ACS Publications最新文献

{"title":"Retraction of “Jejupeptins A and B: Polyketide–Cyclic Peptide Hybrids with Anti-Corticosterone Activity from Streptomyces sp. KCB15JA151”","authors":"Jun-Pil Jang, Jongtae Roh, Gil Soo Kim, Jihun Park, Gwi Ja Hwang, Beomcheol Park, Hyeok-Won Lee, Shunji Takahashi, Young-Soo Hong*, Sung-Kyun Ko* and Jae-Hyuk Jang*, ","doi":"10.1021/acs.jnatprod.5c0043510.1021/acs.jnatprod.5c00435","DOIUrl":"https://doi.org/10.1021/acs.jnatprod.5c00435https://doi.org/10.1021/acs.jnatprod.5c00435","url":null,"abstract":"","PeriodicalId":47,"journal":{"name":"Journal of Natural Products ","volume":"88 4","pages":"1098 1098"},"PeriodicalIF":3.3,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867359","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"生物学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Organocatalytic Atroposelective Cross-Coupling of 2-Naphthols with Diaryliodonium Salts","authors":"Sushree Ranjan Sahoo,&nbsp; and ,&nbsp;Vinod K. Singh*,&nbsp;","doi":"10.1021/acs.orglett.5c0027910.1021/acs.orglett.5c00279","DOIUrl":"https://doi.org/10.1021/acs.orglett.5c00279https://doi.org/10.1021/acs.orglett.5c00279","url":null,"abstract":"<p >Due to their modularity and conciseness, atroposelective cross-coupling is one of the most attractive approaches for synthesizing axially chiral binaphthyl molecules. While transition metal-catalyzed cross-couplings provide reliable synthetic strategies, alternative methods that accommodate a broader range of substrates without their pre-functionalization are highly beneficial. Here, we demonstrate that using the bifunctional organocatalyst (DHQD)₂PHAL enables atroposelective cross-coupling of 2-naphthols and diaryliodonium salts with high efficiency, and yields (up to 72%) and excellent enantioselectivity (up to &gt;99% enantiomeric excess). Further transformations of the products highlight the versatility of other binaphthyl compounds while maintaining their axial chirality.</p>","PeriodicalId":54,"journal":{"name":"Organic Letters","volume":"27 16","pages":"4085–4089 4085–4089"},"PeriodicalIF":4.9,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867300","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}

{"title":"High-Strength, Rapid-Recovery, Solvent-Resistant, and Recyclable Fluorinated Acrylic Polyurethane with Supramolecular and Covalently Dual-Cross-linked Networks","authors":"Pengwei Xie,&nbsp;Guoqiang Wu,&nbsp;Yubo Liu,&nbsp;Keling Hu,&nbsp;Zhengfeng Ma,&nbsp;Xiaowei Pei,&nbsp;Yang Wu* and Feng Zhou,&nbsp;","doi":"10.1021/acsapm.5c0031410.1021/acsapm.5c00314","DOIUrl":"https://doi.org/10.1021/acsapm.5c00314https://doi.org/10.1021/acsapm.5c00314","url":null,"abstract":"<p >High-performance polymer elastomers with high strength, rapid recovery, solvent resistance, and recyclability are desired in engineering fields. The incorporation of supramolecular interactions as sacrificial bonds for energy dissipation is an effective strategy to enhance the mechanical performance of polymers. However, this approach can result in a loss of resilience due to excessive energy consumption. In this study, we developed a kind of noncovalently supramolecular and covalently dual-cross-linked fluorinated acrylic polyurethane (PU-PFOMA) by incorporating adipic acid dihydrazide and acrylate-modified cyclodextrins into the polyurethane main chains and polymerizing perfluorooctyl methacrylate (PFOMA) in the polyacrylate side chains. The resulting PU-PFOMA demonstrated superior mechanical properties (54.36 MPa), elongation at break (1150%), and toughness (248.05 MJ/m³) due to the multiple H-bonds formed by adipic acid dihydrazide and the stable covalently cross-linked structure achieved through radical copolymerization. Furthermore, PU-PFOMA exhibited excellent resilience, attributed to the stable interchain cross-linking and the driving force generated by the poly(oxytetramethylene) glycol (PTMG) and PFOMA segments to reform their respective aggregates, owing to their thermodynamically incompatible nature. PU-PFOMA also demonstrated exceptional low-temperature resistance, including high strength (265.62 MPa), high toughness (648.44 MJ/m³) at −70 °C, and excellent resilience at −60 °C. More importantly, the PU-PFOMA elastomer has good solvent resistance that compared with PU because of the introduction of fluoroalkyl chains and could be reprocessed by hot pressing (130 °C, 10 MPa) and recover more than 70% of its toughness after reprocessing procedure. This study highlights the prospective uses of PU-PFOMA in fields necessitating robust mechanical characteristics and resistance to low temperatures.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 8","pages":"5058–5069 5058–5069"},"PeriodicalIF":4.4,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867296","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Surface Structural Symmetry Breaking of Highly Symmetrical Ag29 Nanoclusters","authors":"Wenqiang Duan,&nbsp;Chen Zhu,&nbsp;Xi Kang* and Manzhou Zhu,&nbsp;","doi":"10.1021/acs.jpclett.5c0069910.1021/acs.jpclett.5c00699","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00699https://doi.org/10.1021/acs.jpclett.5c00699","url":null,"abstract":"<p >An in-depth understanding of the structural symmetry of nanoclusters benefits the investigation of structure–property correlations. In this study, we accomplished the symmetry breaking of the surface structures of a highly symmetrical Ag₂₉ nanocluster. The Ag₂₉ nanocluster exhibited a highly <i>C</i>₃ axisymmetry, while this nanocluster underwent structural symmetry breaking in the presence of large-sized counterions as an asymmetric factor, giving rise to an Ag₂₈ nanocluster with a bare surface and a <i>C</i>₁ symmetric overall structure. Despite both the Ag₂₉ and Ag₂₈ nanoclusters exhibiting comparably electronic structures, the highly symmetrical Ag₂₉ nanocluster displayed a significantly higher photoluminescence intensity compared to the asymmetrical Ag₂₈ nanocluster, which has been rationalized from the perspective of their structures and symmetry. Overall, this study presents a novel silver cluster pair with controllably symmetrical or asymmetrical surface structures, allowing for an atomic-level understanding of how structural symmetry influences the photoluminescence of metal nanoclusters.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 16","pages":"4090–4096 4090–4096"},"PeriodicalIF":4.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143863241","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrochemical Model for Field Effect Conductivities of Electrolytes in Equilibrium Systems","authors":"Mojie Cheng*,&nbsp;","doi":"10.1021/acs.jpclett.5c0052010.1021/acs.jpclett.5c00520","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00520https://doi.org/10.1021/acs.jpclett.5c00520","url":null,"abstract":"<p >Field effect electronic and ionic conductivities come from the electronic and ionic resonances and polarizations in an electrolyte. An external atmosphere field causes field enhanced electronic conductivity and field depressed ionic conductivity. The higher molar formation Gibbs energy of the pi side than that of the ni side in a pin electrolyte heterostructure results in field enhanced electronic conductivity and field depressed ionic conductivity on the pi side as well as field depressed electronic conductivity and field enhanced ionic conductivity on the ni side. An impedance spectrum arises from polarizations at high temperature but from both polarizations and resonances at low temperature. The electrochemical model demonstrates the origins of field effect conductivities in an electrolyte under equilibrium.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 16","pages":"4114–4123 4114–4123"},"PeriodicalIF":4.8,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143863243","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Development and Mechanistic Insights into Nef Reaction for Preparation of Aldehydes Using Singlet Oxygen","authors":"Ira Novita Sari,&nbsp;Bobo Yan,&nbsp;Tatsuya Morozumi,&nbsp;Yuichi Kamiya and Taiki Umezawa*,&nbsp;","doi":"10.1021/acs.orglett.5c0095410.1021/acs.orglett.5c00954","DOIUrl":"https://doi.org/10.1021/acs.orglett.5c00954https://doi.org/10.1021/acs.orglett.5c00954","url":null,"abstract":"<p >The Nef reaction for conversion of nitro compounds to aldehydes is described. Various functional groups, such as ethers, silyl ethers, acetals or esters, were tolerated to give aldehydes in high yields using Cs₂CO₃ and singlet oxygen as an oxidant. Transformations of nitromethyl groups into hydroxymethyl groups were achieved in a one-pot operation. The mechanism involved in the Nef reaction was studied using ion chromatography and radical scavengers, which resulted in the proposal of two unique reaction pathways.</p>","PeriodicalId":54,"journal":{"name":"Organic Letters","volume":"27 16","pages":"4263–4268 4263–4268"},"PeriodicalIF":4.9,"publicationDate":"2025-04-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867301","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}

{"title":"Recognizing Excellence in Photonics: Finalists of the ACS Photonics Young Investigator Award","authors":"Romain Quidant,&nbsp;","doi":"10.1021/acsphotonics.5c0044910.1021/acsphotonics.5c00449","DOIUrl":"https://doi.org/10.1021/acsphotonics.5c00449https://doi.org/10.1021/acsphotonics.5c00449","url":null,"abstract":"","PeriodicalId":23,"journal":{"name":"ACS Photonics","volume":"12 4","pages":"1716–1717 1716–1717"},"PeriodicalIF":6.5,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143833009","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Thermalization without Detailed Balance: Population Oscillations in the Absence of Coherences","authors":"Shay Blum,&nbsp; and ,&nbsp;David Gelbwaser-Klimovsky*,&nbsp;","doi":"10.1021/acs.jpclett.5c0049910.1021/acs.jpclett.5c00499","DOIUrl":"https://doi.org/10.1021/acs.jpclett.5c00499https://doi.org/10.1021/acs.jpclett.5c00499","url":null,"abstract":"<p >Open quantum systems that comply with the master equation and detailed balance decay in a non-oscillatory manner to thermal equilibrium. Beyond the weak coupling limit, systems that break microreversibility (e.g., in the presence of magnetic fields) violate detailed balance but still thermalize. We study the thermalization of these systems and show that a temperature increase produces novel exceptional points that indicate a sharp transition in the thermalization dynamics. A further temperature increase fuels oscillations of the energy level populations, even without quantum coherences. Moreover, the violation of detailed balance introduces an energy scale that characterizes the oscillatory regime at high temperatures.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 16","pages":"4066–4071 4066–4071"},"PeriodicalIF":4.8,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.jpclett.5c00499","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143863220","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Self-Healing Composite Film Made of Cellulose Nanocrystals and a Polyvinyl Acetate Copolymer","authors":"Guofan Xu,&nbsp;Jude Laverock,&nbsp;Todor T. Koev,&nbsp;Yaroslav Z. Khimyak,&nbsp;Onajite Abafe Diejomaoh,&nbsp;Sebastien Rochat and Stephen J. Eichhorn*,&nbsp;","doi":"10.1021/acsapm.5c0021910.1021/acsapm.5c00219","DOIUrl":"https://doi.org/10.1021/acsapm.5c00219https://doi.org/10.1021/acsapm.5c00219","url":null,"abstract":"<p >A cellulose nanocrystal (CNC)-polyvinyl acetate (PVAc) self-healing composite film was fabricated using a grafting-from approach generating polyvinyl acetate (PVAc) chains on CNC macroinitiators. These grafted-to CNCs were then mixed with bulk PVAc polymer to form a composite. Fourier-transform infrared spectroscopy, X-ray photoelectron spectroscopy, and solid-state nuclear magnetic resonance were used to demonstrate the presence of the grafted PVAc chains on the surface of the CNCs. Transmission electron microscopy images revealed the structure of the modified CNCs, which formed closely packed clusters due to the grafted PVAc chains. The thermal properties of the CNCs and their composite films were assessed by using differential scanning calorimetry, determining the appropriate temperature for the healing of the composite film. On this basis, the film was cut into two pieces and rejoined and healed in an oven heated at 40 °C for 6 h. The healed sample was viewed under an optical microscope and electron microscopy, demonstrating the efficacy of the healing process. An array of microindentation tests across the surface of the healed specimen was conducted to quantify stiffness, revealing no detectable differences between the healed and intact regions. This healing was found to only occur for the grafted-to samples and was not evident for the composites made of PVAc and ungrafted CNCs. This work demonstrates that grafting polymer chains onto CNCs and blending these with a bulk polymer are promising approaches for fabricating composite films capable of healing macroscopic fractures.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"7 8","pages":"4982–4991 4982–4991"},"PeriodicalIF":4.4,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsapm.5c00219","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867295","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Enrichment of 1.0 Nanometer Diameter Single-Chirality Single-Walled Carbon Nanotubes Dictated by Conjugated Polymer Characteristics: Implications for High-Performance Thin-Film Transistors","authors":"Jianying Ouyang*,&nbsp;Homin Shin,&nbsp;Paul Finnie,&nbsp;Jianfu Ding,&nbsp;Zhao Li,&nbsp;Brendan Mirka and Patrick R. L. Malenfant,&nbsp;","doi":"10.1021/acsanm.5c0078310.1021/acsanm.5c00783","DOIUrl":"https://doi.org/10.1021/acsanm.5c00783https://doi.org/10.1021/acsanm.5c00783","url":null,"abstract":"<p >In conjugated polymer extraction (CPE), the polymer characteristics impact the chiral selectivity and yield in the enrichment of single-chirality, single-walled carbon nanotubes (SWCNTs). Polyfluorene is one of the most efficient conjugated polymers to enrich semiconducting or single-chirality SWCNTs. We found that copolymers of fluorene and pyridine (PF12-Py2,5) or oxadiazole (P(F₄-alt-Ox)) exhibited a prevailing selectivity toward (8,7) (diameter 1.032 nm). The chiral purity of (8,7) was improved by storage and ultracentrifugation. In addition, <i>p</i>-xylene is better than toluene to achieve a higher selectivity; as a result, 66% (8,7) purity was reached in <i>p</i>-xylene. Furthermore, the length of the alkyl side chain in PF-Py2,5 also influences the selectivity, with the medium length (<i>n</i>-dodecylfluorene, PF12-Py2,5) showing higher (8,7) selectivity than a shorter length (<i>n</i>-octylfluorene, PF8-Py2,5) and a longer length (<i>n</i>-tetradecylfluorene, PF14-Py2,5). Besides, copolymers of fluorene and benzothiadiazole (PFO-BT) and anthracene (PFO=A) enriched (10,5) (diameter 1.050 nm) in <i>p</i>-xylene and (9,5) (diameter 0.976 nm) in toluene with their chiral purity up to 94.5% and 86%, respectively. The chiral purity was calculated based on the area percentage of the optical absorption S₁₁ peak and also evaluated by photoluminescence excitation (PLE) mapping and Raman scattering spectroscopy. All three (n,m) achieved the highest purity within the CPE methodology. The quality of enriched (8,7) was examined by the performance of thin-film transistors (TFT), which exhibited hole and electron mobilities of 2.6 ± 0.7 and 1.5 ± 0.6 cm²/(V s), respectively, and high on/off ratios of ∼10⁴. 1.0 nm diameter was suggested to reach balanced drive current and leakage in high-performance TFTs. Density functional theory calculation shows that polyfluorene exhibits increasing wrapping stability as the tube diameter increases, and the geometric model of polymer wrapping suggests that P(F₄-alt-Ox) has better coverage of nanotube surface toward (8,7).</p>","PeriodicalId":6,"journal":{"name":"ACS Applied Nano Materials","volume":"8 16","pages":"8260–8273 8260–8273"},"PeriodicalIF":5.3,"publicationDate":"2025-04-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsanm.5c00783","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143867567","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}