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Boosting Cancer Cell Uptake of Gold Nanoparticles by Light-Modulated Protein Corona Reorganization for Tumor Ablation
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-02 DOI: 10.1021/acsnano.5c01696
Lin Yang, Shenqing Wang, Chaofan Deng, Jie Chen, Jian Zhao, Bing Yan, Tongtao Yue
{"title":"Boosting Cancer Cell Uptake of Gold Nanoparticles by Light-Modulated Protein Corona Reorganization for Tumor Ablation","authors":"Lin Yang, Shenqing Wang, Chaofan Deng, Jie Chen, Jian Zhao, Bing Yan, Tongtao Yue","doi":"10.1021/acsnano.5c01696","DOIUrl":"https://doi.org/10.1021/acsnano.5c01696","url":null,"abstract":"Nanoparticles (NPs) administered into the human body are spontaneously modified by forming a protein corona, which is crucial for their biological activity. While NP-based photothermal therapy is an established noninvasive modality for tumor ablation, the impact of light irradiation on protein corona formation and clinical outcomes is unclear. This study unveils the promotive role of light irradiation in cancer cell uptake of gold nanoparticles (GNPs) by modulating the GNP–protein and protein–protein interactions within the corona. Specifically, infrared light irradiation increases the local temperature around GNPs to induce partial unfolding of corona proteins, increasing the availability of binding sites and enhancing adsorption. Additionally, light intensifies competition among different proteins for adsorption, resulting in a 25% increase in the abundance of higher molecular weight proteins, such as human serum albumin (HSA), on the GNP surface after irradiation. Notably, GNPs with positively charged surfaces, compared to GNPs with other modifications, exhibit more significant changes in the protein corona due to stronger electrostatic interactions with proteins (1.32 ± 0.17 × 10<sup>3</sup> kJ/mol). These variations in the amount, structure, and composition of associated proteins result in a 14.26% increase in GNP uptake by cancer cells, likely due to modifications at the GNP–cell membrane interface. Our findings highlight the critical role of light irradiation in influencing protein corona dynamics and cellular interactions, suggesting its potential as a valuable engineering tool in nanomedicine.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"6 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143767022","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
Magnetoresponsive Cellulose Nanofiber Hydrogels: Dynamic Structuring, Selective Light Transmission, and Information Encoding 磁致伸缩纤维素纳米纤维水凝胶:动态结构、选择性透光和信息编码
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-02 DOI: 10.1021/acsnano.4c18542
Junhua Xu, Yujun Zou, Huangjingyi Chen, Zhangmin Wan, Ayako Takagi, Zhiguo Wang, Juan Yu, Liang Liu, Yi Lu, Yimin Fan, Orlando J. Rojas
{"title":"Magnetoresponsive Cellulose Nanofiber Hydrogels: Dynamic Structuring, Selective Light Transmission, and Information Encoding","authors":"Junhua Xu, Yujun Zou, Huangjingyi Chen, Zhangmin Wan, Ayako Takagi, Zhiguo Wang, Juan Yu, Liang Liu, Yi Lu, Yimin Fan, Orlando J. Rojas","doi":"10.1021/acsnano.4c18542","DOIUrl":"https://doi.org/10.1021/acsnano.4c18542","url":null,"abstract":"Angle-dependent light reflection is a common phenomenon in nature, typically arising from the spatial arrangement of biological or mineral structures. Various strategies have been developed to replicate these assemblies, particularly to achieve structural color through bottom-up self- and directed assembly. However, dynamic control of light reflection remains a significant challenge. In this study, we present TEMPO-oxidized cellulose nanofibers modified with magnetic nanoparticles (approximately 10 nm in size) that exhibit rapid, directional alignment in aqueous media under magnetic fields, resulting in angle-dependent light reflection. By combining magnetic field manipulation with gas-phase hydrogelation, we were able to arrest the hydrogel structure, preserving the nanofibers’ spatial and temporal orientation. This system enables the creation of on-demand optical patterns, which we demonstrate through selective light transmission and reflection, offering potential for applications in information coding, storage, and encryption.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"23 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766581","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
Emerging Issues and Opportunities of 2D Layered Transition Metal Dichalcogenide Architectures for Supercapacitors
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-02 DOI: 10.1021/acsnano.5c01512
Shude Liu, Huilin Zhang, Xue Peng, Jieming Chen, Ling Kang, Xia Yin, Yamauchi Yusuke, Bin Ding
{"title":"Emerging Issues and Opportunities of 2D Layered Transition Metal Dichalcogenide Architectures for Supercapacitors","authors":"Shude Liu, Huilin Zhang, Xue Peng, Jieming Chen, Ling Kang, Xia Yin, Yamauchi Yusuke, Bin Ding","doi":"10.1021/acsnano.5c01512","DOIUrl":"https://doi.org/10.1021/acsnano.5c01512","url":null,"abstract":"Two-dimensional layered transition metal dichalcogenides (2D TMDs) have emerged as promising candidates for supercapacitor (SCs) owing to their tunable electronic properties, layered structures, and effective ion intercalation capabilities. Despite these advantages, challenges such as low electrical conductivity, the interlayer restacking, oxidation and structural collapse hinder their practical implementation. This review provides a comprehensive overview of recent advances in the development of 2D TMDs for SCs. We begin by outlining the charge storage mechanisms and design principles for SCs, followed by an in-depth discussion of the synthesis methods and the associated challenges in fabricating 2D TMD architectures. The subsequent sections explore their crystal structures and reaction mechanisms, illustrating their electrochemical potential in SCs. Furthermore, we highlight material modification strategies, including nanostructuring, defect engineering, phase control, and surface/interface modulation, which have been proposed to overcome existing challenges. Finally, we address critical issues and emerging opportunities for 2D TMDs to inspire the development of SC technologies.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"32 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766614","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
Insights into Dendrite Regulation by Polymer Hydrogels for Aqueous Batteries
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.5c00354
Jinglin Xian, Rui Fu, Kang Liu, Peihua Yang
{"title":"Insights into Dendrite Regulation by Polymer Hydrogels for Aqueous Batteries","authors":"Jinglin Xian, Rui Fu, Kang Liu, Peihua Yang","doi":"10.1021/acsnano.5c00354","DOIUrl":"https://doi.org/10.1021/acsnano.5c00354","url":null,"abstract":"Aqueous batteries, renowned for their high capacity, safety, and low cost, have emerged as promising candidates for next-generation, sustainable energy storage. However, their large-scale application is hindered by challenges, such as dendrite formation and side reactions at the anode. Hydrogel electrolytes, which integrate the advantages of liquid and solid phases, exhibit superior ionic conductivity and interfacial compatibility, giving them potential to suppress dendrite evolution. This Perspective first briefly introduces the fundamentals underlying dendrite formation and the unique features of hydrogels. It then identifies the key role of water and polymer networks in inhibiting dendrite formation, highlighting their regulation of water activity, ion transport, and electrode kinetics. By elucidating the principles of hydrogels in dendrite suppression, this work aims to provide valuable insights to advance the implementation of aqueous batteries incorporating polymer hydrogels.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"50 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758542","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
Room-Temperature Efficient Single-Photon Generation from CdSe/ZnS Nanoplatelets
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.5c01971
Marianna D’Amato, Ningyuan Fu, Quentin Glorieux, Elisabeth Giacobino, Hanna Le Jeannic, Sandrine Ithurria, Emmanuel Lhuillier, Alberto Bramati
{"title":"Room-Temperature Efficient Single-Photon Generation from CdSe/ZnS Nanoplatelets","authors":"Marianna D’Amato, Ningyuan Fu, Quentin Glorieux, Elisabeth Giacobino, Hanna Le Jeannic, Sandrine Ithurria, Emmanuel Lhuillier, Alberto Bramati","doi":"10.1021/acsnano.5c01971","DOIUrl":"https://doi.org/10.1021/acsnano.5c01971","url":null,"abstract":"In the search for materials for quantum information science applications, colloidal semiconductor nanoplatelets (NPLs) have emerged as a highly promising class of materials due to their interesting optical properties, such as narrow emission line widths and fast photoluminescence (PL) lifetimes at room temperature. So far, only a few works focused on the quantum properties of their emission; however, NPLs, with their atomic-scale thickness and one-dimensional quantum confinement, are promising candidates for single-photon sources. Here, we demonstrate room-temperature single-photon emission from core/shell CdSe/ZnS NPLs, which feature an 8 × 20 nm<sup>2</sup> surface area and 1 nm shell. The limited surface area ensures effective Auger nonradiative recombination, resulting in highly efficient single-photon generation with values of photon purity as low as <i>g</i><sup>(2)</sup>(0) = 0.04. The observed long-period blinking and bleaching typical of such thin shells can be easily reduced by increasing the shell thickness. This work establishes NPLs as single-photon sources that are very well suited for integration into quantum photonic systems.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"37 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758543","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
Actuation and Mapping of Surface Acoustic Wave Induced High-Frequency Wavefields on Suspended Graphene Membranes
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.4c18508
Hande N. Açıkgöz, Dong Hoon Shin, Inge C. van der Knijff, Allard J. Katan, Xiliang Yang, Peter G. Steeneken, Gerard J. Verbiest, Sabina Caneva
{"title":"Actuation and Mapping of Surface Acoustic Wave Induced High-Frequency Wavefields on Suspended Graphene Membranes","authors":"Hande N. Açıkgöz, Dong Hoon Shin, Inge C. van der Knijff, Allard J. Katan, Xiliang Yang, Peter G. Steeneken, Gerard J. Verbiest, Sabina Caneva","doi":"10.1021/acsnano.4c18508","DOIUrl":"https://doi.org/10.1021/acsnano.4c18508","url":null,"abstract":"High-frequency acoustic devices based on two-dimensional (2D) materials are emerging platforms to design and manipulate the spatiotemporal response of acoustic waves for next-generation sensing and contactless actuation applications. Conventional actuation methods, however, cannot be applied to all 2D materials, are frequency-limited or influenced by substrate interactions. Therefore, a universal, high-frequency, on-chip actuation technique is needed. Here, we demonstrate that surface acoustic waves (SAWs) can efficiently actuate suspended 2D materials by exciting suspended graphene membranes with high-frequency (375 MHz) Rayleigh waves and mapping the resulting vibration field with atomic force acoustic microscopy (AFAM), enabling direct visualization of wave propagation without substrate interference. Acoustic waves traveling from supported to suspended graphene experience a reduction in acoustic wavelength from 10 μm to ∼2 μm due to the decrease in effective bending rigidity, leading to a decrease in wave velocity on suspended graphene. By varying the excitation frequency through laser photothermal actuation (0–100 MHz) and SAW excitation (375 MHz), we observed a phase velocity change from ∼160 m/s to ∼700 m/s. This behavior is consistent with the nonlinear dispersion of acoustic waves, as predicted by plate theory, in suspended graphene membranes. The geometry and bending rigidity of the membrane thus play key roles in modulating the acoustic wave pattern and wavelength. This combined SAW actuation and AFAM visualization scheme advances the understanding of acoustic transport at the nanoscale limit and provides a route toward the manipulation of localized wavefields for on-chip patterning and transport over 2D materials surfaces.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"12 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745260","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
Spatial Regulation of Cancer-Associated Fibroblasts and Tumor Cells via pH-Responsive Bispecific Antibody Delivery for Enhanced Chemo-Immunotherapy Synergy. 通过 pH 响应性双特异性抗体递送对癌症相关成纤维细胞和肿瘤细胞进行空间调控以增强化疗与免疫疗法的协同作用
IF 15.8 1区 材料科学
ACS Nano Pub Date : 2025-04-01 Epub Date: 2025-03-21 DOI: 10.1021/acsnano.4c13277
Haojie Liu, Tuying Yong, Xiaoqiong Zhang, Zhaohan Wei, Nana Bie, Shiyi Xu, Xiaojuan Zhang, Shiyu Li, Jing Zhang, Pengfei Zhou, Xiangliang Yang, Lu Gan
{"title":"Spatial Regulation of Cancer-Associated Fibroblasts and Tumor Cells via pH-Responsive Bispecific Antibody Delivery for Enhanced Chemo-Immunotherapy Synergy.","authors":"Haojie Liu, Tuying Yong, Xiaoqiong Zhang, Zhaohan Wei, Nana Bie, Shiyi Xu, Xiaojuan Zhang, Shiyu Li, Jing Zhang, Pengfei Zhou, Xiangliang Yang, Lu Gan","doi":"10.1021/acsnano.4c13277","DOIUrl":"10.1021/acsnano.4c13277","url":null,"abstract":"<p><p>The effectiveness of chemotherapy is often compromised by physiological barriers and an immunosuppressive tumor microenvironment. Cancer-associated fibroblasts (CAFs) significantly contribute to the reconfiguration of the tumor extracellular matrix (ECM) and the suppression of immune responses, making them crucial targets for therapeutic intervention. Here, a tumor acidic microenvironment-responsive delivery system that utilizes tumor cell-derived microparticles (MPs) as carriers for the chemotherapeutic agent doxorubicin (DOX) and the bispecific antibody YM101 targeting both TGF-β and PD-L1 is developed (DOX@MPs-YM101) to spatially regulate both CAFs and tumor cells for enhanced chemotherapeutic efficacy. DOX@MPs-YM101 efficiently targets tumor tissues and releases DOX@MPs and YM101 in response to the acidic tumor microenvironment. YM101 reprograms CAFs and reduces the tumor ECM, facilitating tumor accumulation and deep penetration of DOX@MPs-YM101. DOX@MPs are highly internalized into tumor cells, triggering immunogenic cell death (ICD) and activating CD8<sup>+</sup> T cell-mediated antitumor immunity. The reprogramming of CAFs by YM101 further promotes the accumulation of CD8<sup>+</sup> T cells and reduces the number of immunosuppressive cells within the tumors. Additionally, YM101 effectively neutralizes PD-L1 on tumor cells induced by DOX@MPs, restoring CD8<sup>+</sup> T cell activity and generating long-term antitumor immune memory to prevent tumor recurrence. Our findings highlight the potential of DOX@MPs-YM101 to improve chemotherapy in cancer treatment.</p>","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":" ","pages":"11756-11773"},"PeriodicalIF":15.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143668561","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
Room-Temperature Exciton-Polariton-Driven Self-Phase Modulation in Planar Perovskite Waveguides
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.4c18847
Nikita V. Glebov, Mikhail A. Masharin, Alexei Yulin, Alexey Mikhin, Md Rumon Miah, Hilmi Volkan Demir, Dmitry N. Krizhanovskii, Vasily Kravtsov, Anton K. Samusev, Sergey V. Makarov
{"title":"Room-Temperature Exciton-Polariton-Driven Self-Phase Modulation in Planar Perovskite Waveguides","authors":"Nikita V. Glebov, Mikhail A. Masharin, Alexei Yulin, Alexey Mikhin, Md Rumon Miah, Hilmi Volkan Demir, Dmitry N. Krizhanovskii, Vasily Kravtsov, Anton K. Samusev, Sergey V. Makarov","doi":"10.1021/acsnano.4c18847","DOIUrl":"https://doi.org/10.1021/acsnano.4c18847","url":null,"abstract":"Optical nonlinearities are crucial for advanced photonic technologies since they allow photons to be managed by photons. Exciton-polaritons resulting from strong light–matter coupling are hybrid in nature: they combine the small mass and high coherence of photons with strong nonlinearity enabled by excitons, making them ideal for ultrafast all-optical manipulations. Among the most prospective polaritonic materials are halide perovskites since they require neither cryogenic temperatures nor expensive fabrication techniques. Here, we study strikingly nonlinear self-action of ultrashort polaritonic pulses propagating in planar MAPbBr<sub>3</sub> perovskite slab waveguides. Tuning the input pulse energy and central frequency, we experimentally observe various scenarios of its nonlinear evolution in the spectral domain, which include peak shifts, narrowing, or splitting driven by self-phase modulation, group velocity dispersion, and self-steepening. The theoretical model provides complementary temporal traces of pulse propagation and reveals the transition from the birth of a doublet of optical solitons to the formation of a shock wave, both supported by the system. Our results presented here represent an important step in ultrafast nonlinear on-chip polaritonics in perovskite-based systems.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"15 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758626","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
A One-Component Patchy-Particle Icosahedral Quasicrystal 单组分斑状粒子二十面体准晶体
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.4c14885
Eva G. Noya, Jonathan P. K. Doye
{"title":"A One-Component Patchy-Particle Icosahedral Quasicrystal","authors":"Eva G. Noya, Jonathan P. K. Doye","doi":"10.1021/acsnano.4c14885","DOIUrl":"https://doi.org/10.1021/acsnano.4c14885","url":null,"abstract":"Designing particles that are able to form icosahedral quasicrystals (IQCs) and that are as simple as possible is not only of fundamental interest but is also important to the potential realization of IQCs in materials other than metallic alloys. Here we introduce one-component patchy-particle systems that in simulations are able to form face-centered IQCs that are made up of interconnected icosahedra. The directional bonding of the particles facilitates the formation of a network of bonds with icosahedral orientational order and hence quasiperiodic positional order. The assembled quasicrystals have similar energies to periodic approximants but are entropically stabilized by phason disorder. Their long-range quasiperiodic order is confirmed by a higher-dimensional analysis. These materials, which are predicted to have an almost spherical photonic band gap, can potentially be realized via protein design and DNA origami particles.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"38 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758623","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
tert-Butoxycarbonyl-Modification Driven Disturbance of Molecular Ordering Enables High-Efficiency Dual Drugs Co-Assembly for Synergistic Tumor Inhibition
IF 17.1 1区 材料科学
ACS Nano Pub Date : 2025-04-01 DOI: 10.1021/acsnano.4c16986
Xuequan Zhang, Xiaoxian Zhang, Jiahui Zhu, Tinghua Li, Lianyi Yang, Lei Lei, Fang Wu, Bin He, Jun Cao
{"title":"tert-Butoxycarbonyl-Modification Driven Disturbance of Molecular Ordering Enables High-Efficiency Dual Drugs Co-Assembly for Synergistic Tumor Inhibition","authors":"Xuequan Zhang, Xiaoxian Zhang, Jiahui Zhu, Tinghua Li, Lianyi Yang, Lei Lei, Fang Wu, Bin He, Jun Cao","doi":"10.1021/acsnano.4c16986","DOIUrl":"https://doi.org/10.1021/acsnano.4c16986","url":null,"abstract":"The development of carrier-free drug delivery systems (CDDS) for tailored drug combinations posed a significant challenge, particularly in achieving efficient co-assembly while maintaining therapeutic efficacy. Herein, we proposed a co-assembly strategy based on molecular engineering. Paclitaxel (PTX) and 7-ethyl-10-hydroxycamptothecin (SN38) were chemically modified with <i>tert</i>-butoxycarbonyl (BOC) groups. The successful incorporation of the BOC groups was confirmed by proton nuclear magnetic resonance and mass spectrometry analyses. Further characterization using polarized light microscopy and X-ray diffraction revealed that this modification significantly reduced the crystallinity of both drugs, while simultaneously disrupting their original ordered stacking structure. Molecular dynamics simulations indicated that BOC modification increased molecular spacing, reduced stacking density, and expanded molecular volume, resulting in a looser molecular packing arrangement. This structural alteration enabled the modified drug molecules to efficiently coassemble with α-tocopherol succinate (α-TOS) into spherical nanoparticles at a nearly predefined mass ratio. The resulting nanoparticles exhibited a high drug loading capacity of 52.66% and remained stable at 4 °C for over 50 days. Notably, these nanoparticles displayed controllable release characteristics at pH 5.0. Both <i>in vitro</i> and <i>in vivo</i> studies demonstrated the BOC-modified drugs retained their bioactivity. When co-assembled with α-TOS, the nanoparticles exhibited a significant synergistic antitumor effect and suppressed tumor metastasis through downregulation of matrix metalloproteinase-9 (MMP-9) expression. This study provided a solid theoretical foundation and innovative approach for the development of CDDS, utilizing molecular-scale regulation for drug co-assembly.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"3 1","pages":""},"PeriodicalIF":17.1,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758541","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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