ACS Nanoscience Au最新文献_第9页

Nanoparticles Codelivering mRNA and SiRNA for Simultaneous Restoration and Silencing of Gene/Protein Expression In Vitro and In Vivo 纳米颗粒共递送mRNA和SiRNA用于体外和体内基因/蛋白表达的同时恢复和沉默

IF 4.8

ACS Nanoscience Au Pub Date : 2024-11-15 DOI: 10.1021/acsnanoscienceau.4c0004010.1021/acsnanoscienceau.4c00040

Shireesha Manturthi, Sara El-Sahli, Yuxia Bo, Emma Durocher, Melanie Kirkby, Alyanna Popatia, Karan Mediratta, Redaet Daniel, Seung-Hwan Lee, Umar Iqbal, Marceline Côté, Lisheng Wang* and Suresh Gadde*,

{"title":"Nanoparticles Codelivering mRNA and SiRNA for Simultaneous Restoration and Silencing of Gene/Protein Expression In Vitro and In Vivo","authors":"Shireesha Manturthi, Sara El-Sahli, Yuxia Bo, Emma Durocher, Melanie Kirkby, Alyanna Popatia, Karan Mediratta, Redaet Daniel, Seung-Hwan Lee, Umar Iqbal, Marceline Côté, Lisheng Wang* and Suresh Gadde*, ","doi":"10.1021/acsnanoscienceau.4c0004010.1021/acsnanoscienceau.4c00040","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00040https://doi.org/10.1021/acsnanoscienceau.4c00040","url":null,"abstract":"RNA-based agents (siRNA, miRNA, and mRNA) can selectively manipulate gene expression/proteins and are set to revolutionize a variety of disease treatments. Nanoparticle (NP) platforms have been developed to deliver functional mRNA or siRNA inside cells to overcome their inherent limitations. Recent studies have focused on siRNA to knock down proteins causing drug resistance or mRNA technology to introduce tumor suppressors. However, cancer needs multitargeted approaches to selectively manipulate multiple gene expressions/proteins. In this proof-of-concept study, we developed NPs containing Luc-mRNA and siRNA-GFP as model agents ((M+S)-NPs) and showed that NPs can simultaneously deliver functional mRNA and siRNA and impact the expression of two genes/proteins in vitro. Additionally, after in vivo administration, (M+S)-NPs successfully knocked down GFP while introducing luciferase into a TNBC mouse model, indicating that our NPs have the potential to develop RNA-based anticancer therapeutics. These studies pave the way to develop RNA-based, multitargeted approaches for complex diseases like cancer.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"416–425 416–425"},"PeriodicalIF":4.8,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00040","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142842852","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Flexible Cation Exchange Environment via Ligand-Free Metal Chalcogenide Thin Films. 无配体金属硫系薄膜的柔性阳离子交换环境。

IF 4.8

ACS Nanoscience Au Pub Date : 2024-11-08 eCollection Date: 2025-02-19 DOI: 10.1021/acsnanoscienceau.4c00023

Hannah R Lacey, Kevin D Dobson, Emil A Hernández-Pagán

{"title":"Flexible Cation Exchange Environment via Ligand-Free Metal Chalcogenide Thin Films.","authors":"Hannah R Lacey, Kevin D Dobson, Emil A Hernández-Pagán","doi":"10.1021/acsnanoscienceau.4c00023","DOIUrl":"10.1021/acsnanoscienceau.4c00023","url":null,"abstract":"Cation exchange (CE) has emerged as a premier postsynthetic method to carefully tune the chemical composition and properties of nanocrystals with excellent morphology retention. However, reaction conditions are typically dictated by the ubiquitous ligands bound to their surface, limiting their solubility and influencing the thermodynamics/kinetics of the reaction. To bypass these challenges, we report on CE reactions with Cu+, Ag+, Cu2+, Cd2+, Zn2+, and Mn2+ utilizing ligand-free CdS and Cu x Se y thin films as host templates. The exchange reactions could be performed sequentially or simultaneously (i.e., two guest cations) to access compositionally diverse products. The incorporation of cations on the host films was confirmed using SEM-EDS, XPS, and ICP-MS analyses, as well as tracking wavelength shifts in the UV-vis absorption spectra. The flexibility of this approach was demonstrated as reactions were carried out using an array of different guest precursor salts and solvents with a range of polarities. Moreover, the reactions were generalizable among selenide and sulfide films and proceeded under milder conditions in comparison with reported nanocrystal reactions. A ligand-free environment with flexible reaction conditions, as the work herein, could aid in deconvoluting the different factors involved in CE reactions and further expand its use for fundamental research and applications like photovoltaics, optoelectronics, and catalysis.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"5 1","pages":"9-20"},"PeriodicalIF":4.8,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11843514/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143484062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Role of Exciton Diffusion in the Efficiency of Mn Dopant Emission in Two-Dimensional Perovskites. 激子扩散对二维钙钛矿中Mn掺杂发射效率的影响。

IF 4.8

ACS Nanoscience Au Pub Date : 2024-11-07 eCollection Date: 2025-02-19 DOI: 10.1021/acsnanoscienceau.4c00047

Alvaro J Magdaleno, Anuraj S Kshirsagar, Marc Meléndez, Udara M Kuruppu, Jesse J Suurmond, Mercy M Cutler, Michel Frising, Michael Seitz, Rafael Delgado-Buscalioni, Mahesh K Gangishetty, Ferry Prins

{"title":"Role of Exciton Diffusion in the Efficiency of Mn Dopant Emission in Two-Dimensional Perovskites.","authors":"Alvaro J Magdaleno, Anuraj S Kshirsagar, Marc Meléndez, Udara M Kuruppu, Jesse J Suurmond, Mercy M Cutler, Michel Frising, Michael Seitz, Rafael Delgado-Buscalioni, Mahesh K Gangishetty, Ferry Prins","doi":"10.1021/acsnanoscienceau.4c00047","DOIUrl":"10.1021/acsnanoscienceau.4c00047","url":null,"abstract":"Two-dimensional (2D) metal-halide perovskites have promising characteristics for optoelectronic applications. By incorporating Mn2+ ions into the perovskite structure, improved photoluminescence quantum yield can be achieved. This has been attributed to the formation of defect states that act as efficient recombination centers. Here, we make use of transient photoluminescence microscopy to characterize important material parameters of Mn2+-doped 2D perovskites with different doping levels. From these measurements, we visualize the importance of exciton transport as an intermediate step in the excitation of Mn2+. We model the spatiotemporal dynamics of the excited states to extract the diffusion constant and the transfer rate of the excitations to the Mn dopant sites. Interestingly, from these models, we find that the average distance an exciton needs to travel before transferring to a Mn site is significantly larger than expected from the Mn concentration obtained from elemental analysis. These insights are critical from a device design perspective.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"5 1","pages":"29-36"},"PeriodicalIF":4.8,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11843506/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143484116","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Role of Exciton Diffusion in the Efficiency of Mn Dopant Emission in Two-Dimensional Perovskites 激子扩散对二维钙钛矿中Mn掺杂发射效率的影响

IF 4.8

ACS Nanoscience Au Pub Date : 2024-11-07 DOI: 10.1021/acsnanoscienceau.4c0004710.1021/acsnanoscienceau.4c00047

Alvaro J. Magdaleno, Anuraj S. Kshirsagar, Marc Meléndez, Udara M. Kuruppu, Jesse J. Suurmond, Mercy M. Cutler, Michel Frising, Michael Seitz, Rafael Delgado-Buscalioni, Mahesh K. Gangishetty* and Ferry Prins*,

{"title":"Role of Exciton Diffusion in the Efficiency of Mn Dopant Emission in Two-Dimensional Perovskites","authors":"Alvaro J. Magdaleno, Anuraj S. Kshirsagar, Marc Meléndez, Udara M. Kuruppu, Jesse J. Suurmond, Mercy M. Cutler, Michel Frising, Michael Seitz, Rafael Delgado-Buscalioni, Mahesh K. Gangishetty* and Ferry Prins*, ","doi":"10.1021/acsnanoscienceau.4c0004710.1021/acsnanoscienceau.4c00047","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00047https://doi.org/10.1021/acsnanoscienceau.4c00047","url":null,"abstract":"Two-dimensional (2D) metal-halide perovskites have promising characteristics for optoelectronic applications. By incorporating Mn2+ ions into the perovskite structure, improved photoluminescence quantum yield can be achieved. This has been attributed to the formation of defect states that act as efficient recombination centers. Here, we make use of transient photoluminescence microscopy to characterize important material parameters of Mn2+-doped 2D perovskites with different doping levels. From these measurements, we visualize the importance of exciton transport as an intermediate step in the excitation of Mn2+. We model the spatiotemporal dynamics of the excited states to extract the diffusion constant and the transfer rate of the excitations to the Mn dopant sites. Interestingly, from these models, we find that the average distance an exciton needs to travel before transferring to a Mn site is significantly larger than expected from the Mn concentration obtained from elemental analysis. These insights are critical from a device design perspective.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"5 1","pages":"29–36 29–36"},"PeriodicalIF":4.8,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00047","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435954","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Flexible Cation Exchange Environment via Ligand-Free Metal Chalcogenide Thin Films 无配体金属硫系薄膜的柔性阳离子交换环境

IF 4.8

ACS Nanoscience Au Pub Date : 2024-11-07 DOI: 10.1021/acsnanoscienceau.4c0002310.1021/acsnanoscienceau.4c00023

Hannah R. Lacey, Kevin D. Dobson and Emil A. Hernández-Pagán*,

{"title":"Flexible Cation Exchange Environment via Ligand-Free Metal Chalcogenide Thin Films","authors":"Hannah R. Lacey, Kevin D. Dobson and Emil A. Hernández-Pagán*, ","doi":"10.1021/acsnanoscienceau.4c0002310.1021/acsnanoscienceau.4c00023","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00023https://doi.org/10.1021/acsnanoscienceau.4c00023","url":null,"abstract":"Cation exchange (CE) has emerged as a premier postsynthetic method to carefully tune the chemical composition and properties of nanocrystals with excellent morphology retention. However, reaction conditions are typically dictated by the ubiquitous ligands bound to their surface, limiting their solubility and influencing the thermodynamics/kinetics of the reaction. To bypass these challenges, we report on CE reactions with Cu+, Ag+, Cu2+, Cd2+, Zn2+, and Mn2+ utilizing ligand-free CdS and CuxSey thin films as host templates. The exchange reactions could be performed sequentially or simultaneously (i.e., two guest cations) to access compositionally diverse products. The incorporation of cations on the host films was confirmed using SEM-EDS, XPS, and ICP-MS analyses, as well as tracking wavelength shifts in the UV–vis absorption spectra. The flexibility of this approach was demonstrated as reactions were carried out using an array of different guest precursor salts and solvents with a range of polarities. Moreover, the reactions were generalizable among selenide and sulfide films and proceeded under milder conditions in comparison with reported nanocrystal reactions. A ligand-free environment with flexible reaction conditions, as the work herein, could aid in deconvoluting the different factors involved in CE reactions and further expand its use for fundamental research and applications like photovoltaics, optoelectronics, and catalysis.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"5 1","pages":"9–20 9–20"},"PeriodicalIF":4.8,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00023","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435955","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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 Cation Distribution on Photoluminescence of Ag–In–Se/ZnSe Core/Shell Nanocrystals 阳离子分布对Ag-In-Se /ZnSe核/壳纳米晶体光致发光的影响

IF 4.8

ACS Nanoscience Au Pub Date : 2024-11-04 DOI: 10.1021/acsnanoscienceau.4c0004510.1021/acsnanoscienceau.4c00045

Annina Moser, Olesya Yarema, Noemi Rusch, Nikola D̵ord̵ević, Weyde M. M. Lin, Deniz Bozyigit, Nuri Yazdani, Maksym Yarema*, Mathieu Luisier and Vanessa Wood*,

{"title":"Impact of Cation Distribution on Photoluminescence of Ag–In–Se/ZnSe Core/Shell Nanocrystals","authors":"Annina Moser, Olesya Yarema, Noemi Rusch, Nikola D̵ord̵ević, Weyde M. M. Lin, Deniz Bozyigit, Nuri Yazdani, Maksym Yarema*, Mathieu Luisier and Vanessa Wood*, ","doi":"10.1021/acsnanoscienceau.4c0004510.1021/acsnanoscienceau.4c00045","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00045https://doi.org/10.1021/acsnanoscienceau.4c00045","url":null,"abstract":"Ag–In–Se/ZnSe core/shell nanocrystals exhibit good photoluminescence quantum yield (PLQY), yet intriguingly, the maximum PLQY is first reached after several days of storage. We hypothesize that this may be due to cationic rearrangement in the nanocrystal post-synthesis. To test this hypothesis, we computationally generated ternary Ag–In–Se and quaternary Ag–In–Zn–Se nanocrystals with varying degrees of cationic disorder, as quantified by the distribution of the metal cation valence electrons in the tetrahedra around Se anions. We then used density functional theory-parametrized tight-binding simulations to study the electronic structure and optical properties of these systems as a function of the homogeneity of the valence electron distribution in a tetrahedron. We found that homogeneous distribution of cations leads to a larger band gap and optical coupling, and that, in the presence of AgIn or InAg antisite defects, the introduction of intermediate valence Zn cations decreases the variance in valence electrons and improves the optical properties. We further simulated the impact of a Zn-gradient shell and rearrangement of cations in the outer layers of the nanocrystals and find that diffusion of Zn into the nanocrystal and cationic rearrangement can explain the post-synthetic increase of PLQY. This work highlights the importance of developing syntheses for multinary nanocrystals that result not only in size and composition uniformity but also in nanocrystals with a uniform distribution of charge.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"5 1","pages":"21–28 21–28"},"PeriodicalIF":4.8,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00045","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435952","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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 Cation Distribution on Photoluminescence of Ag-In-Se/ZnSe Core/Shell Nanocrystals. 阳离子分布对Ag-In-Se/ZnSe核/壳纳米晶体光致发光的影响

IF 4.8

ACS Nanoscience Au Pub Date : 2024-11-04 eCollection Date: 2025-02-19 DOI: 10.1021/acsnanoscienceau.4c00045

Annina Moser, Olesya Yarema, Noemi Rusch, Nikola D Ord Ević, Weyde M M Lin, Deniz Bozyigit, Nuri Yazdani, Maksym Yarema, Mathieu Luisier, Vanessa Wood

{"title":"Impact of Cation Distribution on Photoluminescence of Ag-In-Se/ZnSe Core/Shell Nanocrystals.","authors":"Annina Moser, Olesya Yarema, Noemi Rusch, Nikola D Ord Ević, Weyde M M Lin, Deniz Bozyigit, Nuri Yazdani, Maksym Yarema, Mathieu Luisier, Vanessa Wood","doi":"10.1021/acsnanoscienceau.4c00045","DOIUrl":"10.1021/acsnanoscienceau.4c00045","url":null,"abstract":"Ag-In-Se/ZnSe core/shell nanocrystals exhibit good photoluminescence quantum yield (PLQY), yet intriguingly, the maximum PLQY is first reached after several days of storage. We hypothesize that this may be due to cationic rearrangement in the nanocrystal post-synthesis. To test this hypothesis, we computationally generated ternary Ag-In-Se and quaternary Ag-In-Zn-Se nanocrystals with varying degrees of cationic disorder, as quantified by the distribution of the metal cation valence electrons in the tetrahedra around Se anions. We then used density functional theory-parametrized tight-binding simulations to study the electronic structure and optical properties of these systems as a function of the homogeneity of the valence electron distribution in a tetrahedron. We found that homogeneous distribution of cations leads to a larger band gap and optical coupling, and that, in the presence of AgIn or InAg antisite defects, the introduction of intermediate valence Zn cations decreases the variance in valence electrons and improves the optical properties. We further simulated the impact of a Zn-gradient shell and rearrangement of cations in the outer layers of the nanocrystals and find that diffusion of Zn into the nanocrystal and cationic rearrangement can explain the post-synthetic increase of PLQY. This work highlights the importance of developing syntheses for multinary nanocrystals that result not only in size and composition uniformity but also in nanocrystals with a uniform distribution of charge.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"5 1","pages":"21-28"},"PeriodicalIF":4.8,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11843510/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143484068","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Molecular Additives as Competitive Binding Agents to Control Supramolecular-Driven Nanoparticle Assembly. 分子添加剂作为竞争结合剂控制超分子驱动的纳米颗粒组装。

IF 4.8

ACS Nanoscience Au Pub Date : 2024-10-31 eCollection Date: 2024-12-18 DOI: 10.1021/acsnanoscienceau.4c00062

Rebecca L Li, Nicholas Sbalbi, Matthew Ye, Robert J Macfarlane

{"title":"Molecular Additives as Competitive Binding Agents to Control Supramolecular-Driven Nanoparticle Assembly.","authors":"Rebecca L Li, Nicholas Sbalbi, Matthew Ye, Robert J Macfarlane","doi":"10.1021/acsnanoscienceau.4c00062","DOIUrl":"10.1021/acsnanoscienceau.4c00062","url":null,"abstract":"Colloidal nanoparticle assembly methods can produce intricate superlattice structures and often use knowledge of atomic crystallization behaviors to guide their design. While this analogy has enabled multiple routes to programming colloidal crystallization thermodynamics, fewer tools or strategies exist to manipulate nanoparticle superlattice growth kinetics in a controlled manner. Here we investigate how small-molecule additives can be used to modulate the thermodynamics and kinetics of supramolecular-chemistry-driven nanoparticle assembly. Specifically, we introduce monovalent binding agents into the superlattice growth solution that compete with the multivalent interparticle bonding interactions driving particle assembly, thereby altering interparticle bond strength by reducing the number of bridging complexes formed between particles. In this manner, the assemblies can be steered to avoid kinetic traps and crystallize into faceted single crystals under isothermal conditions, alleviating the need for precise thermal control that has conventionally been required to produce large, faceted crystals in prior assembly methods.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"374-380"},"PeriodicalIF":4.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11659897/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142878076","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Molecular Additives as Competitive Binding Agents to Control Supramolecular-Driven Nanoparticle Assembly 分子添加剂作为竞争结合剂控制超分子驱动的纳米颗粒组装

IF 4.8

ACS Nanoscience Au Pub Date : 2024-10-31 DOI: 10.1021/acsnanoscienceau.4c0006210.1021/acsnanoscienceau.4c00062

Rebecca L. Li, Nicholas Sbalbi, Matthew Ye and Robert J. Macfarlane*,

{"title":"Molecular Additives as Competitive Binding Agents to Control Supramolecular-Driven Nanoparticle Assembly","authors":"Rebecca L. Li, Nicholas Sbalbi, Matthew Ye and Robert J. Macfarlane*, ","doi":"10.1021/acsnanoscienceau.4c0006210.1021/acsnanoscienceau.4c00062","DOIUrl":"https://doi.org/10.1021/acsnanoscienceau.4c00062https://doi.org/10.1021/acsnanoscienceau.4c00062","url":null,"abstract":"Colloidal nanoparticle assembly methods can produce intricate superlattice structures and often use knowledge of atomic crystallization behaviors to guide their design. While this analogy has enabled multiple routes to programming colloidal crystallization thermodynamics, fewer tools or strategies exist to manipulate nanoparticle superlattice growth kinetics in a controlled manner. Here we investigate how small-molecule additives can be used to modulate the thermodynamics and kinetics of supramolecular-chemistry-driven nanoparticle assembly. Specifically, we introduce monovalent binding agents into the superlattice growth solution that compete with the multivalent interparticle bonding interactions driving particle assembly, thereby altering interparticle bond strength by reducing the number of bridging complexes formed between particles. In this manner, the assemblies can be steered to avoid kinetic traps and crystallize into faceted single crystals under isothermal conditions, alleviating the need for precise thermal control that has conventionally been required to produce large, faceted crystals in prior assembly methods.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"374–380 374–380"},"PeriodicalIF":4.8,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsnanoscienceau.4c00062","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142850702","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dynamic Control of Chiral Recognition in Water-Soluble Naphthotubes Induced by Hydrostatic Pressure. 静水压力诱导水溶性萘管手性识别的动态控制。

IF 4.8

ACS Nanoscience Au Pub Date : 2024-10-21 eCollection Date: 2024-12-18 DOI: 10.1021/acsnanoscienceau.4c00052

Junnosuke Motoori, Tomokazu Kinoshita, Hongxin Chai, Ming-Shuang Li, Song-Meng Wang, Wei Jiang, Gaku Fukuhara

{"title":"Dynamic Control of Chiral Recognition in Water-Soluble Naphthotubes Induced by Hydrostatic Pressure.","authors":"Junnosuke Motoori, Tomokazu Kinoshita, Hongxin Chai, Ming-Shuang Li, Song-Meng Wang, Wei Jiang, Gaku Fukuhara","doi":"10.1021/acsnanoscienceau.4c00052","DOIUrl":"10.1021/acsnanoscienceau.4c00052","url":null,"abstract":"The dynamic control of chiral (enantiomeric) responses in chiral host-guest complexes through external stimuli is a significant challenge in modern chemistry for developing smart stimuli-responsive materials. Herein, we report the (chir)optical properties and chiral recognition behavior of water-soluble chiral naphthotubes (1) under the influence of hydrostatic pressure as an external stimulus. The hydrostatic pressure spectral profiles compared to those obtained at normal pressure revealed the dynamic behavior of 1 under hydrostatic pressure, owing to the flexible linker. In chiral recognition experiments, hydrophilic amino acids such as phenylalanine (Phe) and tryptophan (Trp) exhibited reaction volume changes (ΔV°) of -0.9 cm3 mol-1 for d-Phe, -1.2 cm3 mol-1 for l-Phe, -5.6 cm3 mol-1 for d-Trp, and -7.0 cm3 mol-1 for l-Trp, with enantioselectivity ranging from 1.2 to 1.6. In contrast, hydrophobic chiral styrene oxide (2) showed ΔV° values of 1.5 cm3 mol-1 for R-2 and 3.5 cm3 mol-1 for S- 2, with a relatively higher enantioselectivity of up to 7.6. These contrasting effects of hydrostatic pressure primarily originate from the dynamics of chiral naphthotubes.","PeriodicalId":29799,"journal":{"name":"ACS Nanoscience Au","volume":"4 6","pages":"435-442"},"PeriodicalIF":4.8,"publicationDate":"2024-10-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11659898/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142878068","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0