Chemical Science最新文献_第10页

Visible-light-driven Net-1,2-Hydrogen Atom Transfer of Amidyl Radicals to Access β-Amido Ketone Derivatives

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-03 DOI: 10.1039/d4sc04997g

Yonggang Jiang, Hui Li, Haoqing Tang, Qingyue Zhang, Haitao Yang, Yu Pang, Chenggang Zou, Hongbin Zhang, Patrick J. Walsh, Xiaodong Yang

引用次数: 0

Multi-target macrocycles: pyrogallol derivatives to control multiple pathological factors associated with Alzheimer’s disease

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-03 DOI: 10.1039/d4sc06417h

Jimin Kwak, Yelim Yi, Seongmin Park, Mi Hee Lim

{"title":"Multi-target macrocycles: pyrogallol derivatives to control multiple pathological factors associated with Alzheimer’s disease","authors":"Jimin Kwak, Yelim Yi, Seongmin Park, Mi Hee Lim","doi":"10.1039/d4sc06417h","DOIUrl":"https://doi.org/10.1039/d4sc06417h","url":null,"abstract":"Designing multi-target chemical tools is a vital approach to understanding the pathology of Alzheimer’s disease (AD), which involves a complex network of pathological factors, such as free organic radicals, amyloid-β (Aβ), and metal-bound Aβ (metal–Aβ). The pyrogallol moiety, known for its ability to lower redox potentials and interact with both Aβ and metal ions, presents a promising framework for this molecular design. Here we show how simple structural variations of pyrogallol can be used to enhance its ability to scavenge free organic radicals and regulate the aggregation of both metal-free Aβ and metal–Aβ. By incorporating multiple pyrogllol units into a macrocyclic scaffold via methylene bridges, we achieve synergistic reactivity against several pathological targets. Our structure–reactivity relationship studies also reveal that the macrocyclic structure noticeably improves antioxidant activity as well as interactions with both Aβ and metal ions, leading to oxidation of Aβ peptides and influencing their conformation and aggregation in both the absence and presence of metal ions. This work demonstrates the potential of simple redox-active structural entities in developing multifunctional chemical reagents that effectively manage the pathological components associated with AD.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"19 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142763741","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

Semiclassical description of nuclear quantum effects in solvated and condensed phase molecular systems

IF 7.6 1区化学

Chemical Science Pub Date : 2024-12-03 DOI: 10.1039/D4SC06383J

Riccardo Conte, Giacomo Mandelli, Giacomo Botti, Davide Moscato, Cecilia Lanzi, Marco Cazzaniga, Chiara Aieta and Michele Ceotto

引用次数: 0

Stereodivergent Assembly of δ-Valerolactones with an Azaarene-Containing Quaternary Stereocenter Enabled by Cu/Ru Relay Catalysis

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-03 DOI: 10.1039/d4sc05852f

Kui Tian, Zhuan Jin, Xin-Lian Liu, Lin He, Hong-Fu Liu, Pinke Yu, Xin Chang, Xiu-Qin Dong, Chun-Jiang Wang

引用次数: 0

Designing a visible light-mediated double photoswitch: A combination of biradical and azobenzene structural motifs that can be switched independently

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-03 DOI: 10.1039/d4sc07247b

Yannic Pilopp, Henrik Beer, Jonas Bresien, Dirk Michalik, Alexander Villinger, Axel Schulz

{"title":"Designing a visible light-mediated double photoswitch: A combination of biradical and azobenzene structural motifs that can be switched independently","authors":"Yannic Pilopp, Henrik Beer, Jonas Bresien, Dirk Michalik, Alexander Villinger, Axel Schulz","doi":"10.1039/d4sc07247b","DOIUrl":"https://doi.org/10.1039/d4sc07247b","url":null,"abstract":"A new molecular switch is presented that combines both biradical and azobenzene motifs to perform visible light-induced constitutional and stereo-isomerisation within the same molecule. The insertion of isonitrile-functionalized azobenzenes into the four-membered biradical [•P(μ-NTer)2P•] (1), yielding a phosphorus-centred cyclopentane-1,3-diyl (E-4B and E-5B), represents a straightforward method to generate the desired double switches (E-4B and E-5B) in excellent yields (>90%). The switching properties are demonstrated for the fluorinated species E-5B and, interestingly, can occur either stepwise or simultaneously, depending on the order in which the sample is irradiated with red and/or green light. All possible isomerisation reactions, i.e. housane formation in the phosphorus-centred cyclopentane-1,3-diyl fragment and E/Z isomerisation at the azobenzene, can be switched by irradiation and the reaction products E-5H, Z-5H and Z-5B (when performing the thermal reverse reaction in the dark) are identified using 19F{1H} and 31P{1H} NMR spectroscopy. Results from quantum chemical calculations contribute to the understanding and visualization of the different isomers of each of the observed compounds (E-5B, E-5H, Z-5H, and Z-5B) caused by the unique structure of the double switches.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"39 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142763694","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

Collective Total Synthesis of Chartreusin Derivatives and Bioactivity Investigations

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-02 DOI: 10.1039/d4sc05629a

Jian-Song Sun, Hong-Zhou Yi, Shu-Min Liang, Jing-Jing Li, Hui Liu, Jin-Xi Liao, De-Yong Liu, Qing-Ju Zhang, Mingzhong Cai

{"title":"Collective Total Synthesis of Chartreusin Derivatives and Bioactivity Investigations","authors":"Jian-Song Sun, Hong-Zhou Yi, Shu-Min Liang, Jing-Jing Li, Hui Liu, Jin-Xi Liao, De-Yong Liu, Qing-Ju Zhang, Mingzhong Cai","doi":"10.1039/d4sc05629a","DOIUrl":"https://doi.org/10.1039/d4sc05629a","url":null,"abstract":"Capitalizing on Hauser annulation and Yu glycosylation, the chemical synthesis of chartreusin-type aromatic polycyclic polyketide glycosides has been investigated, culminating in the successful establishment of chemical approaches toward chartreusin derivatives with intricate chemical structures but promising bioactivities. Based on the chemical synthesis strategy, the first and collective chemical syntheses of chartreusin, D329C, elsamicin A and B have been accomplished. The chemical strategy was featured by the two complementary routes to secure chartarin 10-O-monosaccharide glycosides, the key intermediates in chartreusin derivatives synthesis, as well as the highly stereoselective construction of the difficult glycosidic linkages. Through the synthetic investigations, viable donors and acceptors of 3-C-methyl-branched sugars were determined for the first time. Moreover, facilitated by the established chemical synthetic strategy, the cytotoxic activities of chartreusin derivatives against human cancer cell lines were assessed and profound antineoplastic effects for chartreusin, elsamicin A and B were recorded. Based on RNA-seq analysis, the underlying working mechanisms against ES-2 cells were investigated, and the appended sugar chain-determined function mechanisms were disclosed.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"259 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758245","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

Sluggish Li2O2 Dissolution – A Key to Unlock High-Capacity Lithium-Oxygen Batteries

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-02 DOI: 10.1039/d4sc05911e

Lu He, Shuo Wang, Fengjiao Yu, Yuhui Chen

{"title":"Sluggish Li2O2 Dissolution – A Key to Unlock High-Capacity Lithium-Oxygen Batteries","authors":"Lu He, Shuo Wang, Fengjiao Yu, Yuhui Chen","doi":"10.1039/d4sc05911e","DOIUrl":"https://doi.org/10.1039/d4sc05911e","url":null,"abstract":"While lithium-oxygen batteries have a high theoretical specific energy, the practical discharge capacity is much lower due to the passivation of the solid discharge product, Li2O2, on the electrode surface. Herein, we studied and quantified the deposition and dissolution kinetics of Li2O2 using electrochemical quartz crystal microbalance (EQCM). It is found that the orientation of the electrode greatly influences the formation path and deposition amount of Li2O2. We identified two distinct dissolution modes: surface dissolution and bulk fragmentation, with the latter 100 times faster than the former. By revealing the underlying factors affecting dissolution, 80% of Li2O2 can dissolve within 3 minutes when a desorption potential of 2.9 V is applied. Consequently, we designed an intermittent-desorption discharge strategy, which increased the discharge capacity by an order of magnitude. This work shows that high practical specific energy of Li-O2 battery can be achieved once problems of Li2O2 dissolution are addressed.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"6 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758249","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

Steric Stabilization of Colloidal UiO-66 Nanocrystals with Oleylammonium Octadecylphosphonate

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-02 DOI: 10.1039/d4sc06528j

Sungho V. Park, Lakshmi Bhai, Ga Hyun Lee, Ah-Hyung Alissa Park, Lauren E. Marbella, Jonathan Owen

引用次数: 0

Lattice Oxygen Insertion Mechanism in CeO2-Catalyzed Reactions in Water: Nitrile Hydration Reaction

IF 8.4 1区化学

Chemical Science Pub Date : 2024-12-02 DOI: 10.1039/d4sc06294a

Takaaki Endo, Tatsushi Ikeda, Koki Muraoka, Yusuke Kita, Masazumi Tamura, Akira Nakayama

{"title":"Lattice Oxygen Insertion Mechanism in CeO2-Catalyzed Reactions in Water: Nitrile Hydration Reaction","authors":"Takaaki Endo, Tatsushi Ikeda, Koki Muraoka, Yusuke Kita, Masazumi Tamura, Akira Nakayama","doi":"10.1039/d4sc06294a","DOIUrl":"https://doi.org/10.1039/d4sc06294a","url":null,"abstract":"Cerium oxide (CeO2) exhibits prominent catalytic activity in various organic reactions owing to its unique acid-base and redox properties. One of the most interesting applications of pure CeO2-catalyzed organic reactions is the hydration of nitriles in water. The experimental results showed that the hydration of 2-cyanopyridine to picolinamide in water using CeO2 catalysts proceeds readily at low temperatures (30−100 °C) in high yields and that this reaction occurs exclusively on CeO2 among various metal-oxide catalysts. To elucidate the unique catalytic activity of CeO2, the reaction mechanism is dissected using the density functional theory-based molecular dynamics (DFT-MD) simulations. Based on the free energy analysis, it is demonstrated that the reaction proceeds with the involvement of the surface lattice oxygen, where the lattice oxygen atom is inserted into picolinamide. The involvement of the surface lattice oxygen is notably uncommon given the low temperatures of the reaction, and this computational prediction is verified by the two experiments using H218O solvent and 18O-exchanged CeO2 catalyst, where the introduction of surface lattice oxygen into picolinamide is confirmed. The inherent flexibility of the surface lattice oxygen and the unique acid-base properties of CeO2, which can favorably bind and activate both nitrile and water molecules, are key factors in the high reactivity for various organic reactions, which characterizes the outstanding catalytic activity of CeO2.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":"4 1","pages":""},"PeriodicalIF":8.4,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758250","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

Dual back interface engineering optimized charge carrier dynamics in Sb2(S,Se)3 photocathodes for efficient solar hydrogen production†

IF 7.6 1区化学

Chemical Science Pub Date : 2024-12-02 DOI: 10.1039/D4SC05893C

Hafiz Sartaj Aziz, Tahir Imran, Munir Ahmad, Guo-Jie Chen, Ping Luo, Dong-Lou Ren, Bing-Suo Zou, Ju-Guang Hu, Zheng-Hua Su, Pei-Guang Yan, Guang-Xing Liang and Shuo Chen

{"title":"Dual back interface engineering optimized charge carrier dynamics in Sb2(S,Se)3 photocathodes for efficient solar hydrogen production†","authors":"Hafiz Sartaj Aziz, Tahir Imran, Munir Ahmad, Guo-Jie Chen, Ping Luo, Dong-Lou Ren, Bing-Suo Zou, Ju-Guang Hu, Zheng-Hua Su, Pei-Guang Yan, Guang-Xing Liang and Shuo Chen","doi":"10.1039/D4SC05893C","DOIUrl":"10.1039/D4SC05893C","url":null,"abstract":"Antimony sulfoselenide (Sb2(S,Se)3) is a promising sunlight absorber material for solar energy conversion in photovoltaic (PV) cells and photoelectrochemical (PEC) photoelectrodes due to its excellent photoelectric properties. However, the obtained thin-film and back contact properties significantly influence the PEC performance of photocathodes, causing severe bulk recombination, carrier transport loss, and deteriorating half-cell solar-to-hydrogen (HC-STH) efficiency. This study introduces an intriguing dual back interface engineering strategy for Sb2(S,Se)3 photocathodes by incorporating an intermediate MoO2 layer and a secondary carrier transport channel of Au to strengthen charge carrier dynamics. The synergistic assembly of these dual back interface layers improves the growth kinetics and achieves the optimal orientation of Sb2(S,Se)3 thin films by increasing substrate wettability. Moreover, by shortening the back contact barrier height and passivating defect-assisted recombinations, these dual back underlayers simultaneously enhance carrier transport and separation efficiencies. As a result, the photocurrent density of the champion Sb2(S,Se)3 photocathode increases from 5.89 to 32.60 mA cm−2, and the HC-STH conversion efficiency improves significantly from 0.30% to 3.58%, representing the highest value for Sb2(S,Se)3-based photocathodes. This work highlights the effectiveness of dual back interface engineering in promoting the PEC performance of chalcogenide photocathodes for solar hydrogen evolution applications.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":" 1","pages":" 393-409"},"PeriodicalIF":7.6,"publicationDate":"2024-12-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/sc/d4sc05893c?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142758476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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