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High-Fidelity Transfer of 2D Semiconductors and Electrodes for van der Waals Devices. 用于范德华器件的二维半导体和电极的高保真转移。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-18 DOI: 10.1021/acsnano.4c10551
Lingxiao Yu, Minglang Gao, Qian Lv, Hanyuan Ma, Jingzhi Shang, Zheng-Hong Huang, Zheng Sun, Ting Yu, Feiyu Kang, Ruitao Lv

As traditional silicon-based materials almost reach their limits in the post-Moore era, two-dimensional (2D) transition metal dichalcogenides (TMDCs) have been regarded as next-generation semiconductors for high-performance electrical and optical devices. Chemical vapor deposition (CVD) is a widely used technique for preparing large-area and high-quality TMDCs. Yet, it suffers from the challenge of transfer due to the strong interaction between 2D materials and substrates. The traditional PMMA-assisted wet etching method tends to induce damage, wrinkles, and inevitable polymer residues. In this work, we propose an etch-free and clean transfer method via a water intercalation strategy for TMDCs, ensuring a high-fidelity, wrinkle-free, and crack-free transfer with negligible residues. Furthermore, metal electrodes can also be transferred via this method and back-gate field-effect transistors (FETs) based on CVD-grown monolayer WSe2 with van der Waals (vdW) metal/semiconductor contacts are fabricated. Compared to the PMMA-assisted transfer method (∼1.2 cm2 V-1 s-1 hole mobility with ∼2 × 106 ON/OFF ratio), our high-fidelity transfer method significantly enhances the electrical performance of WSe2 FET over one order of magnitude, achieving a hole mobility of ∼43 cm2 V-1 s-1 and a high ON/OFF ratio of ∼5 × 107 in air at room temperature.

在后摩尔时代,传统的硅基材料几乎达到了极限,因此二维(2D)过渡金属二掺杂化合物(TMDCs)被视为下一代半导体材料,可用于高性能电气和光学设备。化学气相沉积(CVD)是制备大面积和高质量 TMDCs 的广泛应用技术。然而,由于二维材料与基底之间存在强烈的相互作用,它在转移方面面临挑战。传统的 PMMA 辅助湿法蚀刻往往会导致损伤、皱褶和不可避免的聚合物残留。在这项工作中,我们通过水插层策略为 TMDC 提出了一种免蚀刻和清洁的转移方法,确保了高保真、无皱纹和无裂纹的转移,残留物几乎可以忽略不计。此外,还可以通过这种方法转移金属电极,并制造出基于 CVD 生长的单层 WSe2 的背栅场效应晶体管 (FET),该晶体管具有范德华(vdW)金属/半导体触点。与 PMMA 辅助转移法(1.2 cm2 V-1 s-1 的空穴迁移率和 2 × 106 的导通/关断比)相比,我们的高保真转移法显著提高了 WSe2 场效应晶体管的电气性能一个数量级以上,在室温空气中实现了 43 cm2 V-1 s-1 的空穴迁移率和 5 × 107 的高导通/关断比。
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引用次数: 0
Low-Cost, Eco-Friendly, and High-Performance 3D Laser-Induced Graphene Evaporator for Continuous Solar-Powered Water Desalination. 用于连续太阳能海水淡化的低成本、环保、高性能三维激光诱导石墨烯蒸发器。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-18 DOI: 10.1021/acsnano.4c12553
Truong-Son Dinh Le, Dongwook Yang, Han Ku Nam, Younggeun Lee, Chwee Teck Lim, Bong Jae Lee, Seung-Woo Kim, Young-Jin Kim

Water scarcity has become a global challenge attributed to climate change, deforestation, population growth, and increasing water demand. While advanced water production plants are prevalent in urban areas, remote islands and sparsely populated regions face significant obstacles in establishing such technologies. Consequently, there is an urgent need for efficient, affordable, and sustainable water production technologies in these areas. Herein, we present a facile approach utilizing an ultrashort-pulsed laser to directly convert cotton fabric into graphene under ambient conditions. The resulting laser-induced graphene (LIG) demonstrates the highest light absorption efficiency of 99.0% and a broad absorption range (250-2500 nm). As an excellent solar absorber, LIG on cotton fabric can efficiently absorb 98.6% of the total solar irradiance and its surface temperature can reach 84.5 °C under sunlight without optical concentration. Moreover, we propose a cost-effective 3D LIG evaporator (LIGE) for continuous solar-powered desalination. This innovative design effectively mitigates salt formation issues and enhances the steam generation efficiency. The water evaporation rate and the solar-to-vapor conversion efficiency are measured to be around 1.709 kg m-2 h-1 and 95.1%, respectively, which surpass those reported in previous studies. The simplicity, durability, and continuous operational capability of the 3D LIGE offer promising prospects to address the growing challenges in global water scarcity.

由于气候变化、森林砍伐、人口增长和水资源需求增加,水资源短缺已成为全球性挑战。虽然先进的制水厂在城市地区很普遍,但偏远岛屿和人口稀少地区在建立此类技术方面却面临着巨大障碍。因此,这些地区迫切需要高效、经济、可持续的制水技术。在本文中,我们介绍了一种利用超短脉冲激光在环境条件下直接将棉织物转化为石墨烯的简便方法。由此产生的激光诱导石墨烯(LIG)具有最高的光吸收率(99.0%)和宽广的吸收范围(250-2500 nm)。作为一种优异的太阳能吸收剂,棉织物上的石墨烯可有效吸收 98.6% 的太阳总辐照度,其表面温度在阳光照射下可达到 84.5 °C,且无需光学浓缩。此外,我们还提出了一种经济高效的三维 LIG 蒸发器(LIGE),用于连续太阳能海水淡化。这一创新设计有效缓解了盐形成问题,并提高了蒸汽产生效率。经测量,水蒸发率和太阳能到水蒸气的转换效率分别约为 1.709 kg m-2 h-1 和 95.1%,超过了以往研究的结果。三维 LIGE 的简易性、耐用性和连续运行能力为应对全球水资源短缺日益严峻的挑战提供了广阔的前景。
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引用次数: 0
Correction to "Cobalt Ditelluride Meets Tellurium Vacancy: An Efficient Catalyst as a Multifunctional Polysulfide Mediator toward Robust Lithium-Sulfur Batteries". 更正 "二碲化钴与碲空位:一种作为多功能多硫化物媒介的高效催化剂,可用于制造稳健的锂硫电池"。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-18 DOI: 10.1021/acsnano.4c14667
Qianhong Gong, Dawei Yang, Huiping Yang, Konglin Wu, Jie Zhang, Wei Bi, Jiefeng Diao, Canhuang Li, Jing Yu, Chao Yue Zhang, Mengyao Li, Graeme Henkelman, Jordi Arbiol, Qiaobao Zhang, Andreu Cabot
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引用次数: 0
Violation of the Wiedemann-Franz Law and Ultralow Thermal Conductivity of Ti3C2Tx MXene. Ti3C2Tx MXene 违反维德曼-弗朗茨定律和超低导热性。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-17 DOI: 10.1021/acsnano.4c08189
Yubin Huang, Jean Spiece, Tetiana Parker, Asaph Lee, Yury Gogotsi, Pascal Gehring

The high electrical conductivity and good chemical stability of MXenes offer hopes for their use in many applications, such as wearable electronics, energy storage, and electromagnetic interference shielding. While their optical, electronic, and electrochemical properties have been widely studied, information on the thermal properties of MXenes is scarce. In this study, we investigate the heat transport properties of Ti3C2Tx MXene single flakes using scanning thermal microscopy and find exceptionally low anisotropic thermal conductivities within the Ti3C2Tx flakes, leading to an effective thermal conductivity of 0.78 ± 0.21 W m-1 K-1. This observation is in stark contrast to the predictions of the Wiedemann-Franz law, as the estimated Lorenz number is only 0.25 of the classical value. Due to the combination of low thermal conductivity and low emissivity of Ti3C2Tx, the heat loss from it is 2 orders of magnitude smaller than that from common metals. Our study explores the heat transport mechanisms of MXenes and highlights a promising approach for developing thermal insulation, two-dimensional thermoelectric, or infrared stealth materials.

二氧化二烯的高导电性和良好的化学稳定性为其在可穿戴电子设备、能量存储和电磁干扰屏蔽等许多应用领域的应用带来了希望。虽然人们对它们的光学、电子和电化学特性进行了广泛研究,但有关 MXenes 热特性的信息却很少。在本研究中,我们使用扫描热显微镜研究了 Ti3C2Tx MXene 单片的热传输特性,发现 Ti3C2Tx 片状材料内部的各向异性热传导率极低,有效热传导率为 0.78 ± 0.21 W m-1 K-1。这一观察结果与维德曼-弗兰茨定律的预测形成了鲜明对比,因为估计的洛伦兹数仅为经典值的 0.25。由于 Ti3C2Tx 兼具低热导率和低发射率的特点,其热量损失比普通金属小两个数量级。我们的研究探索了 MXenes 的热传输机制,为开发隔热材料、二维热电材料或红外隐形材料提供了一种前景广阔的方法。
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引用次数: 0
Realization of Z2 Topological Photonic Insulators Made from Multilayer Transition Metal Dichalcogenides. 实现由多层过渡金属二卤化物制成的 Z2 拓扑光子绝缘体。
IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-17 DOI: 10.1021/acsnano.4c09295
Tommi Isoniemi, Paul Bouteyre, Xuerong Hu, Fedor Benimetskiy, Yue Wang, Maurice S Skolnick, Dmitry N Krizhanovskii, Alexander I Tartakovskii

Monolayers of semiconducting transition metal dichalcogenides (TMDs) have long attracted interest for their intriguing optical and electronic properties. Recently, TMDs in their quasi-bulk form have started to show considerable promise for nanophotonics thanks to their high refractive indices, large optical anisotropy, wide transparency windows reaching to the visible, and robust room temperature excitons promising for nonlinear optics. Adherence of TMD layers to any substrate via van der Waals forces is a further key enabler for the nanofabrication of complex photonic structures requiring heterointegration. Here, we use the attractive properties of TMDs and realize topological spin-Hall photonic lattices made of arrays of triangular nanoholes in 50 to 100 nm thick WS2 flakes exfoliated on SiO2/Si substrates. High-quality structures are achieved by taking advantage of anisotropic dry etching dictated by the crystal axes of WS2. Reflectance measurements at room temperature show a photonic gap opening in the near-infrared in trivial and topological phases. Unidirectional propagation along the domain interface is demonstrated in real space via circularly polarized laser excitation in samples with both zigzag and armchair domain boundaries. Finite-difference time-domain simulations are used to interpret optical spectroscopy results. Our work demonstrates the feasibility of more complex nanophotonic devices based on the layered (van der Waals) materials platform.

长期以来,半导体过渡金属二掺杂化合物(TMDs)单层因其引人入胜的光学和电子特性而备受关注。最近,准块状 TMD 因其高折射率、大光学各向异性、可达可见光的宽透明度窗口以及有望用于非线性光学的强大室温激子,开始在纳米光子学领域大显身手。TMD 层通过范德华力附着在任何基底上,是纳米制造需要异质结合的复杂光子结构的另一个关键因素。在这里,我们利用 TMD 的诱人特性,在二氧化硅/硅衬底上剥离出的 50 至 100 纳米厚的 WS2 片中实现了由三角形纳米孔阵列组成的拓扑自旋-霍尔光子晶格。通过利用 WS2 晶体轴决定的各向异性干蚀刻,实现了高质量的结构。室温下的反射测量显示,三相和拓扑相的光子间隙在近红外区域打开。在具有人字形和扶手椅形畴边界的样品中,通过圆偏振激光激励,在实际空间中演示了沿畴界面的单向传播。有限差分时域模拟用于解释光学光谱结果。我们的工作证明了基于层状(范德华)材料平台的更复杂的纳米光子器件的可行性。
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引用次数: 0
Enhancing zT in Organic Thermoelectric Materials through Nanoscale Local Control Crystallization 通过纳米级局部控制结晶提高有机热电材料的 zT
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1021/acsnano.4c10801
Gabriele Calabrese, Raimondo Cecchini, Denis Gentili, Diego Marini, Matteo Ferri, Fulvio Mancarella, Luisa Barba, Massimiliano Cavallini, Vittorio Morandi, Fabiola Liscio
Organic thermoelectric materials are promising for wearable heating and cooling devices, as well as near-room-temperature energy generation, due to their nontoxicity, abundance, low cost, and flexibility. However, their primary challenge preventing widespread use is their reduced figure of merit (zT) caused by low electrical conductivity. This study presents a method to enhance the thermoelectric performance of solution-processable organic materials through confined crystallization using the lithographically controlled wetting (LCW) technique. Using PEDOT as a benchmark, we demonstrate that controlled crystallization at the nanoscale improves electrical conductivity by optimizing chain packing and grain morphology. Structural characterizations reveal the formation of a highly compact PEDOT arrangement, achieved through a combination of confined crystallization and DMSO post-treatment, leading to a 4-fold increase in the power factor compared to spin-coated films. This approach also reduces the thermal conductivity dependence on electrical conductivity, improving the zT by up to 260%. The LCW technique, compatible with large-area and flexible substrates, offers a simple, green, and low-cost method to boost the performance of organic thermoelectrics, advancing the potential for sustainable energy solutions and advanced organic electronic devices.
有机热电材料因其无毒性、丰富性、低成本和灵活性,在可穿戴加热和冷却设备以及近室温发电方面大有可为。然而,由于导电率低,它们的优点系数(zT)降低,这是阻碍其广泛应用的主要挑战。本研究介绍了一种利用光刻控制润湿(LCW)技术,通过限制结晶提高可溶液加工有机材料热电性能的方法。以 PEDOT 为基准,我们证明了纳米尺度的受控结晶可通过优化链包装和晶粒形态提高导电性。结构特性分析表明,通过限制结晶和 DMSO 后处理的结合,形成了高度紧凑的 PEDOT 排列,与旋涂薄膜相比,功率因数提高了 4 倍。这种方法还降低了热导率对电导率的依赖性,将 zT 提高了 260%。LCW 技术与大面积和柔性基底兼容,提供了一种简单、绿色和低成本的方法来提高有机热电的性能,推动了可持续能源解决方案和先进有机电子设备的发展潜力。
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引用次数: 0
Photonics of High-Entropy Polymers Revealing Molecular Dispersion via Polymer Mixing 通过聚合物混合揭示分子分散的高熵聚合物光子学
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1021/acsnano.4c10585
Yu-Jr Huang, Jien-Wei Yeh, Arnold Chang-Mou Yang
Blending multiple polymers together to form the so-called “high-entropy polymers (HEPs)” can generate the effects of molecular dispersion in addition to suppressing polymer phase separation. We embedded a semiconducting polymer (conjugated polymers, CPs) in an optically inert matrix composed of n polymer species and found that a molecule-level dispersion is attained in HEPs defined as n ≥ 5. In the regime of dilute CP concentrations, the photonic properties vary widely in the n = 1 matrices owing to diverse solubility parameters, but the distribution narrows with n, and the CP starts to exhibit behaviors of molecule-level dispersion at n ≥ 5, where the matrix polymers compete with each other to exert direct influences on the embedded CP. Specifically, for MEH-PPV, increasing n reduces the fluorescence redshift and spectral width from diminishing aggregation. For the rigid PFO molecules, increasing n creates a dilution effect facilitating formation of the low-energy planar β-phase. For the flexible regioregular P3HT-rr, HEPs offer well-dispersed amorphous chains highly susceptible to chain environments, thus influencing ηR’s in the quasi-fixed amorphous–crystalline energy transfer landscape. The HEP effects continue for greater CP concentrations, consistent with the matrix dispersing behaviors in the dilute regime. This work demonstrates a molecular-level dispersion by HEPs, offering a method of molecular tailoring for polymer research and applications via simple mixing.
将多种聚合物混合在一起形成所谓的 "高熵聚合物(HEPs)",除了能抑制聚合物相分离外,还能产生分子分散效果。我们将半导体聚合物(共轭聚合物)嵌入由 n 种聚合物组成的光学惰性基质中,发现在 n ≥ 5 的 HEPs 中可以实现分子级分散。在氯化石蜡浓度稀释的情况下,由于溶解度参数的不同,光子特性在 n = 1 的基质中差异很大,但随着 n 的增加,分布逐渐缩小,当 n ≥ 5 时,氯化石蜡开始表现出分子级分散的行为,此时基质聚合物相互竞争,对嵌入的氯化石蜡产生直接影响。具体来说,对于 MEH-PPV,n 的增大会因聚集的减弱而降低荧光红移和光谱宽度。对于刚性 PFO 分子,增加 n 会产生稀释效应,促进低能平面 β 相的形成。对于柔性团状 P3HT-rr,HEP 提供了分散良好的无定形链,极易受到链环境的影响,从而影响准固定无定形-晶体能量转移图中的ηR。CP 浓度越高,HEP 效应越强,这与稀释体系中的基质分散行为一致。这项工作证明了 HEP 在分子水平上的分散作用,为聚合物研究和应用提供了一种通过简单混合进行分子定制的方法。
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引用次数: 0
Shell-Isolated Nanoparticle-Enhanced Raman Spectroscopy: Toward High Sensitivity and Broad Applicability 壳隔离纳米粒子增强拉曼光谱:实现高灵敏度和广泛适用性
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-16 DOI: 10.1021/acsnano.4c07037
Yue-Zhou Zhu, Ru-Yu Zhou, Shu Hu, Jian-Feng Li, Zhong-Qun Tian
As a nondestructive and ultrasensitive technique, surface-enhanced Raman spectroscopy (SERS) has captivated the attention of the global scientific community for over 50 years. Among the various spectroscopic techniques derived from SERS, shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS) stands as a cutting-edge advancement. The innovative and versatile core–shell nanoparticle structures used in SHINERS have emerged as an ideal platform for interfacial research, offering high sensitivity and broad applicability across diverse materials and single-crystal surfaces. Consequently, SHINERS has seen widespread adoption in pivotal fields, such as interface chemistry, electrocatalysis, biomedicine, materials, and food safety. In this Perspective, we outline the evolutionary journey of SHINERS, delve deep into its applications in fundamental research for interface characterization and catalysis, and explore its practical utility in critical areas of food safety and biomedicine analysis. Additionally, we map out the prospective trajectory and future milestones that await SHINERS as it continues to revolutionize the landscape of scientific exploration.
作为一种无损和超灵敏的技术,表面增强拉曼光谱(SERS)50 多年来一直吸引着全球科学界的目光。在 SERS 衍生出的各种光谱技术中,壳隔离纳米粒子增强拉曼光谱(SHINERS)是一项前沿进展。SHINERS 中使用的创新型多功能核壳纳米粒子结构是界面研究的理想平台,具有高灵敏度和广泛的适用性,适用于各种材料和单晶表面。因此,SHINERS 已被广泛应用于界面化学、电催化、生物医学、材料和食品安全等关键领域。在本《视角》中,我们概述了 SHINERS 的发展历程,深入探讨了它在界面表征和催化基础研究中的应用,并探讨了它在食品安全和生物医学分析等关键领域的实用性。此外,我们还描绘了 SHINERS 未来的发展轨迹和里程碑,因为它将继续彻底改变科学探索的面貌。
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引用次数: 0
Recent Advances of Stimuli-Responsive Liquid–Liquid Interfaces Stabilized by Nanoparticles 纳米颗粒稳定的刺激响应型液液界面的最新进展
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1021/acsnano.4c11387
Qinpiao Yi, Liang Liu, Ganhua Xie
Liquid–liquid interfaces offer highly controlled, flexible, and adaptable platforms for precise molecular assemblies, enabling the construction of sophisticated functional materials. Interfacial assemblies of specific nanoparticles (NPs) and ligands can alter their physicochemical states under external stimuli, leading to macroscopic dynamic transformations at the interface. This Review summarizes and analyzes the recent advances of the assembly and disassembly behaviors of various stimuli-responsive nanoparticle surfactants (NPSs) at liquid–liquid interfaces, focusing on their responsive behaviors when exposed to external stimuli and the interaction forces between interfacial molecules. Additionally, we outline recent advancements in applications such as reconfigurable all-liquid devices, all-liquid 3D printing, and chemical reaction platforms. Finally, we discuss current challenges and future prospects for the development of applications in this rapidly evolving field.
液-液界面为精确的分子组装提供了高度可控、灵活和适应性强的平台,使复杂功能材料的构建成为可能。特定纳米粒子(NPs)和配体的界面组装可在外部刺激下改变其物理化学状态,从而导致界面的宏观动态变化。本综述总结并分析了各种刺激响应型纳米粒子表面活性剂(NPSs)在液液界面上的组装和拆卸行为的最新进展,重点关注它们在受到外部刺激时的响应行为以及界面分子之间的相互作用力。此外,我们还概述了可重构全液体设备、全液体三维打印和化学反应平台等应用领域的最新进展。最后,我们讨论了在这一快速发展的领域开发应用的当前挑战和未来前景。
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引用次数: 0
Multifunctional Microneedle Patches for Perivascular Gene Delivery and Treatment of Vascular Intimal Hyperplasia 用于血管周围基因递送和血管内膜增生治疗的多功能微针贴片
IF 17.1 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-15 DOI: 10.1021/acsnano.4c09527
Yi Cheng, Xiaoxuan Zhang, Xiangyi Wu, Youjun Ding, Linxi Zhu, Jun Pan, Yuanjin Zhao, Min Zhou
Gene therapy has emerged as a promising approach to address challenging cardiovascular diseases. Extensive efforts have been focused on developing highly efficient gene vectors with precise delivery techniques to enhance its effectiveness. In this study, we present multifunctional dopamine-gelatin microneedle patches with gene therapy capabilities to achieve perivascular gene delivery for intimal hyperplasia treatment. These patches that were fabricated through freeze-drying of gelatin are with recombinant adeno-associated virus (rAAVs)-carrying tips and dopamine coating backing layers. The lyophilized gelatin could not only effectively preserve the therapeutic activity of rAAVs but could also demonstrate the capability to penetrate the adventitia for efficient delivery. The incorporation of dopamine facilitated patch adhesion and extended the release duration. Based on these advantages, we have demonstrated that the rAAVs-loaded microneedle patches (AMNPs) behave satisfactorily in perivascular gene delivery to inhibit carotid artery restenosis in rats. These features indicate that the AMNPs are clinically valuable in the treatment of vascular intimal hyperplasia diseases.
基因疗法已成为解决具有挑战性的心血管疾病的一种前景广阔的方法。人们一直致力于开发高效的基因载体和精确的递送技术,以提高其有效性。在这项研究中,我们提出了具有基因治疗功能的多功能多巴胺明胶微针贴片,以实现血管周围基因递送,治疗内膜增生。这些微针贴片是通过冻干明胶制成的,具有携带重组腺相关病毒(rAAVs)的尖端和多巴胺涂层背层。冻干明胶不仅能有效保存重组腺相关病毒的治疗活性,还能穿透血管内膜进行有效输送。多巴胺的加入促进了贴片的粘附性并延长了释放时间。基于这些优点,我们证明了负载 rAAVs 的微针贴片(AMNPs)在血管周围基因递送方面的表现令人满意,可抑制大鼠颈动脉再狭窄。这些特点表明,AMNPs 在治疗血管内膜增生疾病方面具有临床价值。
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引用次数: 0
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