwei Wang, Yumo Chen, Xian Wu, Junyang Tan, Jiarong Liu, Huiyu Nong, Liqiong He, Qinke Wu, Guangmin Zhou, Xiaolong Zou, Bilu Liu

{"title":"Exclusive Generation of Single-Atom Sulfur for Ultrahigh Quality Monolayer MoS2 Growth","authors":"Yunhao Zhang, Jingwei Wang, Yumo Chen, Xian Wu, Junyang Tan, Jiarong Liu, Huiyu Nong, Liqiong He, Qinke Wu, Guangmin Zhou, Xiaolong Zou, Bilu Liu","doi":"10.1021/jacs.4c10810","DOIUrl":"https://doi.org/10.1021/jacs.4c10810","url":null,"abstract":"Preparation of high-quality two-dimensional (2D) transition metal dichalcogenides (TMDCs) is the precondition for realizing their applications. However, the synthesized 2D TMDCs (e.g., MoS2) crystals suffer from low quality due to the massive defects formed during the growth. Here, we report single-atom sulfur (S1) as a highly reactive sulfur species to grow ultrahigh-quality monolayer MoS2. Derived from battery waste, sulfurized polyacrylonitrile (SPAN) is found to be exclusive and efficient in releasing S1. The monolayer MoS2 prepared by SPAN exhibits an ultralow defect density of ∼7 × 1012 cm–2 and the narrowest photoluminescence (PL) emission peak with full-width at half-maximum of ∼47.11 meV at room temperature. Moreover, the statistical resonance Raman and low-temperature PL results further verify the significantly lower defect density and higher optical quality of SPAN-grown MoS2 than those of the conventional S-powder-grown samples. This work provides an effective approach for preparing ultrahigh-quality 2D single crystals, facilitating their industrial applications.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"8 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685116","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

Oxygen Vacancy Boosts Nitrogen-Centered Radical Coupling Initiated by Primary Amine Electrooxidation 氧空位促进了由伯胺电氧化引发的以氮为中心的自由基耦合

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c12451

Mengwei Han, Yongxiang Luo, Leitao Xu, Wei Chen, Chengmei Li, Yu-Cheng Huang, Yandong Wu, Yimin Jiang, Wenjie Wu, Ruiqi Wang, Ying-Rui Lu, Yuqin Zou, Shuangyin Wang

{"title":"Oxygen Vacancy Boosts Nitrogen-Centered Radical Coupling Initiated by Primary Amine Electrooxidation","authors":"Mengwei Han, Yongxiang Luo, Leitao Xu, Wei Chen, Chengmei Li, Yu-Cheng Huang, Yandong Wu, Yimin Jiang, Wenjie Wu, Ruiqi Wang, Ying-Rui Lu, Yuqin Zou, Shuangyin Wang","doi":"10.1021/jacs.4c12451","DOIUrl":"https://doi.org/10.1021/jacs.4c12451","url":null,"abstract":"Synthesis of nitrogen-centered radicals (NCRs) for radical coupling reactions is a powerful and versatile tool in the arsenal of organic synthetic chemistry. However, there are few reports on the direct synthesis of NCRs based on aqueous electrocatalysis. Herein, we present a new electrochemical primary amine oxidation reaction (ePAOR) system with R1R2-CH-NH2 as the substrate for synthesizing NCRs and N–N coupling products. However, ePAOR on the model catalyst (NiO) suffers from low N–N coupling selectivity due to the weak adsorption energy of imine (R1R2-C═NH) intermediates. Guided by theoretical calculations, the oxygen vacancy gives NiO a strong adsorption capacity of R1R2-C═NH so that it boosts nitrogen-centered radical coupling initiated by the ePAOR on oxygen vacancy-rich NiO (VO-NiO), and the effective utilization rate of NCRs was increased from 36 to 75%. This approach is compatible with a wide range of primary amines and can be applied to N–N cross-coupling systems as well.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"1 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684998","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

Plateau–Rayleigh Instability in Soft-Lattice Inorganic Solids 软晶格无机固体中的高原-雷利不稳定性

IF 15 1区化学

Journal of the American Chemical Society Pub Date : 2024-11-22 DOI: 10.1021/jacs.4c11866

Zhen-Chao Shao, Xianyun Jiang, Chong Zhang, Tianhao Wang, Yan-Ru Wang, Guo-Qiang Liu, Zong-Ying Huang, Yu-Zhuo Zhang, Liang Wu, Zhong-Huai Hou, Huijun Jiang, Yi Li, Shu-Hong Yu

{"title":"Plateau–Rayleigh Instability in Soft-Lattice Inorganic Solids","authors":"Zhen-Chao Shao, Xianyun Jiang, Chong Zhang, Tianhao Wang, Yan-Ru Wang, Guo-Qiang Liu, Zong-Ying Huang, Yu-Zhuo Zhang, Liang Wu, Zhong-Huai Hou, Huijun Jiang, Yi Li, Shu-Hong Yu","doi":"10.1021/jacs.4c11866","DOIUrl":"https://doi.org/10.1021/jacs.4c11866","url":null,"abstract":"Plateau–Rayleigh instability─a macroscopic phenomenon describing the volume-constant breakup of one-dimensional continuous fluids─has now been widely observed in adatoms, liquids, polymers, and liquid metals. This instability enables controlled wetting–dewetting behavior at fluid–solid interfaces and, thereby, the self-limited patterning into ordered structures. However, it has yet to be observed in conventional inorganic solids, as the rigid lattices restrict their “fluidity”. Here, we report the general fluid-like Plateau–Rayleigh instability of silver-based chalcogenide semiconductors featuring soft-lattice ionic crystals. It enables postsynthetic morphing from conformal core–shell nanowires to periodically coaxial ones. We reveal that such self-limited reconstruction is thermodynamically driven by the surface energy and interface energy and kinetically favored by the high ionic diffusion coefficients of subnanoscale soft-lattice shells. The resulting periodic heterostructures can be topotactically transformed for epitaxial combinations of functional semiconductors free from the lattice-matching rule. This fluid-like behavior in soft inorganic solids thus offers routes toward sophisticated nanostructures and controllable patterning at all-inorganic solid–solid interfaces.","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"254 1","pages":""},"PeriodicalIF":15.0,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685114","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