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Smart Vascular Grafts with Integrated Flow Biosensors for Hemodynamic Real-Time Monitoring and Vascular Healthcare
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acsnano.4c09980
Zhiqiang Ma, Jing Zhang, Shangjie Zou, Ke Huang, Wei Li, Mohamed Elhousseini Hilal, Mingze Zhu, Yatian Fu, Bee Luan Khoo
Real-time monitoring of hemodynamics is crucial for diagnosing disorders within implanted vascular grafts and facilitating timely treatment. Integrating vascular grafts with advanced flexible electronics offers a promising approach to developing smart vascular grafts (SVGs) capable of continuous hemodynamic monitoring. However, most existing SVG devices encounter significant challenges in practical applications, particularly regarding biomechanical compatibility and the effective evaluation of vascular status. Here, we present a state-of-the-art SVG device seamlessly integrated with flow biosensors constructed by encapsulating patterned porous graphene within biocompatible polymers. The innovative use of porous graphene imparts the SVG with exceptional mechanical sensing performance, featuring a low strain detection limit of 0.0034% and dynamic stability exceeding 32,400 cycles, thus enabling precise hemodynamic perception. This high sensitivity allows the SVG to accurately diagnose vascular disorders, such as blockage degree and position, by collecting hemodynamic data from an artificial artery model. In vitro thrombi (blood clot) diagnostics, treatment simulation experiments, and in vivo tests using a rabbit model strongly validate the SVG’s outstanding and reliable performance in vascular healthcare. We have also developed a stand-alone and wireless system, demonstrating its capability for remote monitoring and managing vascular health. Our pioneering SVG system showcases great potential in vascular healthcare for precise hemodynamic monitoring of disorders, timely diagnostics, and even drug screening.
{"title":"Smart Vascular Grafts with Integrated Flow Biosensors for Hemodynamic Real-Time Monitoring and Vascular Healthcare","authors":"Zhiqiang Ma, Jing Zhang, Shangjie Zou, Ke Huang, Wei Li, Mohamed Elhousseini Hilal, Mingze Zhu, Yatian Fu, Bee Luan Khoo","doi":"10.1021/acsnano.4c09980","DOIUrl":"https://doi.org/10.1021/acsnano.4c09980","url":null,"abstract":"Real-time monitoring of hemodynamics is crucial for diagnosing disorders within implanted vascular grafts and facilitating timely treatment. Integrating vascular grafts with advanced flexible electronics offers a promising approach to developing smart vascular grafts (SVGs) capable of continuous hemodynamic monitoring. However, most existing SVG devices encounter significant challenges in practical applications, particularly regarding biomechanical compatibility and the effective evaluation of vascular status. Here, we present a state-of-the-art SVG device seamlessly integrated with flow biosensors constructed by encapsulating patterned porous graphene within biocompatible polymers. The innovative use of porous graphene imparts the SVG with exceptional mechanical sensing performance, featuring a low strain detection limit of 0.0034% and dynamic stability exceeding 32,400 cycles, thus enabling precise hemodynamic perception. This high sensitivity allows the SVG to accurately diagnose vascular disorders, such as blockage degree and position, by collecting hemodynamic data from an artificial artery model. In vitro thrombi (blood clot) diagnostics, treatment simulation experiments, and in vivo tests using a rabbit model strongly validate the SVG’s outstanding and reliable performance in vascular healthcare. We have also developed a stand-alone and wireless system, demonstrating its capability for remote monitoring and managing vascular health. Our pioneering SVG system showcases great potential in vascular healthcare for precise hemodynamic monitoring of disorders, timely diagnostics, and even drug screening.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"23 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988168","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Strong and Fireproof Regenerated Wood via a Combined Phosphorylation-Surface Nanofibrillation and Ionic Cross-Linking Strategy
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acsnano.4c13857
Wen-Bin Sun, Zi-Meng Han, Xiao-Han Luo, Huai-Bin Yang, Zhao-Xiang Liu, De-Han Li, Kun-Peng Yang, Qing-Fang Guan, Shu-Hong Yu
To reduce the environmental impact of plastics, an increasing number of high-performance sustainable materials have emerged. Among them, wood-based high-performance structural materials have gained growing attention due to their outstanding mechanical and thermal properties. Here, we introduce phosphate groups onto the wood veneers for surface nanofibrillation, effectively altering both the molecular structure and surface morphology of wood, which enhances the interactions between wood veneers and endows the wood with excellent fire resistance properties. With these phosphorylated wood-based building blocks, “chemical welding” structural materials (CWSMs) obtained through chemical cross-linking exhibit excellent mechanical properties. The flexural strength of CWSM reaches 225 MPa, and the modulus reaches 16 GPa, surpassing those of various types of natural wood. At the same time, phosphorylation has endowed CWSM with excellent fire resistance, with a limiting oxygen index reaching 49%, making it completely noncombustible. More importantly, as a biomass-based structural material, CWSM exhibits mechanical, thermal, and fire resistance properties and degradability far superior to those of traditional petroleum-based plastics, making it an ideal candidate for plastic replacement.
{"title":"Strong and Fireproof Regenerated Wood via a Combined Phosphorylation-Surface Nanofibrillation and Ionic Cross-Linking Strategy","authors":"Wen-Bin Sun, Zi-Meng Han, Xiao-Han Luo, Huai-Bin Yang, Zhao-Xiang Liu, De-Han Li, Kun-Peng Yang, Qing-Fang Guan, Shu-Hong Yu","doi":"10.1021/acsnano.4c13857","DOIUrl":"https://doi.org/10.1021/acsnano.4c13857","url":null,"abstract":"To reduce the environmental impact of plastics, an increasing number of high-performance sustainable materials have emerged. Among them, wood-based high-performance structural materials have gained growing attention due to their outstanding mechanical and thermal properties. Here, we introduce phosphate groups onto the wood veneers for surface nanofibrillation, effectively altering both the molecular structure and surface morphology of wood, which enhances the interactions between wood veneers and endows the wood with excellent fire resistance properties. With these phosphorylated wood-based building blocks, “chemical welding” structural materials (CWSMs) obtained through chemical cross-linking exhibit excellent mechanical properties. The flexural strength of CWSM reaches 225 MPa, and the modulus reaches 16 GPa, surpassing those of various types of natural wood. At the same time, phosphorylation has endowed CWSM with excellent fire resistance, with a limiting oxygen index reaching 49%, making it completely noncombustible. More importantly, as a biomass-based structural material, CWSM exhibits mechanical, thermal, and fire resistance properties and degradability far superior to those of traditional petroleum-based plastics, making it an ideal candidate for plastic replacement.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"23 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988170","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Complex Core–Shell Architectures through Spatially Organized Nano-Assemblies
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acsnano.4c17322
Xiangyu Jiang, Bo Jiang, Manrui Mu, Tongyi Wang, Shi Sun, Jiaxin Xu, Shutao Wang, Yan Zhou, Jun Zhang, Wenle Li
Core–shell structures demonstrate superior capability in customizing properties across multiple scales, offering valuable potential in catalysis, medicine, and performance materials. Integrating functional nanoparticles in a spatially controlled manner is particularly appealing for developing sophisticated architectures that support heterogeneous characteristics and tandem reactions. However, creating such complex structures with site-specific features remains challenging due to the dynamic microenvironment during the shell-forming process, which considerably impacts colloidal particle assembly. Here, we describe a method to spatially deploy nanoscale assemblies within microscale structures comprising a dense shell and a liquid core through colloidal surface decoration coupled with emulsion-based synthesis. Exploiting a spectrum of nanoparticles grafted with incrementally varying densities of organic ligands, we reveal that nanofeatures can be selectively sculpted onto the shell exterior, within the shell wall, and on the interior surface. The versatility of this mechanism is validated by systematically arranging nanoparticles with various compositions, shapes, and dimensions. Spatially integrated nanotitania endows the core–shell structures with localized photocatalytic abilities. Additionally, distinctive surface modifications enable the simultaneous yet independent implantation of diverse nanoparticles, yielding intricate architectures with programmable functions. This generalizable approach showcases a synthetic strategy to attain structural complexity and functional sophistication reminiscent of those of biological systems in nature.
{"title":"Complex Core–Shell Architectures through Spatially Organized Nano-Assemblies","authors":"Xiangyu Jiang, Bo Jiang, Manrui Mu, Tongyi Wang, Shi Sun, Jiaxin Xu, Shutao Wang, Yan Zhou, Jun Zhang, Wenle Li","doi":"10.1021/acsnano.4c17322","DOIUrl":"https://doi.org/10.1021/acsnano.4c17322","url":null,"abstract":"Core–shell structures demonstrate superior capability in customizing properties across multiple scales, offering valuable potential in catalysis, medicine, and performance materials. Integrating functional nanoparticles in a spatially controlled manner is particularly appealing for developing sophisticated architectures that support heterogeneous characteristics and tandem reactions. However, creating such complex structures with site-specific features remains challenging due to the dynamic microenvironment during the shell-forming process, which considerably impacts colloidal particle assembly. Here, we describe a method to spatially deploy nanoscale assemblies within microscale structures comprising a dense shell and a liquid core through colloidal surface decoration coupled with emulsion-based synthesis. Exploiting a spectrum of nanoparticles grafted with incrementally varying densities of organic ligands, we reveal that nanofeatures can be selectively sculpted onto the shell exterior, within the shell wall, and on the interior surface. The versatility of this mechanism is validated by systematically arranging nanoparticles with various compositions, shapes, and dimensions. Spatially integrated nanotitania endows the core–shell structures with localized photocatalytic abilities. Additionally, distinctive surface modifications enable the simultaneous yet independent implantation of diverse nanoparticles, yielding intricate architectures with programmable functions. This generalizable approach showcases a synthetic strategy to attain structural complexity and functional sophistication reminiscent of those of biological systems in nature.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"98 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Biofluid-Permeable and Erosion-Resistant Wireless Neural-Electronic Interfaces for Neurohomeostasis Modulation
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acsnano.4c14320
Zhidong Wei, Fei Jin, Tong Li, Yuyuan He, Lili Qian, Juan Ma, Tao Yuan, Xin Yu, Weiying Zheng, Negar Javanmardi, Esteban Pena-Pitrach, Ting Wang, Jianda Xu, Zhang-Qi Feng
Neural-electronic interfaces through delivering electroceuticals to lesions and modulating pathological endogenous electrical environments offer exciting opportunities to treat drug-refractory neurological disorders. Such an interface should ideally be compatible with the neural tissue and aggressive biofluid environment. Unfortunately, no interface specifically designed for the biofluid environments is available so far; instead, simply stacking an encapsulation layer on silicon-based substrates makes them susceptible to biofluid leakage, device malfunction, and foreign-body reactions. Here, we developed a biofluid-permeable and erosion-resistant wireless neural-electronic interface (BNEI) that is composed of a flexible 3D interconnected poly(l-lactide) fibrous network with a dense and axially aligned piezoelectrical molecular chain arrangement architecture. The organized molecular chain structure enhances the tortuous pathway and longitudinal piezoelectric coefficient of poly(l-lactide) fibers, improves their water barrier properties, and enables efficient conversion of low-intensity acoustic vibrations transmitted in biofluids into electrical signals, achieving long-term stable and wireless neuromodulation. A 3-month clinical trial demonstrated that the BNEI can effectively accelerate the pathological cascade in peripheral neuropathy for nerve regeneration and transcranially modulate cerebellar–cerebral circuit dynamics, suppressing seizures in temporal lobe epilepsy. The BNEI can be a clinically scalable approach for wireless neuromodulation that is broadly applicable to the modulation of neurohomeostasis in both the peripheral and central nervous systems.
{"title":"Biofluid-Permeable and Erosion-Resistant Wireless Neural-Electronic Interfaces for Neurohomeostasis Modulation","authors":"Zhidong Wei, Fei Jin, Tong Li, Yuyuan He, Lili Qian, Juan Ma, Tao Yuan, Xin Yu, Weiying Zheng, Negar Javanmardi, Esteban Pena-Pitrach, Ting Wang, Jianda Xu, Zhang-Qi Feng","doi":"10.1021/acsnano.4c14320","DOIUrl":"https://doi.org/10.1021/acsnano.4c14320","url":null,"abstract":"Neural-electronic interfaces through delivering electroceuticals to lesions and modulating pathological endogenous electrical environments offer exciting opportunities to treat drug-refractory neurological disorders. Such an interface should ideally be compatible with the neural tissue and aggressive biofluid environment. Unfortunately, no interface specifically designed for the biofluid environments is available so far; instead, simply stacking an encapsulation layer on silicon-based substrates makes them susceptible to biofluid leakage, device malfunction, and foreign-body reactions. Here, we developed a biofluid-permeable and erosion-resistant wireless neural-electronic interface (BNEI) that is composed of a flexible 3D interconnected poly(<span>l</span>-lactide) fibrous network with a dense and axially aligned piezoelectrical molecular chain arrangement architecture. The organized molecular chain structure enhances the tortuous pathway and longitudinal piezoelectric coefficient of poly(<span>l</span>-lactide) fibers, improves their water barrier properties, and enables efficient conversion of low-intensity acoustic vibrations transmitted in biofluids into electrical signals, achieving long-term stable and wireless neuromodulation. A 3-month clinical trial demonstrated that the BNEI can effectively accelerate the pathological cascade in peripheral neuropathy for nerve regeneration and transcranially modulate cerebellar–cerebral circuit dynamics, suppressing seizures in temporal lobe epilepsy. The BNEI can be a clinically scalable approach for wireless neuromodulation that is broadly applicable to the modulation of neurohomeostasis in both the peripheral and central nervous systems.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"23 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988319","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
PEGylated Ultrasmall Iron Oxide Nanoparticles as MRI Contrast Agents for Vascular Imaging and Real-Time Monitoring
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acsnano.4c13356
Kuan Lu, Ruru Zhang, Hongzhao Wang, Cang Li, Zhe Yang, Keyang Xu, Xiaoyi Cao, Ning Wang, Wu Cai, Jianfeng Zeng, Mingyuan Gao
Accurate imaging evaluations of pre- and post-treatment of cardiovascular diseases are pivotal for effective clinical interventions and improved patient outcomes. However, current imaging methods lack real-time monitoring capabilities with a high contrast and resolution during treatments. This study introduces PEGylated ultrasmall iron oxide nanoparticles (PUSIONPs), which have undergone comprehensive safety evaluations, boasting an r1 value of 6.31 mM–1 s–1, for contrast-enhanced magnetic resonance angiography (MRA). Systematic comparisons against common clinical methods in rabbits reveal that PUSIONPs-enhanced MRA exhibited improved vascular contrast, clearer vascular boundaries, and superior vessel resolution. Moreover, owing to their nanosize, PUSIONPs demonstrate significantly prolonged blood circulation compared to small molecular contrast agents such as Magnevist and Ultravist. This extended circulation enables captivating real-time monitoring of thrombolysis treatment for up to 4 h in rabbit models postsingle contrast agent injection. Additionally, in larger animal models such as beagles and Bama minipigs, PUSIONPs-enhanced MRA also showcases superior contrast effects, boundary delineation, and microvessel visualization, underscoring their potential to transform cardiovascular imaging, particularly in real-time monitoring and high-resolution visualization during treatment processes.
{"title":"PEGylated Ultrasmall Iron Oxide Nanoparticles as MRI Contrast Agents for Vascular Imaging and Real-Time Monitoring","authors":"Kuan Lu, Ruru Zhang, Hongzhao Wang, Cang Li, Zhe Yang, Keyang Xu, Xiaoyi Cao, Ning Wang, Wu Cai, Jianfeng Zeng, Mingyuan Gao","doi":"10.1021/acsnano.4c13356","DOIUrl":"https://doi.org/10.1021/acsnano.4c13356","url":null,"abstract":"Accurate imaging evaluations of pre- and post-treatment of cardiovascular diseases are pivotal for effective clinical interventions and improved patient outcomes. However, current imaging methods lack real-time monitoring capabilities with a high contrast and resolution during treatments. This study introduces PEGylated ultrasmall iron oxide nanoparticles (PUSIONPs), which have undergone comprehensive safety evaluations, boasting an <i>r</i><sub>1</sub> value of 6.31 mM<sup>–1</sup> s<sup>–1</sup>, for contrast-enhanced magnetic resonance angiography (MRA). Systematic comparisons against common clinical methods in rabbits reveal that PUSIONPs-enhanced MRA exhibited improved vascular contrast, clearer vascular boundaries, and superior vessel resolution. Moreover, owing to their nanosize, PUSIONPs demonstrate significantly prolonged blood circulation compared to small molecular contrast agents such as Magnevist and Ultravist. This extended circulation enables captivating real-time monitoring of thrombolysis treatment for up to 4 h in rabbit models postsingle contrast agent injection. Additionally, in larger animal models such as beagles and Bama minipigs, PUSIONPs-enhanced MRA also showcases superior contrast effects, boundary delineation, and microvessel visualization, underscoring their potential to transform cardiovascular imaging, particularly in real-time monitoring and high-resolution visualization during treatment processes.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"27 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988169","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Targeted Modulation of the Meningeal Lymphatic Reverse Pathway for Immunotherapy of Breast Cancer Brain Metastases
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-17 DOI: 10.1021/acsnano.4c15860
Yanfeng Dai, Xiang Yu, Yifan Zhao, Jianshuang Wei, Dong Lin, Jialu Wang, Ren Zhang, Xuenan Yuan, Sanmu Li, Songlin Huang, Qian Liu, Zhihong Zhang
Treatment of tumor brain metastases remains challenging due to the ineffectiveness of drugs in crossing the blood–brain barrier (BBB). Here, we proposed a potential strategy to target and modulate the meningeal lymphatic system for immunotherapy of breast cancer brain metastases (BCBM) through peripheral administration. CT/fluorescence dual-modality imaging demonstrated that the phospholipid nanoprobe (α-PLNPs) through intracisternal magna injection effectively labeled and long-range tracked the meningeal lymphatic pathway from meningeal lymphatic vessels (MLVs) to periphery drainage cervical lymph nodes (CLNs). Interestingly, the reverse pathway from CLNs to MLVs was also successfully labeled with α-PLNPs through cervical subcutaneous injection, facilitating the noninvasive delivery of immunomodulators to the meningeal lymphatics. Given this, we used melittin-carrying α-M-PLNPs to trigger the modulation of the meningeal lymphatic reverse pathway, which effectively prevents BCBM and prolongs the survival of mice through activating the antigen-presenting cells in the CLNs and promoting the migration of CD8+ T cells into the metastatic brain tumors. This study highlights the potential of the meningeal lymphatic reverse pathway for the immunotherapy of BCBM, which holds great promise for central nervous system disease therapy without the need for drug delivery via BBB.
{"title":"Targeted Modulation of the Meningeal Lymphatic Reverse Pathway for Immunotherapy of Breast Cancer Brain Metastases","authors":"Yanfeng Dai, Xiang Yu, Yifan Zhao, Jianshuang Wei, Dong Lin, Jialu Wang, Ren Zhang, Xuenan Yuan, Sanmu Li, Songlin Huang, Qian Liu, Zhihong Zhang","doi":"10.1021/acsnano.4c15860","DOIUrl":"https://doi.org/10.1021/acsnano.4c15860","url":null,"abstract":"Treatment of tumor brain metastases remains challenging due to the ineffectiveness of drugs in crossing the blood–brain barrier (BBB). Here, we proposed a potential strategy to target and modulate the meningeal lymphatic system for immunotherapy of breast cancer brain metastases (BCBM) through peripheral administration. CT/fluorescence dual-modality imaging demonstrated that the phospholipid nanoprobe (α-PLNPs) through intracisternal magna injection effectively labeled and long-range tracked the meningeal lymphatic pathway from meningeal lymphatic vessels (MLVs) to periphery drainage cervical lymph nodes (CLNs). Interestingly, the reverse pathway from CLNs to MLVs was also successfully labeled with α-PLNPs through cervical subcutaneous injection, facilitating the noninvasive delivery of immunomodulators to the meningeal lymphatics. Given this, we used melittin-carrying α-M-PLNPs to trigger the modulation of the meningeal lymphatic reverse pathway, which effectively prevents BCBM and prolongs the survival of mice through activating the antigen-presenting cells in the CLNs and promoting the migration of CD8<sup>+</sup> T cells into the metastatic brain tumors. This study highlights the potential of the meningeal lymphatic reverse pathway for the immunotherapy of BCBM, which holds great promise for central nervous system disease therapy without the need for drug delivery via BBB.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"69 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Molecular Determinants of Optical Modulation in ssDNA–Carbon Nanotube Biosensors
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acsnano.4c13814
Andrew T. Krasley, Sayantani Chakraborty, Lela Vuković, Abraham G. Beyene
Most traditional optical biosensors operate through molecular recognition, where ligand binding causes conformational changes that lead to optical perturbations in the emitting motif. Optical sensors developed from single-stranded DNA-functionalized single-walled carbon nanotubes (ssDNA–SWCNTs) have started to make useful contributions to biological research. However, the mechanisms underlying their function have remained poorly understood. In this study, we combine experimental and computational approaches to show that ligand binding alone is not sufficient for optical modulation in this class of synthetic biosensors. Instead, the optical response that occurs after ligand binding is highly dependent on the chemical properties of the ligands, resembling mechanisms seen in activity-based biosensors. Specifically, we show that in ssDNA–SWCNT catecholamine sensors, the optical response correlates positively with the electron density on the aryl motif, even among ligands with similar ligand binding affinities. Importantly, despite the strong correlations with electrochemical properties, we find that catechol oxidation itself is not necessary to drive the sensor optical response. We discuss how these findings could serve as a framework for tuning the performance of existing sensors and guiding the development of new biosensors of this class.
{"title":"Molecular Determinants of Optical Modulation in ssDNA–Carbon Nanotube Biosensors","authors":"Andrew T. Krasley, Sayantani Chakraborty, Lela Vuković, Abraham G. Beyene","doi":"10.1021/acsnano.4c13814","DOIUrl":"https://doi.org/10.1021/acsnano.4c13814","url":null,"abstract":"Most traditional optical biosensors operate through molecular recognition, where ligand binding causes conformational changes that lead to optical perturbations in the emitting motif. Optical sensors developed from single-stranded DNA-functionalized single-walled carbon nanotubes (ssDNA–SWCNTs) have started to make useful contributions to biological research. However, the mechanisms underlying their function have remained poorly understood. In this study, we combine experimental and computational approaches to show that ligand binding alone is not sufficient for optical modulation in this class of synthetic biosensors. Instead, the optical response that occurs after ligand binding is highly dependent on the chemical properties of the ligands, resembling mechanisms seen in activity-based biosensors. Specifically, we show that in ssDNA–SWCNT catecholamine sensors, the optical response correlates positively with the electron density on the aryl motif, even among ligands with similar ligand binding affinities. Importantly, despite the strong correlations with electrochemical properties, we find that catechol oxidation itself is not necessary to drive the sensor optical response. We discuss how these findings could serve as a framework for tuning the performance of existing sensors and guiding the development of new biosensors of this class.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"37 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Framework Nucleic Acid-Based and Neutrophil-Based Nanoplatform Loading Baicalin with Targeted Drug Delivery for Anti-Inflammation Treatment
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acsnano.4c12917
Mi Zhou, Yuanlin Tang, Yifei Lu, Tianxu Zhang, Shunhao Zhang, Xiaoxiao Cai, Yunfeng Lin
Targeted drug delivery is a promising strategy for treating inflammatory diseases, with recent research focusing on the combination of neutrophils and nanomaterials. In this study, a targeted nanodrug delivery platform (Ac-PGP-tFNA, APT) was developed using tetrahedral framework nucleic acid (tFNA) along with a neutrophil hitchhiking mechanism to achieve precise delivery and anti-inflammatory effects. The tFNA structure, known for its excellent drug-loading capacity and cellular uptake efficiency, was used to carry a therapeutic agent─baicalin. The results demonstrate that the development of this drug delivery platform not only considerably enhances the bioavailability and effective concentration of the drug (baicalin) but also promotes the polarization of pro-inflammatory M1 macrophages to anti-inflammatory M2 macrophages by modulating the interactions between the neutrophils and macrophages. This targeted therapeutic method effectively treats inflammatory conditions such as sepsis and introduces a strategy for managing inflammatory diseases characterized by neutrophil infiltration.
{"title":"Framework Nucleic Acid-Based and Neutrophil-Based Nanoplatform Loading Baicalin with Targeted Drug Delivery for Anti-Inflammation Treatment","authors":"Mi Zhou, Yuanlin Tang, Yifei Lu, Tianxu Zhang, Shunhao Zhang, Xiaoxiao Cai, Yunfeng Lin","doi":"10.1021/acsnano.4c12917","DOIUrl":"https://doi.org/10.1021/acsnano.4c12917","url":null,"abstract":"Targeted drug delivery is a promising strategy for treating inflammatory diseases, with recent research focusing on the combination of neutrophils and nanomaterials. In this study, a targeted nanodrug delivery platform (Ac-PGP-tFNA, APT) was developed using tetrahedral framework nucleic acid (tFNA) along with a neutrophil hitchhiking mechanism to achieve precise delivery and anti-inflammatory effects. The tFNA structure, known for its excellent drug-loading capacity and cellular uptake efficiency, was used to carry a therapeutic agent─baicalin. The results demonstrate that the development of this drug delivery platform not only considerably enhances the bioavailability and effective concentration of the drug (baicalin) but also promotes the polarization of pro-inflammatory M1 macrophages to anti-inflammatory M2 macrophages by modulating the interactions between the neutrophils and macrophages. This targeted therapeutic method effectively treats inflammatory conditions such as sepsis and introduces a strategy for managing inflammatory diseases characterized by neutrophil infiltration.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"29 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Low-Frequency Resistance Noise in Near-Magic-Angle Twisted Bilayer Graphene
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acsnano.4c11141
Pritam Pal, Saisab Bhowmik, Aparna Parappurath, Saloni Kakkar, Kenji Watanabe, Takashi Taniguchi, Arindam Ghosh
The low-frequency resistance fluctuations, or noise, in electrical resistance not only set a performance benchmark in devices but also form a sensitive tool to probe nontrivial electronic phases and band structures in solids. Here, we report the measurement of such noise in the electrical resistance in twisted bilayer graphene (tBLG), where the layers are misoriented close to the magic angle (θ ∼ 1°). At high temperatures (T ≳ 60–70 K), the power spectral density (PSD) of the fluctuation inside the low-energy moiré bands is predominantly ∝1/f, where f is the frequency, being generally lowest close to the magic angle, and can be well-explained within the conventional McWhorter model of the ‘1/f noise’ with trap-assisted density-mobility fluctuations. At low T (≲10 K), the measured noise exhibits a strong two-level random telegraphic signal (RTS), especially close to the moiré gap, which exhibits a ∝1/f2-like PSD that can be attributed to poorly screened resonances of the Fermi energy to specific bands of defects in the encapsulating boron nitride (hBN) layers. The low-T noise within the moiré band exhibits a series of minima at the integral as well as half-integral fillings, which align with the frequently observed van Hove singularities in the density-of-states driven by strong Coulomb interaction. Apart from providing a comprehensive account of the origin and the magnitude of noise in tBLG, our experiment also reveals noise to be significantly more sensitive to the underlying interaction effects in tBLG than the conventional time-averaged transport.
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引用次数: 0
MXene Hollow Microsphere-Boosted Nanocomposite Electrodes for Thermocells with Enhanced Thermal Energy Harvesting Capability
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2025-01-16 DOI: 10.1021/acsnano.4c12294
Zhaopeng Liu, Dianlun Wu, Shouhao Wei, Kangqian Xing, Meilin Li, Yue Jiang, Rongfeng Yuan, Guangming Chen, Zhe Hu, Yang Huang, Zhuoxin Liu
Thermal energy, constantly being produced in natural and industrial processes, constitutes a significant portion of energy lost through various inefficiencies. Employing the thermogalvanic effect, thermocells (TECs) can directly convert thermal energy into electricity, representing a promising energy-conversion technology for efficient, low-grade heat harvesting. However, the use of high-cost platinum electrodes in TECs has severely limited their widespread adoption, highlighting the need for more cost-effective alternatives that maintain comparable thermoelectrochemical performance. In this study, a nanocomposite electrode featuring Ti3C2Tx with hollow microsphere structures is rationally designed. This design addresses the restacking issue inherent in MXene nanosheets, increases the electrochemically active surface area, and modifies the original MXene surfaces with oxygen terminations, leading to improved redox kinetics at the electrode–electrolyte interface, particularly in n-type TECs employing Fe2+/3+ redox ions. The optimized n-type TEC achieved an output power of 84.55 μW cm–2 and a normalized power density of 0.53 mW m–2 K–2 under a ΔT of 40 K, outperforming noble platinum-based TECs by a factor of 5.5. An integrated device consisting of 32 TEC units with a p–n connection is also fabricated, which can be successfully utilized to power various small electronics. These results demonstrate the potential of MXene-based composite electrodes to revolutionize TEC technology by offering a cost-effective, high-performance alternative to traditional noble metal electrodes and contributing to efficient low-grade heat harvesting.
{"title":"MXene Hollow Microsphere-Boosted Nanocomposite Electrodes for Thermocells with Enhanced Thermal Energy Harvesting Capability","authors":"Zhaopeng Liu, Dianlun Wu, Shouhao Wei, Kangqian Xing, Meilin Li, Yue Jiang, Rongfeng Yuan, Guangming Chen, Zhe Hu, Yang Huang, Zhuoxin Liu","doi":"10.1021/acsnano.4c12294","DOIUrl":"https://doi.org/10.1021/acsnano.4c12294","url":null,"abstract":"Thermal energy, constantly being produced in natural and industrial processes, constitutes a significant portion of energy lost through various inefficiencies. Employing the thermogalvanic effect, thermocells (TECs) can directly convert thermal energy into electricity, representing a promising energy-conversion technology for efficient, low-grade heat harvesting. However, the use of high-cost platinum electrodes in TECs has severely limited their widespread adoption, highlighting the need for more cost-effective alternatives that maintain comparable thermoelectrochemical performance. In this study, a nanocomposite electrode featuring Ti<sub>3</sub>C<sub>2</sub>T<sub><i>x</i></sub> with hollow microsphere structures is rationally designed. This design addresses the restacking issue inherent in MXene nanosheets, increases the electrochemically active surface area, and modifies the original MXene surfaces with oxygen terminations, leading to improved redox kinetics at the electrode–electrolyte interface, particularly in n-type TECs employing Fe<sup>2+/3+</sup> redox ions. The optimized n-type TEC achieved an output power of 84.55 μW cm<sup>–2</sup> and a normalized power density of 0.53 mW m<sup>–2</sup> K<sup>–2</sup> under a Δ<i>T</i> of 40 K, outperforming noble platinum-based TECs by a factor of 5.5. An integrated device consisting of 32 TEC units with a p–n connection is also fabricated, which can be successfully utilized to power various small electronics. These results demonstrate the potential of MXene-based composite electrodes to revolutionize TEC technology by offering a cost-effective, high-performance alternative to traditional noble metal electrodes and contributing to efficient low-grade heat harvesting.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"49 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-01-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142988173","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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ACS Nano
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