The therapeutic efficacy of chemotherapy in various malignancies and solid tumors is significantly limited when used as monotherapy. This study explored a combined treatment approach for breast cancer cells involving sequential delivery of doxorubicin followed by quercetin, both delivered via polydimethylsiloxane nanoparticles decorated with hyaluronic acid. Quercetin inhibits P-glycoprotein efflux action to enhance doxorubicin activity by increasing its intracellular accumulation; hence, both synergistically suppress cancer cell growth by promoting cytotoxicity and apoptosis. Quercetin reverses multidrug resistance, induces arrest in the cell cycle, and alters the mitochondrial membrane potential. The successful delivery and internalization of these drugs into breast cancer cells were confirmed through CD44 ligand recognition, inhibiting cell viability via apoptosis (caspase-induced) and cell arrest in the G2/M phase of the cell cycle. Furthermore, MCF-7 (breast cancer) cells-derived xenograft tumor model using NOD/SCID mice, the core-shell PDMS-HA nanoparticle system carrying quercetin and doxorubicin resulted in approximately 65% of tumor volume reduction, outperforming the loaded single drug and free drug combination. These results were supported by the TUNEL assay and proliferation index by Ki-67 immunohistochemistry staining, which shows substantial cell death and tissue necrosis in the tumor sections. Histological studies of tumor tissues confirm enhanced anticancer efficacy with negligible systemic toxicity to normal organs. Overall, the PDMS-HA delivery system efficiently transports quercetin and doxorubicin to tumor cells, enhancing the antitumor effects against the MCF-7 tumor xenograft model in mice without adverse effects. This study suggests that the targeted co-delivery of phytochemicals and anti-cancer agents can synergistically overcome many barriers associated with tumor treatment.
{"title":"Active Tumor Targeting by Core-Shell PDMS-HA Nanoparticles with Sequential Delivery of Doxorubicin and Quercetin to overcome P-glycoprotein efflux pump","authors":"Madhu Verma, Krishna Yadav, Rashmi Parihar, Debjani Dutta, Surabhi Chaudhuri, Sivakumar Sri","doi":"10.1039/d4nr03040k","DOIUrl":"https://doi.org/10.1039/d4nr03040k","url":null,"abstract":"The therapeutic efficacy of chemotherapy in various malignancies and solid tumors is significantly limited when used as monotherapy. This study explored a combined treatment approach for breast cancer cells involving sequential delivery of doxorubicin followed by quercetin, both delivered via polydimethylsiloxane nanoparticles decorated with hyaluronic acid. Quercetin inhibits P-glycoprotein efflux action to enhance doxorubicin activity by increasing its intracellular accumulation; hence, both synergistically suppress cancer cell growth by promoting cytotoxicity and apoptosis. Quercetin reverses multidrug resistance, induces arrest in the cell cycle, and alters the mitochondrial membrane potential. The successful delivery and internalization of these drugs into breast cancer cells were confirmed through CD44 ligand recognition, inhibiting cell viability via apoptosis (caspase-induced) and cell arrest in the G2/M phase of the cell cycle. Furthermore, MCF-7 (breast cancer) cells-derived xenograft tumor model using NOD/SCID mice, the core-shell PDMS-HA nanoparticle system carrying quercetin and doxorubicin resulted in approximately 65% of tumor volume reduction, outperforming the loaded single drug and free drug combination. These results were supported by the TUNEL assay and proliferation index by Ki-67 immunohistochemistry staining, which shows substantial cell death and tissue necrosis in the tumor sections. Histological studies of tumor tissues confirm enhanced anticancer efficacy with negligible systemic toxicity to normal organs. Overall, the PDMS-HA delivery system efficiently transports quercetin and doxorubicin to tumor cells, enhancing the antitumor effects against the MCF-7 tumor xenograft model in mice without adverse effects. This study suggests that the targeted co-delivery of phytochemicals and anti-cancer agents can synergistically overcome many barriers associated with tumor treatment.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"52 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975228","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}
Olga Kamanina, Pavel Rybochkin, Daria Borzova, Vitaliy N. Soromotin, Alexey Galushko, Alexey S. Kashin, Nina Ivanova, Anton Zvonarev, Natalia Suzina, Angelina Holicheva, Daniil Boiko, Vyacheslav Arlyapov, Valentine P. Ananikov
Adapting biological systems for nanoparticle synthesis opens an orthogonal Green direction in nanoscience by reducing the reliance on harsh chemicals and energy-intensive procedures. This study addresses the challenge of efficient catalyst preparation for organic synthesis, focusing on the rapid formation of palladium (Pd) nanoparticles using bacterial cells as a renewable and eco-friendly support. The preparation of catalytically active nanoparticles on the bacterium Paracoccus yeei represents a more suitable approach to increase the reaction efficiency due to its resistance to metal salts. We introduce an efficient method that significantly reduces the preparation time of Pd nanoparticles on Paracoccus yeei VKM B-3302 bacteria to only 7 min, greatly accelerating the process compared with traditional methods. Our findings reveal the major role of live bacterial cells in the formation and stabilization of Pd nanoparticles, which exhibit high catalytic activity in the Mizoroki–Heck reaction. This method not only ensures high yields of the desired product but also offers a greener and more sustainable alternative to conventional catalytic processes. The rapid preparation and high efficiency of this biohybrid catalyst opens new perspectives for the application of biosupported nanoparticles in organic synthesis and a transformative sustainable pathway for chemical production processes.
{"title":"Sustainable Catalysts in a Short Time: Harnessing Bacteria for Swift Palladium Nanoparticle Production","authors":"Olga Kamanina, Pavel Rybochkin, Daria Borzova, Vitaliy N. Soromotin, Alexey Galushko, Alexey S. Kashin, Nina Ivanova, Anton Zvonarev, Natalia Suzina, Angelina Holicheva, Daniil Boiko, Vyacheslav Arlyapov, Valentine P. Ananikov","doi":"10.1039/d4nr03661a","DOIUrl":"https://doi.org/10.1039/d4nr03661a","url":null,"abstract":"Adapting biological systems for nanoparticle synthesis opens an orthogonal Green direction in nanoscience by reducing the reliance on harsh chemicals and energy-intensive procedures. This study addresses the challenge of efficient catalyst preparation for organic synthesis, focusing on the rapid formation of palladium (Pd) nanoparticles using bacterial cells as a renewable and eco-friendly support. The preparation of catalytically active nanoparticles on the bacterium Paracoccus yeei represents a more suitable approach to increase the reaction efficiency due to its resistance to metal salts. We introduce an efficient method that significantly reduces the preparation time of Pd nanoparticles on Paracoccus yeei VKM B-3302 bacteria to only 7 min, greatly accelerating the process compared with traditional methods. Our findings reveal the major role of live bacterial cells in the formation and stabilization of Pd nanoparticles, which exhibit high catalytic activity in the Mizoroki–Heck reaction. This method not only ensures high yields of the desired product but also offers a greener and more sustainable alternative to conventional catalytic processes. The rapid preparation and high efficiency of this biohybrid catalyst opens new perspectives for the application of biosupported nanoparticles in organic synthesis and a transformative sustainable pathway for chemical production processes.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"68 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975230","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}
Atikur Hassan, Ayush Kumar, Sk Abdul Wahed, Subhadip Mondal, Amit Kumar, Neeladri Das
Covalent organic frameworks (COFs) are crystalline porous materials bearing well-ordered two- or three-dimensional molecular tectons in their polymeric skeletal framework. COFs are structurally robust as well as physiochemically stable. Recently, these are being developed for their use as “heterogeneous catalysts” for various organic transformations. In particular, research in the use of COFs for catalysis for different C-C cross-coupling reactions is in its infancy. To date, COF catalysts reported for such reactions bear Pd(II) bound to an exclusive coordination environment and have been explored for a particular organic reaction. Herein, we report, for the first time, a COF (Pd@COF-TFP_TzPy) that can anchor Pd(II) units in the polymeric framework in two different coordination environments. Thus, Pd@COF-TFP_TzPy is a porous material with dual confinement environment for Pd(II) units. The precursor COF (COF-TFP_TzPy) was easily synthesized and it features a two-dimensional hexagonal sheet structure, for facile incorporation of Pd(II) ions. Loading of Pd(II) in Pd@COF-TFP_TzPy was low (4.859 wt% of Pd), yet the material exhibited excellent catalytic activity in the diverse C-C cross-coupling reactions with broad substrate scope. Furthermore, Pd@COF-TFP_TzPy is highly stable and recyclable, thereby ensuring sustainable utilization of expensive Pd metal. We anticipate that our approach will stimulate further research into designing and utilizing functional COF materials for catalysis.
{"title":"Simultaneous Pore Confinement and Sidewall Modification of a N-rich COF with Pd(II): An Efficient and Sustainable Heterogeneous Catalyst for Cross-coupling Reactions","authors":"Atikur Hassan, Ayush Kumar, Sk Abdul Wahed, Subhadip Mondal, Amit Kumar, Neeladri Das","doi":"10.1039/d4nr03796k","DOIUrl":"https://doi.org/10.1039/d4nr03796k","url":null,"abstract":"Covalent organic frameworks (COFs) are crystalline porous materials bearing well-ordered two- or three-dimensional molecular tectons in their polymeric skeletal framework. COFs are structurally robust as well as physiochemically stable. Recently, these are being developed for their use as “heterogeneous catalysts” for various organic transformations. In particular, research in the use of COFs for catalysis for different C-C cross-coupling reactions is in its infancy. To date, COF catalysts reported for such reactions bear Pd(II) bound to an exclusive coordination environment and have been explored for a particular organic reaction. Herein, we report, for the first time, a COF (Pd@COF-TFP_TzPy) that can anchor Pd(II) units in the polymeric framework in two different coordination environments. Thus, Pd@COF-TFP_TzPy is a porous material with dual confinement environment for Pd(II) units. The precursor COF (COF-TFP_TzPy) was easily synthesized and it features a two-dimensional hexagonal sheet structure, for facile incorporation of Pd(II) ions. Loading of Pd(II) in Pd@COF-TFP_TzPy was low (4.859 wt% of Pd), yet the material exhibited excellent catalytic activity in the diverse C-C cross-coupling reactions with broad substrate scope. Furthermore, Pd@COF-TFP_TzPy is highly stable and recyclable, thereby ensuring sustainable utilization of expensive Pd metal. We anticipate that our approach will stimulate further research into designing and utilizing functional COF materials for catalysis.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"58 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981603","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}
Rares Banu, Adea Loxha, Nicole Mueller Mueller, Stylianos Spyroglou, Egon Erwin Rosenberg, E Palomares, Fernando Rey, C. Marini, Noelia Barrabes
In the field of nanocluster catalysis, it is crucial to understand the interplay of different parameters, such as ligands, support and pretreatment and their effect on the catalytic process. In this study we chose the selective hydrogenation of phenylacetylene as a model reaction and employed two gold nanoclusters as catalysts, the phosphine protected Au11 and the thiolate protected Au25, each with different binding motifs and supported them on MgO, Al2O3 and a hydrotalcite (HT), chosen for their different acidity. We found that while in the case of the Au11 MgO was the preferred support and the pretreatment had a positive impact on the catalysis, for the Au25 the HT performed best and pretreating had negative effects, indicating that the bonding motif of the ligands and their interaction with the support is crucial for the catalytic process. Using X-Ray absorption spectroscopy we could trace these phenomena to changes in the cluster-ligand interface, which seem to impact on the stability of the catalysts.
{"title":"Synergistic Effect of Ligand-Cluster Structure and Support in Gold Nanocluster Catalysts for Selective Hydrogenation of Alkynes","authors":"Rares Banu, Adea Loxha, Nicole Mueller Mueller, Stylianos Spyroglou, Egon Erwin Rosenberg, E Palomares, Fernando Rey, C. Marini, Noelia Barrabes","doi":"10.1039/d4nr03865g","DOIUrl":"https://doi.org/10.1039/d4nr03865g","url":null,"abstract":"In the field of nanocluster catalysis, it is crucial to understand the interplay of different parameters, such as ligands, support and pretreatment and their effect on the catalytic process. In this study we chose the selective hydrogenation of phenylacetylene as a model reaction and employed two gold nanoclusters as catalysts, the phosphine protected Au11 and the thiolate protected Au25, each with different binding motifs and supported them on MgO, Al2O3 and a hydrotalcite (HT), chosen for their different acidity. We found that while in the case of the Au11 MgO was the preferred support and the pretreatment had a positive impact on the catalysis, for the Au25 the HT performed best and pretreating had negative effects, indicating that the bonding motif of the ligands and their interaction with the support is crucial for the catalytic process. Using X-Ray absorption spectroscopy we could trace these phenomena to changes in the cluster-ligand interface, which seem to impact on the stability of the catalysts.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"29 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975227","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}
Laura G. Vivas, Alejandra Ruiz de Clavijo, Olga Caballero-Calero, David Navas, Amanda A. Ordoñez-Cencerrado, Cristina V. Manzano, Ruy Sanz, Marisol S. Martín-González
Three-dimensional magnetic nanowire networks (3DNNs) have shown promise for applications beyond those of their linear counterparts. However, understanding the underlying magnetization reversal mechanisms has been limited. In this study, we present a combined experimental and computational investigation on simplified 3DNNs to address this gap. Our findings reveal a previously unidentified in-plane magnetoelastic anisotropy, validated through comparisons between experimental and simulated magnetic data. Notably, we discovered that magnetization reversal in 3DNNs is driven by highly localized magnetic states, arising from the interplay of exchange and dipolar interactions, magnetoelastic anisotropy, and nanowire microstructure. This discovery challenges the prevailing understanding of magnetization reversal in nickel nanowires. Our work provides critical insights into the magnetic behavior of 3DNNs, opening doors for their tailored design and optimization.
{"title":"Magnetoelastic Anisotropy Drives Localized Magnetization Reversal in 3D Nanowire Networks","authors":"Laura G. Vivas, Alejandra Ruiz de Clavijo, Olga Caballero-Calero, David Navas, Amanda A. Ordoñez-Cencerrado, Cristina V. Manzano, Ruy Sanz, Marisol S. Martín-González","doi":"10.1039/d4nr04078c","DOIUrl":"https://doi.org/10.1039/d4nr04078c","url":null,"abstract":"Three-dimensional magnetic nanowire networks (3DNNs) have shown promise for applications beyond those of their linear counterparts. However, understanding the underlying magnetization reversal mechanisms has been limited. In this study, we present a combined experimental and computational investigation on simplified 3DNNs to address this gap. Our findings reveal a previously unidentified in-plane magnetoelastic anisotropy, validated through comparisons between experimental and simulated magnetic data. Notably, we discovered that magnetization reversal in 3DNNs is driven by highly localized magnetic states, arising from the interplay of exchange and dipolar interactions, magnetoelastic anisotropy, and nanowire microstructure. This discovery challenges the prevailing understanding of magnetization reversal in nickel nanowires. Our work provides critical insights into the magnetic behavior of 3DNNs, opening doors for their tailored design and optimization.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"28 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975231","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}
José Fernando Rubio-Valle, Concepcion Valencia, J. E. Martin-Alfonso, Estrada Villegas, José M. Franco
This study explores the preparation of lubricating oleo-dispersions using electrospun nanofibrous mats made from low-sulfonate lignin (LSL) and polycaprolactone (PCL).The rheological and tribological properties of the oleo-dispersions were significantly modulated for the first time through the exploration of LSL/PCL ratio and electrospinning conditions such as applied voltage, distance between the tip and collector, flow rate, ambient humidity, and collector configuration. Adequate uniform ultrathin fibers and Small Amplitude Oscillation (SAOS) functions of the oleo-dispersions, with storage modulus values ranging from 102 to 105 Pa at 25ºC, were obtained with a flow rate of 0.5 ml/h, an applied voltage of 15 kV, relative humidity 45% and a static collector. The LSL/PCL ratio directly affected the mechanical properties of the membranes, influencing stiffness and wear resistance. Higher PCL content enhanced membrane stiffness, reflected in increased SAOS values, but also led to higher friction coefficients (from 0.11 to 0.18) and more pronounced wear traces (measured by wear diameter: 440 to 860 µm). These interactions underscore the complex relationship between micro-nano structure and tribological performance. This study establishes a clear link between electrospinning conditions and the performance of oleo-dispersions, offering a versatile platform for the development of customizable, renewable lubricants. These findings contribute to the advancement of sustainable lubrication technologies, demonstrating the potential of tailor-made oleo-dispersions as alternatives to traditional lubricants
{"title":"Exploration of low-sulfonate lignin electrospinning conditions for the development of new renewable lubricant formulations","authors":"José Fernando Rubio-Valle, Concepcion Valencia, J. E. Martin-Alfonso, Estrada Villegas, José M. Franco","doi":"10.1039/d4nr04426f","DOIUrl":"https://doi.org/10.1039/d4nr04426f","url":null,"abstract":"This study explores the preparation of lubricating oleo-dispersions using electrospun nanofibrous mats made from low-sulfonate lignin (LSL) and polycaprolactone (PCL).The rheological and tribological properties of the oleo-dispersions were significantly modulated for the first time through the exploration of LSL/PCL ratio and electrospinning conditions such as applied voltage, distance between the tip and collector, flow rate, ambient humidity, and collector configuration. Adequate uniform ultrathin fibers and Small Amplitude Oscillation (SAOS) functions of the oleo-dispersions, with storage modulus values ranging from 102 to 105 Pa at 25ºC, were obtained with a flow rate of 0.5 ml/h, an applied voltage of 15 kV, relative humidity 45% and a static collector. The LSL/PCL ratio directly affected the mechanical properties of the membranes, influencing stiffness and wear resistance. Higher PCL content enhanced membrane stiffness, reflected in increased SAOS values, but also led to higher friction coefficients (from 0.11 to 0.18) and more pronounced wear traces (measured by wear diameter: 440 to 860 µm). These interactions underscore the complex relationship between micro-nano structure and tribological performance. This study establishes a clear link between electrospinning conditions and the performance of oleo-dispersions, offering a versatile platform for the development of customizable, renewable lubricants. These findings contribute to the advancement of sustainable lubrication technologies, demonstrating the potential of tailor-made oleo-dispersions as alternatives to traditional lubricants","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"9 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981602","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}
Muhammad Hussnain Afzal, Wajeeha Pervaiz, Zhuo Huang, Zhengyun Wang, Guangfang Li, Hongfang Liu
Acetaminophen (AP) is a widely used analgesic and antipyretic drug, but its excessive use poses health risks and contributes to environmental contamination. In response to the need for rapid, accurate, and cost-effective detection methods, we developed a highly sensitive and selective electrochemical sensor for AP. The sensor was based on a composite of UIO-66-NH2 (UN) and MXene (Ti3C2). The UIO-66-NH2 was in-situ synthesized onto the MXene via a one-step hydrothermal process with varying MXene content, followed by calcination at 300ºC under argon (Ar) flow. This treatment induced the formation of TiO2 on the MXene surface and increased the interlayer spacing, which enhanced its electrochemical performance. The resulting UN@Ti3C2-C electrode exhibited remarkable electrochemical activity due to the high surface area and excellent conductivity of MXene. The fabricated sensor demonstrated a simple yet effective approach for the rapid and quantitative detection of AP, with a linear detection range of 0.032-160 µM and a low detection limit of 10 nM. Moreover, the sensor was successfully applied to detect AP in different water samples, validating its potential as a reliable and efficient tool for AP monitoring.
{"title":"In-Situ Synthesis of UIO-66-NH2@Ti3C2 Composite for Advanced Electrochemical Detection of Acetaminophen","authors":"Muhammad Hussnain Afzal, Wajeeha Pervaiz, Zhuo Huang, Zhengyun Wang, Guangfang Li, Hongfang Liu","doi":"10.1039/d4nr04388j","DOIUrl":"https://doi.org/10.1039/d4nr04388j","url":null,"abstract":"Acetaminophen (AP) is a widely used analgesic and antipyretic drug, but its excessive use poses health risks and contributes to environmental contamination. In response to the need for rapid, accurate, and cost-effective detection methods, we developed a highly sensitive and selective electrochemical sensor for AP. The sensor was based on a composite of UIO-66-NH<small><sub>2</sub></small> (UN) and MXene (Ti<small><sub>3</sub></small>C<small><sub>2</sub></small>). The UIO-66-NH<small><sub>2</sub></small> was in-situ synthesized onto the MXene via a one-step hydrothermal process with varying MXene content, followed by calcination at 300ºC under argon (Ar) flow. This treatment induced the formation of TiO<small><sub>2</sub></small> on the MXene surface and increased the interlayer spacing, which enhanced its electrochemical performance. The resulting UN@Ti<small><sub>3</sub></small>C<small><sub>2</sub></small>-C electrode exhibited remarkable electrochemical activity due to the high surface area and excellent conductivity of MXene. The fabricated sensor demonstrated a simple yet effective approach for the rapid and quantitative detection of AP, with a linear detection range of 0.032-160 µM and a low detection limit of 10 nM. Moreover, the sensor was successfully applied to detect AP in different water samples, validating its potential as a reliable and efficient tool for AP monitoring.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"91 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975229","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}
Siyu Chen, Mariem Triki, Simone Pinto Carneiro, Olivia M Merkel
CRISPR-Cas9 has emerged as a highly effective and customizable genome editing tool, holding significant promise for the treatment of KRAS mutations in lung cancer. In this study, we introduce a novel micelleplex, named C14-PEI, designed to co-deliver Cas9 mRNA and sgRNA efficiently to excise the mutated KRAS allele in lung cancer cells. C14-PEI is synthesised from 1,2-epoxytetradecane and branched PEI 600 Da via a ring-opening reaction. The resulting C14-PEI has a critical micelle concentration (CMC) of approximately 20.86 ± 0.15 mg/L, indicating its ability to form stable micelles at low concentrations. C14-PEI efficiently encapsulates mRNA into micelleplexes through electrostatic interactions. When the mass ratio is 8 (w/w 8), the C14-PEI formulation exhibits conducive properties, which showed encapsulation efficiency of eGFP mRNA at 99% and led to a 130-fold increase in eGFP expression in A549 cells compared to untreated cells, demonstrating the robust delivery and expression capability of the micelleplexes. Importantly, toxicity tests using intracellular reduction of a tetrazolium salt revealed no significant cytotoxicity, underscoring the biocompatibility of C14-PEI. C14-PEI also shows high efficiency in co-encapsulating Cas9 mRNA and sgRNA, as confirmed by agarose gel electrophoresis. At an sgRNA to Cas9 mRNA molar ratio of 10, the micelleplexes successfully mediate the cutting of mutated KRAS with an indel efficiency exceeding 60%, as determined by the T7 Endonuclease I (T7EI) assay. Digital droplet PCR (ddPCR) further demonstrates that the gene editing efficiency, measured by edited gene copies, is 48.5% in the w/w 4 group and 37.8% in the w/w 8 group. Treatment with C14-PEI micelleplexes containing Cas9 mRNA and sgRNA targeting the KRAS G12S mutation significantly impairs the migration capability of A549 cells and increases apoptosis rates. These findings suggest that C14-PEI effectively disrupts KRAS signalling pathways, leading to reduced tumor cell proliferation and enhanced cell death.
{"title":"A Novel Micelleplex for Tumour-Targeted Delivery of CRISPR-Cas9 against KRAS-Mutated Lung Cancer","authors":"Siyu Chen, Mariem Triki, Simone Pinto Carneiro, Olivia M Merkel","doi":"10.1039/d4nr03471f","DOIUrl":"https://doi.org/10.1039/d4nr03471f","url":null,"abstract":"CRISPR-Cas9 has emerged as a highly effective and customizable genome editing tool, holding significant promise for the treatment of KRAS mutations in lung cancer. In this study, we introduce a novel micelleplex, named C14-PEI, designed to co-deliver Cas9 mRNA and sgRNA efficiently to excise the mutated KRAS allele in lung cancer cells. C14-PEI is synthesised from 1,2-epoxytetradecane and branched PEI 600 Da via a ring-opening reaction. The resulting C14-PEI has a critical micelle concentration (CMC) of approximately 20.86 ± 0.15 mg/L, indicating its ability to form stable micelles at low concentrations. C14-PEI efficiently encapsulates mRNA into micelleplexes through electrostatic interactions. When the mass ratio is 8 (w/w 8), the C14-PEI formulation exhibits conducive properties, which showed encapsulation efficiency of eGFP mRNA at 99% and led to a 130-fold increase in eGFP expression in A549 cells compared to untreated cells, demonstrating the robust delivery and expression capability of the micelleplexes. Importantly, toxicity tests using intracellular reduction of a tetrazolium salt revealed no significant cytotoxicity, underscoring the biocompatibility of C14-PEI. C14-PEI also shows high efficiency in co-encapsulating Cas9 mRNA and sgRNA, as confirmed by agarose gel electrophoresis. At an sgRNA to Cas9 mRNA molar ratio of 10, the micelleplexes successfully mediate the cutting of mutated KRAS with an indel efficiency exceeding 60%, as determined by the T7 Endonuclease I (T7EI) assay. Digital droplet PCR (ddPCR) further demonstrates that the gene editing efficiency, measured by edited gene copies, is 48.5% in the w/w 4 group and 37.8% in the w/w 8 group. Treatment with C14-PEI micelleplexes containing Cas9 mRNA and sgRNA targeting the KRAS G12S mutation significantly impairs the migration capability of A549 cells and increases apoptosis rates. These findings suggest that C14-PEI effectively disrupts KRAS signalling pathways, leading to reduced tumor cell proliferation and enhanced cell death.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"22 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968610","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}
V. G. Dileep Kumar, Swapna Pahra, Nieves López-Salas, Basavaraja M. Basavanakote, Afaq Ahmad Khan, Nagaraj Sumanth, Pooja Devi, M. S. Santosh
Alkali metal doping is a new and promising approach to enhance the photo/electrocatalytic activity of NiS-based catalyst systems. This work investigates the impact of sodium on the structural, electronic, and catalytic properties of NiS. Comprehensive characterization techniques demonstrate that Na-doping causes significant changes in the NiS lattice and surface chemistry translating into a larger bandgap than NiS. Photocatalytic experiments demonstrate 98.5% degradation of 2,4-DCP under visible light, attributing it to improved light absorption and charge separation by Na-NiS nanoparticles. The effect of pH and pKa on the degradation of 2,4-DCP has also been studied and reported. Additionally, electrochemical measurements indicate reduced overpotentials of 110 mV for Na-NiS compared to 336 mV by NiS nanoparticles towards hydrogen evolution reaction (HER). The material's overall water splitting is found to be 1.59 V at a current density of 10 mA/cm2. The results highlight the potential of Na-NiS as a versatile catalyst for environmental remediation and clean energy applications, paving the way for further exploration and optimization of doped transition metal sulfides.
{"title":"Enhancing NiS Performance: Na-Doping for Advanced Photocatalytic and Electrocatalytic Applications","authors":"V. G. Dileep Kumar, Swapna Pahra, Nieves López-Salas, Basavaraja M. Basavanakote, Afaq Ahmad Khan, Nagaraj Sumanth, Pooja Devi, M. S. Santosh","doi":"10.1039/d4nr04293j","DOIUrl":"https://doi.org/10.1039/d4nr04293j","url":null,"abstract":"Alkali metal doping is a new and promising approach to enhance the photo/electrocatalytic activity of NiS-based catalyst systems. This work investigates the impact of sodium on the structural, electronic, and catalytic properties of NiS. Comprehensive characterization techniques demonstrate that Na-doping causes significant changes in the NiS lattice and surface chemistry translating into a larger bandgap than NiS. Photocatalytic experiments demonstrate 98.5% degradation of 2,4-DCP under visible light, attributing it to improved light absorption and charge separation by Na-NiS nanoparticles. The effect of pH and pKa on the degradation of 2,4-DCP has also been studied and reported. Additionally, electrochemical measurements indicate reduced overpotentials of 110 mV for Na-NiS compared to 336 mV by NiS nanoparticles towards hydrogen evolution reaction (HER). The material's overall water splitting is found to be 1.59 V at a current density of 10 mA/cm2. The results highlight the potential of Na-NiS as a versatile catalyst for environmental remediation and clean energy applications, paving the way for further exploration and optimization of doped transition metal sulfides.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"28 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142975423","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}
Single atom alloys (SAAs) have gained tremendous attention as promising materials with unique physicochemical properties, particularly in catalysis. The stability of SAAs relies on the formation of a single active dopant on the surface of a metal host, quantified by the surface segregation and aggregation energy. Previous studies have investigated the surface segregation of non-ligated and ligated SAAs to reveal the driving forces underlying such phenomena. In this work we address another key factor dictating the stability in non-ligated and ligated SAAs: the aggregation energy (Eagg) of dopants. Specifically, we examine how thiols and amines, commonly found ligands in colloidal bimetallic nanoparticle synthesis, affect the aggregation of dopants (forming dimers and trimers) on the surface of a metal host. Utilizing Density Functional Theory (DFT) and machine learning (ML), we explore the stability patterns of SAAs through the energetics of low-index surfaces, such as (111) and (100), consisting of d8- (Pt, Pd, Ni) and d9- (Ag, Au, Cu) metals, both in the presence and absence of ligands. Collecting rich and accurate DFT data, we developed a four-feature support vector regression using the radial basis function (SVR RBF) to predict the Eagg. The model revealed important and easily accessible (tabulated) thermodynamic stability features that drive metal aggregation in SAAs, such as the bulk cohesive energy of the metal considering the exposed coordination environment on the surface, the charge transfer represented by the difference in electron affinities of metals and the radii of the metals describing strain effects. Additional incorporated features include adsorbate properties, such as the binding energy of the ligand on a single atom considering the coordination environment of the adsorbate. Through our study, we have revealed that stable SAAs are formed in Ni-, Pd-, Pt-based SAAs in the presence of ligands, while Ag-, Au-, Cu- doped with Ni-, Pd-, Pt- lead to aggregation. Finally, we tested our model against several experimental studies and demonstrated its robustness in predicting the formation of SAAs, enabling rapid screening across the vast material space of SAAs. Additionally, we suggest criteria for stabilization of SAAs, guiding experimental efforts. Overall, our study advances the understanding of thermodynamic stability of colloidal SAAs, paving the way for rational SAA design.
{"title":"Single Atom Alloys Aggregation in the Presence of Ligands","authors":"Maya Salem, Giannis Mpourmpakis","doi":"10.1039/d4nr04202f","DOIUrl":"https://doi.org/10.1039/d4nr04202f","url":null,"abstract":"Single atom alloys (SAAs) have gained tremendous attention as promising materials with unique physicochemical properties, particularly in catalysis. The stability of SAAs relies on the formation of a single active dopant on the surface of a metal host, quantified by the surface segregation and aggregation energy. Previous studies have investigated the surface segregation of non-ligated and ligated SAAs to reveal the driving forces underlying such phenomena. In this work we address another key factor dictating the stability in non-ligated and ligated SAAs: the aggregation energy (Eagg) of dopants. Specifically, we examine how thiols and amines, commonly found ligands in colloidal bimetallic nanoparticle synthesis, affect the aggregation of dopants (forming dimers and trimers) on the surface of a metal host. Utilizing Density Functional Theory (DFT) and machine learning (ML), we explore the stability patterns of SAAs through the energetics of low-index surfaces, such as (111) and (100), consisting of d8- (Pt, Pd, Ni) and d9- (Ag, Au, Cu) metals, both in the presence and absence of ligands. Collecting rich and accurate DFT data, we developed a four-feature support vector regression using the radial basis function (SVR RBF) to predict the Eagg. The model revealed important and easily accessible (tabulated) thermodynamic stability features that drive metal aggregation in SAAs, such as the bulk cohesive energy of the metal considering the exposed coordination environment on the surface, the charge transfer represented by the difference in electron affinities of metals and the radii of the metals describing strain effects. Additional incorporated features include adsorbate properties, such as the binding energy of the ligand on a single atom considering the coordination environment of the adsorbate. Through our study, we have revealed that stable SAAs are formed in Ni-, Pd-, Pt-based SAAs in the presence of ligands, while Ag-, Au-, Cu- doped with Ni-, Pd-, Pt- lead to aggregation. Finally, we tested our model against several experimental studies and demonstrated its robustness in predicting the formation of SAAs, enabling rapid screening across the vast material space of SAAs. Additionally, we suggest criteria for stabilization of SAAs, guiding experimental efforts. Overall, our study advances the understanding of thermodynamic stability of colloidal SAAs, paving the way for rational SAA design.","PeriodicalId":92,"journal":{"name":"Nanoscale","volume":"45 1","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142968571","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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