ACS Combinatorial Science最新文献_第7页

Protamine-Mediated Tangles Produce Extreme Deoxyribonucleic Acid Compaction 原胺介导的缠结会产生极度的脱氧核糖核酸压积

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-29 DOI: 10.1021/jacs.4c1246810.1021/jacs.4c12468

Vikhyaat Ahlawat, Anshika Dhiman, Hashini Ekanayake Mudiyanselage and Huan-Xiang Zhou*,

{"title":"Protamine-Mediated Tangles Produce Extreme Deoxyribonucleic Acid Compaction","authors":"Vikhyaat Ahlawat, Anshika Dhiman, Hashini Ekanayake Mudiyanselage and Huan-Xiang Zhou*, ","doi":"10.1021/jacs.4c1246810.1021/jacs.4c12468","DOIUrl":"https://doi.org/10.1021/jacs.4c12468https://doi.org/10.1021/jacs.4c12468","url":null,"abstract":"In sperm cells, protamine replaces histones to compact DNA 10–20 times more than in somatic cells. To characterize the extreme compaction, we employed confocal microscopy and optical tweezers to determine the conformations and stability of protamine-bound λ-DNA. Confocal images show increasing compaction of λ-DNA at increasing protamine concentration. In the presence of protamine, single λ-DNA molecules form tangles that withstand forces strong enough (∼55 pN) for strand separation and shorten the contour length by up to 40% even at high forces, as well as bends and loops that rupture at 10–40 pN forces. Strand separation nucleates tangles, implicating protamine interactions with DNA bases. Molecular dynamics simulations show that Arg sidechains of protamine each form hydrogen bonds with multiple bases, frequently in the form of a wedge between the two strands of DNA. Protamine may participate in both local and higher-order chromatin organization, leading to extreme compaction and global transcription silencing.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30668–30677 30668–30677"},"PeriodicalIF":14.4,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585991","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Cobalt Nitride-Implanted PtCo Intermetallic Nanocatalysts for Ultrahigh Fuel Cell Cathode Performance 氮化钴植入铂钴金属间纳米催化剂实现超高燃料电池阴极性能

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-29 DOI: 10.1021/jacs.4c0951410.1021/jacs.4c09514

Muhammad Irfansyah Maulana, Tae Hwan Jo, Ha-Young Lee, Chaehyeon Lee, Caleb Gyan-Barimah, Cheol-Hwan Shin, Jeong-Hoon Yu, Kug-Seung Lee, Seoin Back* and Jong-Sung Yu*,

{"title":"Cobalt Nitride-Implanted PtCo Intermetallic Nanocatalysts for Ultrahigh Fuel Cell Cathode Performance","authors":"Muhammad Irfansyah Maulana, Tae Hwan Jo, Ha-Young Lee, Chaehyeon Lee, Caleb Gyan-Barimah, Cheol-Hwan Shin, Jeong-Hoon Yu, Kug-Seung Lee, Seoin Back* and Jong-Sung Yu*, ","doi":"10.1021/jacs.4c0951410.1021/jacs.4c09514","DOIUrl":"https://doi.org/10.1021/jacs.4c09514https://doi.org/10.1021/jacs.4c09514","url":null,"abstract":"Stable and active oxygen reduction electrocatalysts are essential for practical fuel cells. Herein, we report a novel class of highly ordered platinum-cobalt (Pt-Co) alloys embedded with cobalt nitride. The intermetallic core–shell catalyst demonstrates an initial mass activity of 0.88 A mgPt–1 at 0.9 V with 71% retention after 30,000 potential cycles of an aggressive square-wave accelerated durability test and loses only 9% of its electrochemical surface area, far exceeding the US Department of Energy 2025 targets, with unprecedented stability and only a minimal voltage loss under practical fuel cell operating conditions. We discover that regulating the atomic ordering in the core results in an optimal lattice configuration that accelerates the oxygen reduction kinetics. The presence of cobalt nitride decorated within PtCo superlattices guarantees a larger barrier to Co dissolution, leading to the excellent endurance of the electrocatalysts. This work brings up a transformative structural engineering strategy for rationally designing high-performing Pt-based catalysts with a unique atomic configuration for broad practical uses in energy conversion technology.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 45","pages":"30922–30932 30922–30932"},"PeriodicalIF":14.4,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142609176","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Magnetoplasmonic Triblock Nanorods for Collective Linear Dichroism 用于集体线性分色的磁光电三嵌段纳米棒

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-29 DOI: 10.1021/jacs.4c1137710.1021/jacs.4c11377

Jinxing Chen*, Ji Feng, Panpan Xu and Yadong Yin*,

引用次数: 0

Photobiocatalytic Platform for the Efficient Enantio-Divergent Synthesis of β-Fluoromethylated Ketones 高效对映-歧化合成 β-氟甲基化酮的光生物催化平台

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-29 DOI: 10.1021/jacs.4c1044110.1021/jacs.4c10441

Yuan-Yang Guo*, Ze-Hua Tian, Linghong Zhang, Yu-Chen Han, Bei-Bei Zhang, Qing Xing, Tianju Shao, Yang Liu and Zhiyong Jiang*,

引用次数: 0

A Carborane-Derived Proton-Coupled Electron Transfer Reagent 硼烷衍生质子耦合电子转移试剂

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-28 DOI: 10.1021/jacs.4c0900710.1021/jacs.4c09007

Enric H. Adillon, and , Jonas C. Peters*,

{"title":"A Carborane-Derived Proton-Coupled Electron Transfer Reagent","authors":"Enric H. Adillon,  and , Jonas C. Peters*, ","doi":"10.1021/jacs.4c0900710.1021/jacs.4c09007","DOIUrl":"https://doi.org/10.1021/jacs.4c09007https://doi.org/10.1021/jacs.4c09007","url":null,"abstract":"Reagents capable of concerted proton–electron transfer (CPET) reactions can access reaction pathways with lower reaction barriers compared to stepwise pathways involving electron transfer (ET) and proton transfer (PT). To realize reductive multielectron/proton transformations involving CPET, one approach that has shown recent promise involves coupling a cobaltocene ET site with a protonated arylamine Brønsted acid PT site. This strategy colocalizes the electron/proton in a matter compatible with a CPET step and net reductive electrocatalysis. To probe the generality of such an approach a class of C,C′-diaryl-o-carboranes is herein explored as a conceptual substitute for the cobaltocene subunit, with an arylamine linkage still serving as a colocalized Brønsted base suitable for protonation. The featured o-carborane (PhCbPhN) can be reduced and protonated to generate an N–H bond with a weak effective bond dissociation free energy (BDFEeff) of 31 kcal/mol, estimated with measured thermodynamic data. This N–H bond is among the lowest measured element–H bonds for analyzed nonmetal compounds. Distinct solid-state crystal structures of the one- and two-electron reduced forms of diaryl-o-carboranes are disclosed to gain insight into their well-behaved redox characteristics. The singly reduced, protonated form of the diaryl-o-carborane can mediate multi-ET/PT reductions of azoarenes, diphenylfumarate, and nitrotoluene. In contrast to the aforementioned cobaltocene system, available mechanistic data disclosed herein support these reactions occurring by a rate-limiting ET step and not a CPET step. A relevant hydrogen evolution reaction (HER) reaction was also studied, with data pointing to a PT/ET/PT mechanism, where the reduced carborane core is itself highly stable to protonation.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30204–30211 30204–30211"},"PeriodicalIF":14.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c09007","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585757","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Lipidation Engineering in Daptomycin Biosynthesis 达托霉素生物合成中的脂化工程

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-28 DOI: 10.1021/jacs.4c1096610.1021/jacs.4c10966

Chang-Hun Ji, Sehong Park, Kunwoo Lee, Hyun-Woo Je and Hahk-Soo Kang*,

{"title":"Lipidation Engineering in Daptomycin Biosynthesis","authors":"Chang-Hun Ji, Sehong Park, Kunwoo Lee, Hyun-Woo Je and Hahk-Soo Kang*, ","doi":"10.1021/jacs.4c1096610.1021/jacs.4c10966","DOIUrl":"https://doi.org/10.1021/jacs.4c10966https://doi.org/10.1021/jacs.4c10966","url":null,"abstract":"Lipopeptides are an important family of natural products, some of which are clinically used as antibiotics to treat multidrug-resistant pathogens. Although the lipid moieties play a crucial role in balancing antibacterial activity and hemolytic toxicity, modifying the lipid moieties has been challenging due to the complexity of the lipidation process in lipopeptide biosynthesis. Here, we show that the lipid profile can be altered by engineering both secondary and primary metabolisms, using daptomycin as an example. First, swapping the fatty acyl AMP ligase (FAAL) gene dptF with foreign FAAL homologs improved the fatty acyl specificity of the lipidation process for decanoic acid. Then, the introduction of Mycobacterium type I fatty acid synthase operon (MvFAS-Ib/MvAcpS) and Cryptosporidium thioesterase (CpTEII) enriched the fatty acid pool with decanoic acid in Streptomyces roseosporus. The engineered fatty acid metabolism eliminates the need for external decanoic acid supplementation by enabling S. roseosporus to biosynthesize decanoic acid. By complete engineering of the lipidation process, we achieved, for the first time, high-purity, natural production of daptomycin. The lipidation engineering approach we demonstrate here lays the foundation for the lipidation control in lipopeptide biosynthesis.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30434–30442 30434–30442"},"PeriodicalIF":14.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585984","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Programmable Plasma-Microdroplet Cascade Reactions for Multicomponent Systems 多组分系统的可编程等离子体-微滴级联反应

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-28 DOI: 10.1021/jacs.4c0705310.1021/jacs.4c07053

Alexander J. Grooms, Isabella M. Marcelo, Robert T. Huttner and Abraham K. Badu-Tawiah*,

{"title":"Programmable Plasma-Microdroplet Cascade Reactions for Multicomponent Systems","authors":"Alexander J. Grooms, Isabella M. Marcelo, Robert T. Huttner and Abraham K. Badu-Tawiah*, ","doi":"10.1021/jacs.4c0705310.1021/jacs.4c07053","DOIUrl":"https://doi.org/10.1021/jacs.4c07053https://doi.org/10.1021/jacs.4c07053","url":null,"abstract":"The concept of programmable cascade reactions in charged microdroplets is introduced using carbon–carbon (C–C) bond formation via uncatalyzed Michael addition in a three-tier study culminating in programmable Hantzsch multicomponent, multistep reactions. In situ generated reactive oxygen species (ROS) from nonthermal plasma discharge are fused with charged water microdroplets (devoid of ROS) in real time for accelerated chemical reactions. This plasma-microdroplet fusion platform utilizing a coaxial spray configuration enabled product selection while avoiding unwanted side reactions. Hydrogen abstraction via ROS facilitated the formation of enolate anions without strong base use. Reaction enhancement factors >103 were calculated for plasma-microdroplet fusion versus microdroplet-only reactions. The platform programmability was showcased through (i) uncatalyzed 1,4-Michael addition of α,β-unsaturated carbonyls, (ii) novel C–C bond formation via the use of pro-electrophilic amine and alcohol substrates─activated through collisions in the microdroplet environment to serve as Michael acceptors, and (iii) selective Hantzsch cascade reaction with cross-coupling products, avoiding side reactions including N-alkylation and self-coupling product formation. Milligram quantity product collection is achieved, showcasing plasma-microdroplet fusion as an effective tool for preparative-scale synthesis. Thus, the controlled generation of ROS via plasma discharge during charged water microdroplet evolution establishes a green synthetic method for uncatalyzed C–C bond formation.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30068–30077 30068–30077"},"PeriodicalIF":14.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585941","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"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

Giant Uniaxial Magnetocrystalline Anisotropy in SmCrGe3 SmCrGe3 中的巨型单轴磁晶各向异性

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-28 DOI: 10.1021/jacs.4c1005610.1021/jacs.4c10056

Mingyu Xu, Yongbin Lee, Xianglin Ke, Min-Chul Kang, Matt Boswell, Sergey L. Bud’ko, Lin Zhou, Liqin Ke, Mingda Li, Paul C. Canfield* and Weiwei Xie*,

{"title":"Giant Uniaxial Magnetocrystalline Anisotropy in SmCrGe3","authors":"Mingyu Xu, Yongbin Lee, Xianglin Ke, Min-Chul Kang, Matt Boswell, Sergey L. Bud’ko, Lin Zhou, Liqin Ke, Mingda Li, Paul C. Canfield* and Weiwei Xie*, ","doi":"10.1021/jacs.4c1005610.1021/jacs.4c10056","DOIUrl":"https://doi.org/10.1021/jacs.4c10056https://doi.org/10.1021/jacs.4c10056","url":null,"abstract":"Magnetic anisotropy is a crucial characteristic for enhancing the spintronic device performance. The synthesis of SmCrGe3 single crystals through a high-temperature solution method has led to the determination of uniaxial magnetocrystalline anisotropy. Phase verification was achieved by using scanning transmission electron microscopy (STEM), powder, and single-crystal X-ray diffraction techniques. Electrical transport and specific heat measurements indicate a Curie temperature (TC) of approximately 160 K, while magnetization measurements were utilized to determine the anisotropy fields and constants. Curie–Weiss fitting applied to magnetization data suggests the contribution of both Sm and Cr in the paramagnetic phase. Additionally, density functional theory (DFT) calculations explored the electronic structures and magnetic properties of SmCrGe3, revealing a significant easy-axis single-ion Sm magnetocrystalline anisotropy of 16 meV/fu. Based on the magnetization measurements, easy-axis magnetocrystalline anisotropy at 20 K is 13 meV/fu.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30294–30302 30294–30302"},"PeriodicalIF":14.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c10056","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585953","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Arylthianthrenium Salts for Triplet Energy Transfer Catalysis 用于三重能量转移催化的芳基噻蒽盐

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-28 DOI: 10.1021/jacs.4c1109910.1021/jacs.4c11099

Yuan Cai, Triptesh Kumar Roy, Till J. B. Zähringer, Beatrice Lansbergen, Christoph Kerzig* and Tobias Ritter*,

{"title":"Arylthianthrenium Salts for Triplet Energy Transfer Catalysis","authors":"Yuan Cai, Triptesh Kumar Roy, Till J. B. Zähringer, Beatrice Lansbergen, Christoph Kerzig* and Tobias Ritter*, ","doi":"10.1021/jacs.4c1109910.1021/jacs.4c11099","DOIUrl":"https://doi.org/10.1021/jacs.4c11099https://doi.org/10.1021/jacs.4c11099","url":null,"abstract":"Sigma bond cleavage through electronically excited states allows synthetically useful transformations with two radical species. Direct excitation of simple aryl halides to form both aryl and halogen radicals necessitates UV-C light, so undesired side reactions are often observed and specific equipment is required. Moreover, only aryl halides with extended π systems and comparatively low triplet energy are applicable to synthetically useful energy transfer catalysis. Here we show the conceptual advantages of arylthianthrenium salts (ArTTs) for energy transfer catalysis with high energy efficiency compared to conventional aryl (pseudo)halides and their utility in arylation reactions of ethylene. The fundamental advance is enabled by the low triplet energy of ArTTs that may originate in large part from the electronic interplay between the distinct sulfur atoms in the tricyclic thianthrene scaffold, which is not accessible in either simple (pseudo)halides or other conventional sulfonium salts.","PeriodicalId":14,"journal":{"name":"ACS Combinatorial Science","volume":"146 44","pages":"30474–30482 30474–30482"},"PeriodicalIF":14.4,"publicationDate":"2024-10-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/jacs.4c11099","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142585948","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Impact of Cavity Length Non-uniformity on Reaction Rate Extraction in Strong Coupling Experiments 空腔长度不均匀对强耦合实验中反应速率提取的影响

IF 14.4 3区化学

ACS Combinatorial Science Pub Date : 2024-10-28 DOI: 10.1021/jacs.4c1226910.1021/jacs.4c12269

Michael A. Michon, and , Blake S. Simpkins*,

引用次数: 0