Melanoma is the most invasive and lethal form of skin cancer that arises from the malignant transformation of specialized pigmented cell melanocytes. Nanomedicine represents an important prospect to mitigate the difficulties and to provide significant benefit to cure melanoma. In the present manuscript, we have investigated the in vitro and in vivo therapeutic efficacy of copper nitroprusside analogue nanoparticles (abbreviated as CuNPANP) towards melanoma. Initially, in vitro anti-cancer activities of CuNPANP towards melanoma cells (B16F10) are evaluated by several experiments such as [methyl 3H]-thymidine incorporation assay, cell cycle & apoptosis assays using FACS analysis, ROS generation using DCFDA, DHE and DAF2A reagent, internalization of nanoparticles through ICP-OES analysis, co-localization of the nanoparticles using confocal microscopy, JC-1 staining to investigate the mitochondrial membrane potential (MMP) and immunofluorescence studies to analyze the expressions of cytochrome-c, Ki-67, E-cadherin as well as phalloidin staining to analyze the cytoskeletal integrity. Further, the in vivo therapeutic effectiveness of the nanoparticles has been established towards malignant melanoma by inoculating B16F10 cells in the dorsal right abdomen of C57BL/6J mice. Intraperitoneal administrations of CuNPANP inhibit tumor growth and increase the survivability of melanoma mice. The in vivo immunofluorescence studies (Ki-67, CD-31, E-cadherin) and TUNEL assay further supports the anti-proliferative and apoptosis inducing potential of CuNPANP, respectively. Finally, the various signaling pathways and molecular mechanisms involved for anti-cancer activity are further evaluated by Western blot analysis. The results altogether offer the use of copper-based nanomedicine for the treatment of malignant melanoma.
{"title":"Copper nitroprusside analogue nanoparticles against melanoma: Detailed in vitro and in vivo investigation","authors":"Sanchita Tripathy, Swapnali Londhe, Arti Patel, Sudipta Saha, Yogesh Chandra, Chittaranjan Patra","doi":"10.1039/d4nr01857e","DOIUrl":"https://doi.org/10.1039/d4nr01857e","url":null,"abstract":"Melanoma is the most invasive and lethal form of skin cancer that arises from the malignant transformation of specialized pigmented cell melanocytes. Nanomedicine represents an important prospect to mitigate the difficulties and to provide significant benefit to cure melanoma. In the present manuscript, we have investigated the in vitro and in vivo therapeutic efficacy of copper nitroprusside analogue nanoparticles (abbreviated as CuNPANP) towards melanoma. Initially, in vitro anti-cancer activities of CuNPANP towards melanoma cells (B16F10) are evaluated by several experiments such as [methyl 3H]-thymidine incorporation assay, cell cycle & apoptosis assays using FACS analysis, ROS generation using DCFDA, DHE and DAF2A reagent, internalization of nanoparticles through ICP-OES analysis, co-localization of the nanoparticles using confocal microscopy, JC-1 staining to investigate the mitochondrial membrane potential (MMP) and immunofluorescence studies to analyze the expressions of cytochrome-c, Ki-67, E-cadherin as well as phalloidin staining to analyze the cytoskeletal integrity. Further, the in vivo therapeutic effectiveness of the nanoparticles has been established towards malignant melanoma by inoculating B16F10 cells in the dorsal right abdomen of C57BL/6J mice. Intraperitoneal administrations of CuNPANP inhibit tumor growth and increase the survivability of melanoma mice. The in vivo immunofluorescence studies (Ki-67, CD-31, E-cadherin) and TUNEL assay further supports the anti-proliferative and apoptosis inducing potential of CuNPANP, respectively. Finally, the various signaling pathways and molecular mechanisms involved for anti-cancer activity are further evaluated by Western blot analysis. The results altogether offer the use of copper-based nanomedicine for the treatment of malignant melanoma.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141333634","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Rahman Basaran, Darshita Budhadev, Amy Kempf, Inga Nehlmeier, Nicole S Hondow, Stefan Pöhlmann, Yuan Guo, Dejian Zhou
Multivalent lectin-glycan interactions (MLGIs) are pivotal for viral infection and immune regulation. Their structural and biophysical data are thus highly valuable, not only for understanding their basic mechanisms but also for designing potent glycoconjugate therapeutics against target MLGIs. However, such information for some important MGLIs remain poorly understood, which has greatly limited the research progress. We have recently developed densely glycosylated nanoparticles, e.g., ~4 nm quantum dot (QD) or ~5 nm gold nanoparticle (GNP), as mechanistic probes for MLGIs. Using two important model lectin viral receptors, DC-SIGN and DC-SIGNR, we have shown these probes not only can offer sensitive fluorescence assays for quantifying MLGI affinities, but also reveal key structural information (e.g., binding site orientation and binding mode) useful for MLGI targeting. However, the small sizes of the previous scaffolds may not be optimal for maximising MLGI affinity and targeting specificity. Herein, using -manno--1,2-biose (DiMan) functionalised GNP (GNP-DiMan) probes, we have systematically studied how GNP scaffold size (e.g., 5, 13, and 27 nm) and glycan density (e.g., 100, 75, 50 and 25%) determine their MLGI affinities, thermodynamics, and antiviral properties. We have developed a new GNP fluorescence quenching assay format to minimise the possible interference of GNP’s strong inner filter effect in MLGI affinity quantification, revealing that increasing GNP size is highly beneficial for enhancing MLGI affinity. We have further determined the MLGI thermodynamics by combining temperature-dependent affinity and Van’t Hoff analyses, revealing that GNP-DiMan-DC-SIGN/R binding is enthalpy driven and their favourable binding Gibbs free energy changes (G0) being enhanced with the increasing GNP size. Finally, we show that increasing GNP size significantly enhances their antiviral potency. Notably, the DiMan coated 27 nm GNP potently and robustly blocks both DC-SIGN and DC-SIGNR mediated pseudo-Ebola virus cellular entry with an EC50 of ~23 and ~49 pM, respectively, making it the most potent glycoconjugate inhibitor against DC-SIGN/R-mediated Ebola cellular infections. Our results have established GNP-glycans as a new tool for quantifying MLGI biophysical parameters and revealed that increasing GNP scaffold size significantly enhances their MLGI affinities and antiviral potencies.
{"title":"Probing scaffold size effects on multivalent lectin-glycan binding affinity, thermodynamics and antiviral properties using polyvalent glycan-gold nanoparticles","authors":"Rahman Basaran, Darshita Budhadev, Amy Kempf, Inga Nehlmeier, Nicole S Hondow, Stefan Pöhlmann, Yuan Guo, Dejian Zhou","doi":"10.1039/d4nr00484a","DOIUrl":"https://doi.org/10.1039/d4nr00484a","url":null,"abstract":"Multivalent lectin-glycan interactions (MLGIs) are pivotal for viral infection and immune regulation. Their structural and biophysical data are thus highly valuable, not only for understanding their basic mechanisms but also for designing potent glycoconjugate therapeutics against target MLGIs. However, such information for some important MGLIs remain poorly understood, which has greatly limited the research progress. We have recently developed densely glycosylated nanoparticles, e.g., ~4 nm quantum dot (QD) or ~5 nm gold nanoparticle (GNP), as mechanistic probes for MLGIs. Using two important model lectin viral receptors, DC-SIGN and DC-SIGNR, we have shown these probes not only can offer sensitive fluorescence assays for quantifying MLGI affinities, but also reveal key structural information (e.g., binding site orientation and binding mode) useful for MLGI targeting. However, the small sizes of the previous scaffolds may not be optimal for maximising MLGI affinity and targeting specificity. Herein, using -manno--1,2-biose (DiMan) functionalised GNP (GNP-DiMan) probes, we have systematically studied how GNP scaffold size (e.g., 5, 13, and 27 nm) and glycan density (e.g., 100, 75, 50 and 25%) determine their MLGI affinities, thermodynamics, and antiviral properties. We have developed a new GNP fluorescence quenching assay format to minimise the possible interference of GNP’s strong inner filter effect in MLGI affinity quantification, revealing that increasing GNP size is highly beneficial for enhancing MLGI affinity. We have further determined the MLGI thermodynamics by combining temperature-dependent affinity and Van’t Hoff analyses, revealing that GNP-DiMan-DC-SIGN/R binding is enthalpy driven and their favourable binding Gibbs free energy changes (G0) being enhanced with the increasing GNP size. Finally, we show that increasing GNP size significantly enhances their antiviral potency. Notably, the DiMan coated 27 nm GNP potently and robustly blocks both DC-SIGN and DC-SIGNR mediated pseudo-Ebola virus cellular entry with an EC50 of ~23 and ~49 pM, respectively, making it the most potent glycoconjugate inhibitor against DC-SIGN/R-mediated Ebola cellular infections. Our results have established GNP-glycans as a new tool for quantifying MLGI biophysical parameters and revealed that increasing GNP scaffold size significantly enhances their MLGI affinities and antiviral potencies.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141333539","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Recent research has shed light on the importance of four-phonon scattering processes in the thermal conductivity (k) of 2D materials. Inclusion of 4 phonon scattering processes from first-principles has been shown to lead to a thermal conductivity of ~1290 W/mK in graphene at 300 K, significantly lower than values predicted to be in excess of 4000 W/mK based only on 3 phonon scattering processes. Four phonon processes are shown to be most significant for flexural ZA phonon modes, where the reflection symmetry selection rule (RSSR) is less restrictive for 4-phonon relative to 3-phonon scattering processes. This combined with the low frequencies of ZA phonon modes, leading to high populations leads to higher 4-phonon compared to 3-phonon scattering of low frequency ZA phonon modes in graphene at 300 K. In this review the role of parameters such as atomic structure, phonon dispersion and temperature on 4-phonon scattering processes in wide range of 2D materials is reviewed. Materials such as graphene nanoplatelets (GnPs) have been extensively investigated for enhancement of thermal conductivity of polymer composites. However, such enhancement is limited by the poor interfacial thermal conductance between polymer and filler material. Interconnected filler networks, overcome this issue, through highly efficient continuous percolative heat transfer paths throughout the composite. Such 3D networks have been shown to enable ultra-high polymer thermal conductivities, approaching ~100 W/mK, and exceeding that of even several metals. In this review, different techniques to achieve such interconnected 3D filler networks such as aerogels, foams, ice-templating, expanded graphite, hot pressing of filler coated polymer particles, synergy effect between multiple fillers, and stitching of filler sheets are discussed and their impact on thermal conductivity enhancement presented.
最近的研究揭示了四声子散射过程在二维材料热导率（k）中的重要性。研究表明，在第一原理中加入 4 个声子散射过程，可使石墨烯在 300 K 时的热导率达到约 1290 W/mK，大大低于仅根据 3 个声子散射过程预测的超过 4000 W/mK 的数值。研究表明，四声子过程对挠曲ZA声子模式最为重要，相对于三声子散射过程，反射对称性选择规则（RSSR）对四声子散射过程的限制较少。这与 ZA 声子模式的低频相结合，导致了石墨烯在 300 K 时，低频 ZA 声子模式的高群体导致了比 3 声子散射更高的 4 声子散射。石墨烯纳米片（GnPs）等材料在增强聚合物复合材料导热性方面已得到广泛研究。然而，由于聚合物与填充材料之间的界面导热性较差，这种增强作用受到了限制。相互连接的填料网络通过在整个复合材料中形成高效的连续渗透传热路径，克服了这一问题。事实证明，这种三维网络可实现超高的聚合物热导率，接近 ~100 W/mK，甚至超过几种金属的热导率。本综述讨论了实现这种互连三维填料网络的不同技术，如气凝胶、泡沫、冰模板、膨胀石墨、填料涂层聚合物颗粒的热压、多种填料之间的协同效应以及填料片的拼接，并介绍了它们对热导率增强的影响。
{"title":"Role of four-phonon processes in thermal conductivity of two-dimensional materials and thermal-transport enhancement arising from interconnected nanofiller networks in polymer/nanofiller composites","authors":"Swapneel S. Danayat,, Zarin Mona, Nayal Avinash, Roshan Sameer Annam, Jivtesh Garg","doi":"10.1039/d4nr01352b","DOIUrl":"https://doi.org/10.1039/d4nr01352b","url":null,"abstract":"Recent research has shed light on the importance of four-phonon scattering processes in the thermal conductivity (k) of 2D materials. Inclusion of 4 phonon scattering processes from first-principles has been shown to lead to a thermal conductivity of ~1290 W/mK in graphene at 300 K, significantly lower than values predicted to be in excess of 4000 W/mK based only on 3 phonon scattering processes. Four phonon processes are shown to be most significant for flexural ZA phonon modes, where the reflection symmetry selection rule (RSSR) is less restrictive for 4-phonon relative to 3-phonon scattering processes. This combined with the low frequencies of ZA phonon modes, leading to high populations leads to higher 4-phonon compared to 3-phonon scattering of low frequency ZA phonon modes in graphene at 300 K. In this review the role of parameters such as atomic structure, phonon dispersion and temperature on 4-phonon scattering processes in wide range of 2D materials is reviewed. Materials such as graphene nanoplatelets (GnPs) have been extensively investigated for enhancement of thermal conductivity of polymer composites. However, such enhancement is limited by the poor interfacial thermal conductance between polymer and filler material. Interconnected filler networks, overcome this issue, through highly efficient continuous percolative heat transfer paths throughout the composite. Such 3D networks have been shown to enable ultra-high polymer thermal conductivities, approaching ~100 W/mK, and exceeding that of even several metals. In this review, different techniques to achieve such interconnected 3D filler networks such as aerogels, foams, ice-templating, expanded graphite, hot pressing of filler coated polymer particles, synergy effect between multiple fillers, and stitching of filler sheets are discussed and their impact on thermal conductivity enhancement presented.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141333635","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muyao Wang, Xiaohan Liu, Xiaowei Huang, Liangliang Liu
Metallizing σ electrons provides a promising route to design high-temperature superconducting materials, such as MgB2 and high-pressure hydrides. Here, we focus on two MgB2-like layered carborides of Li2BC3 and LiBC, in which their bulks do not have superconductivity because of B-C σ states far away from the Fermi level (EF), while, based on the first-principles calculation, we found that upon both bulk systems are cleaved into surfaces with B-C termination, high Tc of ~ 80 K could be observed in the exposed B-C layer at their surfaces. The detailed analysis reveals that surface symmetry reduction not only introduces hole self-doping into surface B-C layer and shifts its σ-bonding states towards crossing the EF associated with emergent large electronic occupation, but also makes in-plane stretching modes of surface layer experience significant softness. The enhanced σ states and softened phonon modes work intimately to produce strong coupling, thus to yield high-Tc surface superconductivity, which distinctly differs from the superconducting feature of MgB2 film that surface leads to phonon stiffness accompanied by suppressing the superconductivity. Our findings point to the importance of surface effect for achieving strong electron-phonon coupling superconductivity in Li2BC3 and LiBC, and also offer a practicable way to design more surface superconductors with high-Tc values in the future research via metallizing σ electrons.
{"title":"Surface inducing high-temperature superconductivity in layered metal carborides Li2BC3 and LiBC by metallizing σ electrons","authors":"Muyao Wang, Xiaohan Liu, Xiaowei Huang, Liangliang Liu","doi":"10.1039/d4nr01482k","DOIUrl":"https://doi.org/10.1039/d4nr01482k","url":null,"abstract":"Metallizing σ electrons provides a promising route to design high-temperature superconducting materials, such as MgB2 and high-pressure hydrides. Here, we focus on two MgB2-like layered carborides of Li2BC3 and LiBC, in which their bulks do not have superconductivity because of B-C σ states far away from the Fermi level (EF), while, based on the first-principles calculation, we found that upon both bulk systems are cleaved into surfaces with B-C termination, high Tc of ~ 80 K could be observed in the exposed B-C layer at their surfaces. The detailed analysis reveals that surface symmetry reduction not only introduces hole self-doping into surface B-C layer and shifts its σ-bonding states towards crossing the EF associated with emergent large electronic occupation, but also makes in-plane stretching modes of surface layer experience significant softness. The enhanced σ states and softened phonon modes work intimately to produce strong coupling, thus to yield high-Tc surface superconductivity, which distinctly differs from the superconducting feature of MgB2 film that surface leads to phonon stiffness accompanied by suppressing the superconductivity. Our findings point to the importance of surface effect for achieving strong electron-phonon coupling superconductivity in Li2BC3 and LiBC, and also offer a practicable way to design more surface superconductors with high-Tc values in the future research via metallizing σ electrons.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141319905","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Molybdenum disulfide (MoS2) attracts the attention of the scientific community due to its thickness dependent properties. To fully exploit these features, it is necessary to produce the material in mono or few-layers on a large scale. Several methodologies have been developed for this purpose, being the most promising one the liquid phase exfoliation (LPE). LPE allows to obtain good quality exfoliated MoS2 in a simple and scalable manner. Herein we report the simultaneous exfoliation and functionalization of MoS2 in chloroform using a specific porphyrin, namely tetrapyridyl porphyrin. We have corroborated that the exfoliation of MoS2 in the volatile solvent increases in the presence of the porphyrin due to the different interactions between them, obtaining good exfoliation yields. Additionally, the optical properties of the porphyrin are modified by these interactions. The characterization carried out by several techniques supports the hypothesis that the interactions occur through the pyridyl rings of the porphyrin and the molybdenum atoms of the material.
{"title":"Simultaneous exfoliation and functionalization of MoS2 with tetrapyridyl porphyrin","authors":"Marina Garrido, Alejandro Criado, Maurizio Prato","doi":"10.1039/d4nr01802h","DOIUrl":"https://doi.org/10.1039/d4nr01802h","url":null,"abstract":"Molybdenum disulfide (MoS2) attracts the attention of the scientific community due to its thickness dependent properties. To fully exploit these features, it is necessary to produce the material in mono or few-layers on a large scale. Several methodologies have been developed for this purpose, being the most promising one the liquid phase exfoliation (LPE). LPE allows to obtain good quality exfoliated MoS2 in a simple and scalable manner. Herein we report the simultaneous exfoliation and functionalization of MoS2 in chloroform using a specific porphyrin, namely tetrapyridyl porphyrin. We have corroborated that the exfoliation of MoS2 in the volatile solvent increases in the presence of the porphyrin due to the different interactions between them, obtaining good exfoliation yields. Additionally, the optical properties of the porphyrin are modified by these interactions. The characterization carried out by several techniques supports the hypothesis that the interactions occur through the pyridyl rings of the porphyrin and the molybdenum atoms of the material.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141319921","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Luca Schio, Gregor Bavdek, Cesare Grazioli, Claudia Obersnù, Albano Cossaro, Andrea Goldoni, Alberto Calloni, Alberto Bossi, Gianlorenzo Bussetti, Alessio Orbelli Biroli, Andrea Vittadini, Luca Floreano
Coordination polymers may be synthesized by linear bridging ligands to metal ions with conventional chemistry methods (e.g. in solution). Such complexes can be hardly brought onto a substrate with the chemical, spatial and geometrical homogeneity required for device integration. Instead, we follow an in-situ synthesis approach, where the anchoring points are provided by a monolayer of metal(II)-tetraphenylporphyrin (M-TPP, M = Cu, Zn, Co) grown in vacuum on the rutile-TiO2(110) surface. We probed the metal affinity to axial coordination by further deposition of symmetric dipyridyl-naphthalenediimide (DPNDI). By NEXAFS linear polarization dichroism, we show that DPNDI stands up on Zn- and Co-TPP thanks to axial coordination, whereas it lies down on the substrate for Cu-TPP. Calculations for a model pyridine ligand predict strong binding to Zn and Co cations, whose interaction with the O anions underneath is disrupted by surface trans effect. The weaker interactions between pyridine and Cu-TPP are then overcome by the strong attraction between TiO2 and DPNDI. The binding sites exposed by the homeotropic alignment of the ditopic DPNDI ligand on Zn- and Co-TPP are the foundations to grow coordination polymers preserving the lateral coherence of the basal layer.
{"title":"Seeding the vertical growth of laterally coherent coordination polymers on the rutile-TiO2(110) surface","authors":"Luca Schio, Gregor Bavdek, Cesare Grazioli, Claudia Obersnù, Albano Cossaro, Andrea Goldoni, Alberto Calloni, Alberto Bossi, Gianlorenzo Bussetti, Alessio Orbelli Biroli, Andrea Vittadini, Luca Floreano","doi":"10.1039/d4nr01309c","DOIUrl":"https://doi.org/10.1039/d4nr01309c","url":null,"abstract":"Coordination polymers may be synthesized by linear bridging ligands to metal ions with conventional chemistry methods (e.g. in solution). Such complexes can be hardly brought onto a substrate with the chemical, spatial and geometrical homogeneity required for device integration. Instead, we follow an in-situ synthesis approach, where the anchoring points are provided by a monolayer of metal(II)-tetraphenylporphyrin (M-TPP, M = Cu, Zn, Co) grown in vacuum on the rutile-TiO<small><sub>2</sub></small>(110) surface. We probed the metal affinity to axial coordination by further deposition of symmetric dipyridyl-naphthalenediimide (DPNDI). By NEXAFS linear polarization dichroism, we show that DPNDI stands up on Zn- and Co-TPP thanks to axial coordination, whereas it lies down on the substrate for Cu-TPP. Calculations for a model pyridine ligand predict strong binding to Zn and Co cations, whose interaction with the O anions underneath is disrupted by surface trans effect. The weaker interactions between pyridine and Cu-TPP are then overcome by the strong attraction between TiO<small><sub>2</sub></small> and DPNDI. The binding sites exposed by the homeotropic alignment of the ditopic DPNDI ligand on Zn- and Co-TPP are the foundations to grow coordination polymers preserving the lateral coherence of the basal layer.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141319889","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
In carbon allotropes, a series of topological semi-metals have been predicated, while both novel electronic properties and mechanics characters, e.g., negative Poisson’s rate (NPR), are rarely discovered in one sp2 type system. Here, a new three-dimensional carbon network, named WZGN, constructed with the distorted one-dimensional zigzag graphene nanoribbon is proposed. The stability of the system is fully ensured by the phonon dispersion, AIMD simulation, and binding energy calculations. Besides, it is investigated that the system holds both topologically protected nodal line semi-metal properties together with NPR property. Especially, the value of NPR can exceed -0.36 when 21% tensile uniaxial strain along the c’-direction is applied. Our findings point out that nodal line semi-metals can be compatible with intrinsic NPR properties in a wide strain range in carbon systems with sp2 hybridization, suggesting candidate applications in mechanics and electronic fields.
{"title":"Topological nodal line semi-metal with a negative Poisson's ratio in a three-dimensional carbon network with sp2 hybridization","authors":"Wen Jiang, Jun Jiang, zhixun Zhang, Wenjie Wu, Lichuan Zhang, Yuee Xie, Yuanping Chen","doi":"10.1039/d4nr01298d","DOIUrl":"https://doi.org/10.1039/d4nr01298d","url":null,"abstract":"In carbon allotropes, a series of topological semi-metals have been predicated, while both novel electronic properties and mechanics characters, e.g., negative Poisson’s rate (NPR), are rarely discovered in one sp2 type system. Here, a new three-dimensional carbon network, named WZGN, constructed with the distorted one-dimensional zigzag graphene nanoribbon is proposed. The stability of the system is fully ensured by the phonon dispersion, AIMD simulation, and binding energy calculations. Besides, it is investigated that the system holds both topologically protected nodal line semi-metal properties together with NPR property. Especially, the value of NPR can exceed -0.36 when 21% tensile uniaxial strain along the c’-direction is applied. Our findings point out that nodal line semi-metals can be compatible with intrinsic NPR properties in a wide strain range in carbon systems with sp2 hybridization, suggesting candidate applications in mechanics and electronic fields.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141319818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Daisuke Konish, Eri Hirata, Yuta Takano, Yukari Maeda, Natsumi Ushijima, Masako Yudasaka, Atsuro Yokoyama
Dental implant therapy is a reliable treatment for replacing missing teeth. However, as dental implants become more widely used, peri-implantitis increasingly has become a severe complication, making successful treatment more difficult. As a result, the development of effective drug delivery systems (DDSs) and treatments for peri-implantitis are urgently needed. Carbon nanohorns (CNHs) are carbon nanomaterials that have shown promise for use in DDSs and have photothermal effects. The present study exploited the unique properties of CNHs to develop a phototherapy employing a near-infrared (NIR) photoresponsive composite of minocycline, hyaluronan, and CNH (MC/HA/CNH) for peri-implantitis treatments. MC/HA/CNH demonstrated antibacterial effects that were potentiated by NIR-light irradiation, a property that was mediated by photothermal-mediated drug release from HA/CNH. These antibacterial effects persisted even following 48 h of dialysis, a promising indication for the clinical use of this material. We propose that the treatment of peri-implantitis using NIR and MC/HA/CNH, in combination with surgical procedures, might be employed to target relatively deep affected areas in a timely and efficacious manner. We envision that this innovative approach will pave the way for future developments in implant therapy.
{"title":"Near-infrared Light-boosted Antimicrobial Activity of Minocycline /Hyaluronan/ Carbon Nanohorn Composite toward peri-implantitis Treatments","authors":"Daisuke Konish, Eri Hirata, Yuta Takano, Yukari Maeda, Natsumi Ushijima, Masako Yudasaka, Atsuro Yokoyama","doi":"10.1039/d4nr01036a","DOIUrl":"https://doi.org/10.1039/d4nr01036a","url":null,"abstract":"Dental implant therapy is a reliable treatment for replacing missing teeth. However, as dental implants become more widely used, peri-implantitis increasingly has become a severe complication, making successful treatment more difficult. As a result, the development of effective drug delivery systems (DDSs) and treatments for peri-implantitis are urgently needed. Carbon nanohorns (CNHs) are carbon nanomaterials that have shown promise for use in DDSs and have photothermal effects. The present study exploited the unique properties of CNHs to develop a phototherapy employing a near-infrared (NIR) photoresponsive composite of minocycline, hyaluronan, and CNH (MC/HA/CNH) for peri-implantitis treatments. MC/HA/CNH demonstrated antibacterial effects that were potentiated by NIR-light irradiation, a property that was mediated by photothermal-mediated drug release from HA/CNH. These antibacterial effects persisted even following 48 h of dialysis, a promising indication for the clinical use of this material. We propose that the treatment of peri-implantitis using NIR and MC/HA/CNH, in combination with surgical procedures, might be employed to target relatively deep affected areas in a timely and efficacious manner. We envision that this innovative approach will pave the way for future developments in implant therapy.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141319949","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Charly Hélaine, Abdallah Amedlous, Jérôme Toutain, Carole Brunaud, Oleg Lebedev, Charlotte Marie, Cyrille Alliot, Myriam Bernaudin, Ferid Haddad, Svetlana Mintova and Samuel Valable
Nanoparticles have emerged as promising theranostic tools for biomedical applications, notably in the treatment of cancers. However, to fully exploit their potential, a thorough understanding of their biodistribution is imperative. In this context, we prepared radioactive [64Cu]-exchanged faujasite nanosized zeolite ([64Cu]-FAU) to conduct positron emission tomography (PET) imaging tracking in preclinical glioblastoma models. In vivo results revealed a rapid and gradual accumulation over time of intravenously injected [64Cu]-FAU zeolite nanocrystals within the brain tumor, while no uptake in the healthy brain was observed. Although a specific tumor targeting was observed in the brain, the kinetics of uptake into tumor tissue was found to be dependent on the glioblastoma model. Indeed, our results showed a rapid uptake in U87-MG model while in U251-MG glioblastoma model tumor uptake was gradual over the time. Interestingly, a [64Cu] activity, decreasing over time, was also observed in organs of elimination such as kidney and liver without showing a difference in activity between both glioblastoma models. Ex vivo analyses confirmed the presence of zeolite nanocrystals in brain tumor with detection of both Si and Al elements originated from them. This radiolabelling strategy, performed for the first time using nanozeolites, enables precise tracking through PET imaging and confirms their accumulation within the glioblastoma. These findings further bolster the potential use of zeolite nanocrystals as valuable theranostic tools.
纳米粒子已成为生物医学应用中前景广阔的治疗工具，尤其是在癌症治疗方面。然而，要充分挖掘其潜力，就必须对其生物分布有透彻的了解。在此背景下，我们制备了放射性[64Cu]-交换褐铁矿纳米沸石（[64Cu]-FAU），在临床前胶质母细胞瘤模型中进行正电子发射断层扫描（PET）成像跟踪。体内研究结果表明，静脉注射的[64Cu]-FAU沸石纳米晶体在脑肿瘤内随着时间的推移迅速逐渐积累，而在健康脑内则未观察到吸收。虽然在大脑中观察到了特定的肿瘤靶向性，但发现肿瘤组织的吸收动力学取决于胶质母细胞瘤模型。事实上，我们的研究结果表明，U87-MG 模型中的摄取速度很快，而在 U251-MG 胶质母细胞瘤模型中，肿瘤的摄取是随着时间的推移逐渐进行的。有趣的是，在肾脏和肝脏等排泄器官中也观察到[64Cu]活性随着时间的推移而降低，但两种胶质母细胞瘤模型的活性并无差异。体内外分析证实了脑肿瘤中存在沸石纳米晶体，并检测到其中的硅和铝元素。这是首次使用纳米沸石进行放射性标记，可通过 PET 成像进行精确跟踪，并确认它们在胶质母细胞瘤内的积累情况。这些发现进一步增强了沸石纳米晶体作为有价值的治疗工具的潜在用途。
{"title":"In vivo biodistribution and tumor uptake of [64Cu]-FAU nanozeolite via positron emission tomography Imaging†","authors":"Charly Hélaine, Abdallah Amedlous, Jérôme Toutain, Carole Brunaud, Oleg Lebedev, Charlotte Marie, Cyrille Alliot, Myriam Bernaudin, Ferid Haddad, Svetlana Mintova and Samuel Valable","doi":"10.1039/D3NR05947B","DOIUrl":"10.1039/D3NR05947B","url":null,"abstract":"<p >Nanoparticles have emerged as promising theranostic tools for biomedical applications, notably in the treatment of cancers. However, to fully exploit their potential, a thorough understanding of their biodistribution is imperative. In this context, we prepared radioactive [<small><sup>64</sup></small>Cu]-exchanged faujasite nanosized zeolite ([<small><sup>64</sup></small>Cu]-FAU) to conduct positron emission tomography (PET) imaging tracking in preclinical glioblastoma models. <em>In vivo</em> results revealed a rapid and gradual accumulation over time of intravenously injected [<small><sup>64</sup></small>Cu]-FAU zeolite nanocrystals within the brain tumor, while no uptake in the healthy brain was observed. Although a specific tumor targeting was observed in the brain, the kinetics of uptake into tumor tissue was found to be dependent on the glioblastoma model. Indeed, our results showed a rapid uptake in U87-MG model while in U251-MG glioblastoma model tumor uptake was gradual over the time. Interestingly, a [<small><sup>64</sup></small>Cu] activity, decreasing over time, was also observed in organs of elimination such as kidney and liver without showing a difference in activity between both glioblastoma models. <em>Ex vivo</em> analyses confirmed the presence of zeolite nanocrystals in brain tumor with detection of both Si and Al elements originated from them. This radiolabelling strategy, performed for the first time using nanozeolites, enables precise tracking through PET imaging and confirms their accumulation within the glioblastoma. These findings further bolster the potential use of zeolite nanocrystals as valuable theranostic tools.</p>","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":5.8,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2024/nr/d3nr05947b?page=search","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141316027","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The conductive bridge random access memories (CBRAMs) exhibit great potential as the next-generation nonvolatile memories. However, they suffer from two major disadvantages, such as the relatively high power consumption and large cycle-to-cycle and device-to-device variations, which hinder their more extensive commercialization. To learn how to enhance their device performance, the kinetic Monte Carlo (KMC) simulations were employed to illustrate variation of electroforming processes in nanomanipulated CBRAMs through introducing an ion-blocking layer with scalable nanopores and tuning microstructures of dielectric layers. Both the size of nanopores and inhomogeneity of dielectric layers have significant impacts on the forming processes of conductive filaments. The dielectric layer with high-content loose texture plus the scalable-nanopores-containing ion-blocking layer leads to formation of size-controlled and uniform filaments, which remarkably contributes to miniaturizable and stable CBRAMs. Our study provides insights into nanomanipulation strategies to realize high-performance CBRAMs, still awaiting future experimental confirmation.
{"title":"Kinetic Monte Carlo simulations on electroforming in nanomanipulated conductive bridge random access memories","authors":"Yi-Chen Li, Ping Xi, Yang-Yang Lv, Wei Fa, Shuang Chen","doi":"10.1039/d4nr01546k","DOIUrl":"https://doi.org/10.1039/d4nr01546k","url":null,"abstract":"The conductive bridge random access memories (CBRAMs) exhibit great potential as the next-generation nonvolatile memories. However, they suffer from two major disadvantages, such as the relatively high power consumption and large cycle-to-cycle and device-to-device variations, which hinder their more extensive commercialization. To learn how to enhance their device performance, the kinetic Monte Carlo (KMC) simulations were employed to illustrate variation of electroforming processes in nanomanipulated CBRAMs through introducing an ion-blocking layer with scalable nanopores and tuning microstructures of dielectric layers. Both the size of nanopores and inhomogeneity of dielectric layers have significant impacts on the forming processes of conductive filaments. The dielectric layer with high-content loose texture plus the scalable-nanopores-containing ion-blocking layer leads to formation of size-controlled and uniform filaments, which remarkably contributes to miniaturizable and stable CBRAMs. Our study provides insights into nanomanipulation strategies to realize high-performance CBRAMs, still awaiting future experimental confirmation.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":null,"pages":null},"PeriodicalIF":6.7,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141319883","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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