Chemistry of Materials最新文献_第8页

Silicon Caught Carbon Copying Wolff–Kishner Reduction in Two Dimensional Siloxene Nanosheets

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-17 DOI: 10.1021/acs.chemmater.4c02642

Nav Deepak, Rahul Kumar Das, Dhara Raval, Shobha Shukla, Sumit Saxena

{"title":"Silicon Caught Carbon Copying Wolff–Kishner Reduction in Two Dimensional Siloxene Nanosheets","authors":"Nav Deepak, Rahul Kumar Das, Dhara Raval, Shobha Shukla, Sumit Saxena","doi":"10.1021/acs.chemmater.4c02642","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02642","url":null,"abstract":"Despite vast potential, silicon chemistry has taken a back foot in the recent past as compared to its counterpart, carbon. Recently, silicon-based inorganic compounds containing silicon and oxygen have attracted significant attention. Of these, one intriguing nanostructure is Siloxene, a 2D oxide of silicon. Its close structural resemblance to 2D carbon compounds provides an opportunity to explore chemistries similar to carbon in silicon. Here, we have investigated the stability and reduction of Si═O bonds in 2D-Siloxene using hydrazine in potassium hydroxide. The reduction of 2D Siloxene shows striking similarity to Wolff–Kishner reduction, which is well-known in carbon chemistry. Specifically, the polarization of the Si═O bond in Siloxene results in charge separation between the silicon and oxygen atoms. This significantly enhances the reactivity of the Si═O bond and renders it susceptible to reduction. Mulliken charge analysis within the framework of density functional theory calculations suggests the electronegative behavior of O atoms, when attached to Si both as Si═O and Si–OH. The electropositive Si atom in Si═O is attacked by hydrazine hydrate, subsequently, when treated with a strong base, typically potassium hydroxide, affects the reduction of the hydrazone. Our study provides strong theoretical and experimental evidence for a reduction mechanism analogous to the Wolff–Kishner reduction, in 2D silicon, enabling developing insights in silicon reduction.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"6 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640207","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ultra-Microporous Zinc-Diaminotriazolate-Oxalate Metal Organic Framework with Nonlayered-Pillared Structure Showing High Carbon Dioxide Uptakes at Low Partial Pressures

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-17 DOI: 10.1021/acs.chemmater.4c03231

Piyush Singh, Himan Dev Singh, Pragalbh Shekhar, Chitvan Jain, Ping Song, Mahsa Loloei, Michael Edwin, Yan Gao, Nima Masoumifard, Ramanathan Vaidhyanathan

{"title":"Ultra-Microporous Zinc-Diaminotriazolate-Oxalate Metal Organic Framework with Nonlayered-Pillared Structure Showing High Carbon Dioxide Uptakes at Low Partial Pressures","authors":"Piyush Singh, Himan Dev Singh, Pragalbh Shekhar, Chitvan Jain, Ping Song, Mahsa Loloei, Michael Edwin, Yan Gao, Nima Masoumifard, Ramanathan Vaidhyanathan","doi":"10.1021/acs.chemmater.4c03231","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03231","url":null,"abstract":"We report a zinc-diaminotriazolato-oxalate metal–organic framework (IISERP-MOF36, 1) inspired by the exceptional CO2 selectivity demonstrated by its triazolate analogue, CALF-20. Unlike the CALF-20 family, 1 adopts a nonlayered, pillared structure, despite their similar composition. The 1D ultramicroporous channels in this MOF enhance strong interactions with the carbon dioxide CO2. Additionally, the t-shaped orientation of CO2 molecules within the pores promotes cooperative CO2–CO2 interactions, resulting in superior low-pressure CO2 uptake compared to that of CALF-20. This suggests that 1 has potential as a sorbent in applications such as the natural gas combined cycle or direct air capture. However, despite its structural and compositional similarities to CALF-20, 1 exhibits reduced hydrophobicity due to subtle differences in the pore environment. These findings open possibilities for designing advanced sorbents combining the best characteristics of both of these MOFs.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"43 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143640209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Transport Number Determination and Relevance for Lithium Metal Batteries Using Localized Highly Concentrated Electrolytes

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-17 DOI: 10.1021/acs.chemmater.4c0306710.1021/acs.chemmater.4c03067

Hafiz Ahmad Ishfaq, Carolina Cruz Cardona, Elena Tchernychova, Patrik Johansson, Miran Gaberšček, Robert Dominko and Sara Drvarič Talian*,

{"title":"Transport Number Determination and Relevance for Lithium Metal Batteries Using Localized Highly Concentrated Electrolytes","authors":"Hafiz Ahmad Ishfaq, Carolina Cruz Cardona, Elena Tchernychova, Patrik Johansson, Miran Gaberšček, Robert Dominko and Sara Drvarič Talian*, ","doi":"10.1021/acs.chemmater.4c0306710.1021/acs.chemmater.4c03067","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03067https://doi.org/10.1021/acs.chemmater.4c03067","url":null,"abstract":"The lithium transport number <math><mo>(</mo><msub><mrow><mi>t</mi></mrow><mrow><msup><mrow><mi>Li</mi></mrow><mrow><mo>+</mo></mrow></msup></mrow></msub><mo>)</mo></math> determination of fluorinated ether (1,2-(1,1,2,2-tetrafluoroethoxy) ethane, TFEE)-based localized highly concentrated electrolytes (LHCEs) with 1,2-dioxolane (DOL) and dimethoxyethane (DME) as solvents has been explored using molecular dynamics simulations, nuclear magnetic resonance spectroscopy, Bruce-Vincent’s method, and low-frequency electrochemical impedance spectroscopy (EIS). We showcase that the TFEE-DOL LHCE has a <math><msub><mrow><mi>t</mi></mrow><mrow><msup><mrow><mi>Li</mi></mrow><mrow><mo>+</mo></mrow></msup></mrow></msub></math> as high as 0.65 but, on the other hand, exhibits low Coulombic efficiency (<90%) and poor stability vs Li metal anodes, i.e., in a lithium metal battery (LMB) setting. In contrast, the TFEE-DME LHCE shows high Coulombic efficiency (98.9%) and stability, despite a much lower <math><msub><mrow><mi>t</mi></mrow><mrow><msup><mrow><mi>Li</mi></mrow><mrow><mo>+</mo></mrow></msup></mrow></msub></math> (0.25). A significant migration resistance through the porous solid electrolyte interphase (SEI) for the former is the likely explanation, as revealed by EIS and assisted by scanning electron microscopy and X-ray photoelectron spectroscopy experiments. We thus find the interfacial properties at the Li metal anode to be more crucial than the ionic transport through the bulk of the electrolyte for LMB performance. We therefore propose that the focus should be put on the full (operando) impedance spectra of Li metal anodes in contact with electrolytes, since it enables the characterization of the interphase layer(s), rather than solely determining the (bulk) <math><msub><mrow><mi>t</mi></mrow><mrow><msup><mrow><mi>Li</mi></mrow><mrow><mo>+</mo></mrow></msup></mrow></msub></math> of the electrolytes.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 7","pages":"2485–2495 2485–2495"},"PeriodicalIF":7.2,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c03067","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143790584","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}

引用次数: 0

Structure–Activity Relationship Studies of Glycosaminoglycan Mimetic Macrocycles Against Herpes

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-17 DOI: 10.1021/acs.chemmater.4c02016

Sujeet Pawar, Hien Thi Tran, Melis Özkan, Deepika Sardana, Cynthia Paloma Aigroz, Paulo Jacob Silva, Anita Zucchi, Francesco Stellacci

{"title":"Structure–Activity Relationship Studies of Glycosaminoglycan Mimetic Macrocycles Against Herpes","authors":"Sujeet Pawar, Hien Thi Tran, Melis Özkan, Deepika Sardana, Cynthia Paloma Aigroz, Paulo Jacob Silva, Anita Zucchi, Francesco Stellacci","doi":"10.1021/acs.chemmater.4c02016","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02016","url":null,"abstract":"The herpes simplex virus (HSV) is associated with serious conditions, such as encephalitis and blindness, and its infection is closely linked to significant vascular complications and coagulation issues, particularly in individuals with compromised immune systems. Current antiviral treatments often fall short of effectively eliminating viral shedding and face resistance and are not entirely effective in managing coagulation. HSV recognition of heparan sulfate on cell walls for entry is well-established. A possible strategy to effectively address HSV infections involves developing agents with both antiviral and anticoagulant properties. Recently, multivalent entry inhibitors (MEI) against HSV have been developed. Among the most promising candidates is an MEI that uses a β-cyclodextrin as a scaffold to hold six elongated 11-methylene long alkyl (C11) chains, each terminated with sodium sulfonates. This MEI exhibits irreversible inhibition of viral infectivity (virucidal mechanism) with some good results in vivo. The role of the cyclodextrin core is simply to hold the arms together. Here, we present an investigation of other potential core candidates, and we compare their structure–activity for viral inhibition. We find that all cores functionalized with C12 chains terminated with either sulfate or sulfonate are effective in inhibiting both HSV1 and HSV2, all with a virucidal mechanism. We find significant differences in the half inhibitory concentration (IC50), the best core being p-tert-butylcalix[4]arene when functionalized with C12 sodium sulfonate terminated arms. This core showed an IC50 of 8.3 μM against HSV-1 and 10.6 μM against HSV-2 a drastic improvement over the β-cyclodextrin. We investigated the anticoagulant property of our lead compound by inhibiting factor Xa, a key enzyme in coagulation cascade pathways, and found similar inhibition to that of the FDA-approved drug fondaparinux. Thus, our compound presents a nonsaccharide-based prophylactic dual inhibitor against HSV infections.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"39 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143635770","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Transport Number Determination and Relevance for Lithium Metal Batteries Using Localized Highly Concentrated Electrolytes

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-17 DOI: 10.1021/acs.chemmater.4c03067

Hafiz Ahmad Ishfaq, Carolina Cruz Cardona, Elena Tchernychova, Patrik Johansson, Miran Gaberšček, Robert Dominko, Sara Drvarič Talian

引用次数: 0

Structure–Activity Relationship Studies of Glycosaminoglycan Mimetic Macrocycles Against Herpes

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-17 DOI: 10.1021/acs.chemmater.4c0201610.1021/acs.chemmater.4c02016

Sujeet Pawar, Hien Thi Tran, Melis Özkan, Deepika Sardana, Cynthia Paloma Aigroz, Paulo Jacob Silva, Anita Zucchi and Francesco Stellacci*,

{"title":"Structure–Activity Relationship Studies of Glycosaminoglycan Mimetic Macrocycles Against Herpes","authors":"Sujeet Pawar, Hien Thi Tran, Melis Özkan, Deepika Sardana, Cynthia Paloma Aigroz, Paulo Jacob Silva, Anita Zucchi and Francesco Stellacci*, ","doi":"10.1021/acs.chemmater.4c0201610.1021/acs.chemmater.4c02016","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02016https://doi.org/10.1021/acs.chemmater.4c02016","url":null,"abstract":"The herpes simplex virus (HSV) is associated with serious conditions, such as encephalitis and blindness, and its infection is closely linked to significant vascular complications and coagulation issues, particularly in individuals with compromised immune systems. Current antiviral treatments often fall short of effectively eliminating viral shedding and face resistance and are not entirely effective in managing coagulation. HSV recognition of heparan sulfate on cell walls for entry is well-established. A possible strategy to effectively address HSV infections involves developing agents with both antiviral and anticoagulant properties. Recently, multivalent entry inhibitors (MEI) against HSV have been developed. Among the most promising candidates is an MEI that uses a β-cyclodextrin as a scaffold to hold six elongated 11-methylene long alkyl (C11) chains, each terminated with sodium sulfonates. This MEI exhibits irreversible inhibition of viral infectivity (virucidal mechanism) with some good results in vivo. The role of the cyclodextrin core is simply to hold the arms together. Here, we present an investigation of other potential core candidates, and we compare their structure–activity for viral inhibition. We find that all cores functionalized with C12 chains terminated with either sulfate or sulfonate are effective in inhibiting both HSV1 and HSV2, all with a virucidal mechanism. We find significant differences in the half inhibitory concentration (IC50), the best core being p-tert-butylcalix[4]arene when functionalized with C12 sodium sulfonate terminated arms. This core showed an IC50 of 8.3 μM against HSV-1 and 10.6 μM against HSV-2 a drastic improvement over the β-cyclodextrin. We investigated the anticoagulant property of our lead compound by inhibiting factor Xa, a key enzyme in coagulation cascade pathways, and found similar inhibition to that of the FDA-approved drug fondaparinux. Thus, our compound presents a nonsaccharide-based prophylactic dual inhibitor against HSV infections.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2087–2096 2087–2096"},"PeriodicalIF":7.2,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.4c02016","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678685","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}

引用次数: 0

Fluorine-Induced Anomalous Optical Stability and Pressure-Enhanced Emission Property of 0D Lead Perovskite Derivatives

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-16 DOI: 10.1021/acs.chemmater.5c0011210.1021/acs.chemmater.5c00112

Congcong Chen, Yifan Zhang, Huan Liu, Xuanyu Zhang, Zhongshiqi Luo, Jiawei Lin, Yuhong Mao, Rui Chen, Songhao Guo*, Xujie Lü and Lingling Mao*,

{"title":"Fluorine-Induced Anomalous Optical Stability and Pressure-Enhanced Emission Property of 0D Lead Perovskite Derivatives","authors":"Congcong Chen, Yifan Zhang, Huan Liu, Xuanyu Zhang, Zhongshiqi Luo, Jiawei Lin, Yuhong Mao, Rui Chen, Songhao Guo*, Xujie Lü and Lingling Mao*, ","doi":"10.1021/acs.chemmater.5c0011210.1021/acs.chemmater.5c00112","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00112https://doi.org/10.1021/acs.chemmater.5c00112","url":null,"abstract":"Low-dimensional metal halides, especially zero-dimensional (0D) compounds, are important derivative members of the halide perovskite family primarily due to their highly emissive properties. Here, we report two highly luminescent 0D lead bromides, (BPP)2PbBr4 and (BPPF)2PbBr4·2H2O, abbreviated as BPP-0D and BPPF-0D (BPP = benzyltriphenylphosphonium, BPPF = (4-fluorobenzyl)triphenylphosphonium). Both compounds share mutual seesaw inorganic units [PbBr4]2– separated by bulky organic cations. BPP-0D and BPPF-0D emit yellow and green lights, respectively, with photoluminescence (PL) quantum yields (PLQYs) of ∼15 and ∼55% at ambient conditions. Both compounds show excellent environmental stability and practical applications in light-emitting diodes. Upon compression, BPP-0D experiences a rapid decrease in PL intensity, accompanied by an obvious change in its emissive color from yellow to blue. In contrast, BPPF-0D demonstrates excellent optical stability, retaining its green emission, while the PL increases by ∼1.7 times at 0.8 GPa and the PLQY increases to 93%. For BPPF-0D, the presence of an extra highly electronegative fluoride group adds many more noncovalent interactions, such as C–H···F hydrogen bond and F···F interactions. These interactions strengthen the structural and optical stabilities of BPPF-0D, maintaining its emission peak position with elevated pressure. The straightforward comparison between two similar compounds and their optical properties under pressure modulation underscores the importance of engineering organic cations to control and optimize their properties.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2314–2324 2314–2324"},"PeriodicalIF":7.2,"publicationDate":"2025-03-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678502","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Redox-Responsive Polyprodrugs: Recent Innovations in Reduction- and Oxidation-Responsive Drug Delivery Systems

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-15 DOI: 10.1021/acs.chemmater.4c0318110.1021/acs.chemmater.4c03181

Arjaree Jobdeedamrong, and , Daniel Crespy*,

{"title":"Redox-Responsive Polyprodrugs: Recent Innovations in Reduction- and Oxidation-Responsive Drug Delivery Systems","authors":"Arjaree Jobdeedamrong,  and , Daniel Crespy*, ","doi":"10.1021/acs.chemmater.4c0318110.1021/acs.chemmater.4c03181","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03181https://doi.org/10.1021/acs.chemmater.4c03181","url":null,"abstract":"Redox-responsive polyprodrugs are innovative drug delivery systems that exploit the fact that diseased tissues display distinct microenvironments. These systems feature polymeric backbones or side chains displaying redox-sensitive bonds, enabling a targeted, site-specific drug release in response to oxidation or reduction. This approach minimizes off-target effects and enhances the therapeutic outcomes. Reduction-responsive polyprodrugs contain cleavable bonds, such as disulfide linkages and Pt–ligand bonds in platinum complexes, which can be cleaved through reduction reactions. Disulfide bonds are cleaved in the presence of increased concentrations of intracellular glutathione, hence specifically triggering drug release within tumor cells. The reduction of Pt(IV) to Pt(II) converts inactive platinum prodrugs into active chemotherapeutic agents, enabling targeted cancer treatment. Oxidation-responsive bonds, including boronate esters, thioketal, oxalate, and thiolacetal bonds, are cleaved by reactive oxygen species (ROS) such as hydrogen peroxide, releasing drugs in ROS-rich tumor microenvironments. Furthermore, combining both reduction- and oxidation-responsive bonds in a single polyprodrug enhances selectivity and efficacy, allowing for synchronized drug release in complex tumor environments characterized by both oxidative stress and high glutathione levels. Additionally, redox-responsive polyprodrugs can be engineered to lead to greater stability, controlled degradation, and multifunctional responsiveness, making them versatile tools in precision medicine. Beyond cancer, these polyprodrugs have potential applications in treating inflammatory diseases and creating smart materials for industrial use, such as anticorrosion coatings.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2073–2086 2073–2086"},"PeriodicalIF":7.2,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Redox-Responsive Polyprodrugs: Recent Innovations in Reduction- and Oxidation-Responsive Drug Delivery Systems

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-15 DOI: 10.1021/acs.chemmater.4c03181

Arjaree Jobdeedamrong, Daniel Crespy

{"title":"Redox-Responsive Polyprodrugs: Recent Innovations in Reduction- and Oxidation-Responsive Drug Delivery Systems","authors":"Arjaree Jobdeedamrong, Daniel Crespy","doi":"10.1021/acs.chemmater.4c03181","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03181","url":null,"abstract":"Redox-responsive polyprodrugs are innovative drug delivery systems that exploit the fact that diseased tissues display distinct microenvironments. These systems feature polymeric backbones or side chains displaying redox-sensitive bonds, enabling a targeted, site-specific drug release in response to oxidation or reduction. This approach minimizes off-target effects and enhances the therapeutic outcomes. Reduction-responsive polyprodrugs contain cleavable bonds, such as disulfide linkages and Pt–ligand bonds in platinum complexes, which can be cleaved through reduction reactions. Disulfide bonds are cleaved in the presence of increased concentrations of intracellular glutathione, hence specifically triggering drug release within tumor cells. The reduction of Pt(IV) to Pt(II) converts inactive platinum prodrugs into active chemotherapeutic agents, enabling targeted cancer treatment. Oxidation-responsive bonds, including boronate esters, thioketal, oxalate, and thiolacetal bonds, are cleaved by reactive oxygen species (ROS) such as hydrogen peroxide, releasing drugs in ROS-rich tumor microenvironments. Furthermore, combining both reduction- and oxidation-responsive bonds in a single polyprodrug enhances selectivity and efficacy, allowing for synchronized drug release in complex tumor environments characterized by both oxidative stress and high glutathione levels. Additionally, redox-responsive polyprodrugs can be engineered to lead to greater stability, controlled degradation, and multifunctional responsiveness, making them versatile tools in precision medicine. Beyond cancer, these polyprodrugs have potential applications in treating inflammatory diseases and creating smart materials for industrial use, such as anticorrosion coatings.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"23 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143627572","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Circularly Polarized Light-Regulable Crystal–Liquid Phase Transition of Self-Assembled Macroscopic Chiral Twisted Ribbons

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-14 DOI: 10.1021/acs.chemmater.5c0047810.1021/acs.chemmater.5c00478

Xin Dong, Yixuan Jiang, Yanyi He, Jingsong Feng, Xiao-Qi Yu and Shanshan Yu*,

{"title":"Circularly Polarized Light-Regulable Crystal–Liquid Phase Transition of Self-Assembled Macroscopic Chiral Twisted Ribbons","authors":"Xin Dong, Yixuan Jiang, Yanyi He, Jingsong Feng, Xiao-Qi Yu and Shanshan Yu*, ","doi":"10.1021/acs.chemmater.5c0047810.1021/acs.chemmater.5c00478","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00478https://doi.org/10.1021/acs.chemmater.5c00478","url":null,"abstract":"Chirality is a fundamental property of nature, observed at the subatomic, molecular, supramolecular, and macroscopic levels. Circularly polarized light (CPL) has attracted extensive attention as an effective tool for regulating and inducing chirality on various scales. Herein, we report the formation of micron-scale twisted ribbons from homochiral molecular H8-BAz through self-assembly driven by solvophobic interactions. The chiral information in H8-BAz is effectively transferred and amplified in the supramolecular structure and finally appears as macroscopic homochiral twisted ribbons that match the chirality of the monomers. The ribbons undergo a photoinduced crystal-to-liquid transition (PCLT) when exposed to 365 nm light due to the isomerization of the azobenzene structure. Additionally, the PCLT behavior of chiral ribbons is regulated by CPL: When irradiated with homochiral right-handed CPL (RCP), the ribbon with a P-helix formed by (R)-H8-BAz undergoes a faster phase transition. The M-helix ribbon undergoes a faster phase transition with left-handed CPL (LCP). The average time difference for the phase transition reaches 1.5 times. Our results demonstrate a simple method for creating macroscopic chiral structures and the impact of chiral light sources on their phase transition process.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2379–2388 2379–2388"},"PeriodicalIF":7.2,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678666","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0