Tiancong Zhao

Collaborative Innovation Center of Chemistry for Energy Materials

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Xiaomin Li

Collaborative Innovation Center of Chemistry for Energy Materials

Dongyuan Zhao

Fudan University

Minchao Liu

Fudan University

Fan Zhang

Jinan University

Ahmed A. Elzatahry

University of Houston

Liang Chen

Fudan University

Runfeng Lin

Fudan University

Hongyue Yu

Collaborative Innovation Center of Chemistry for Energy Materials

Wei Li

Fudan University

Chin‐Te Hung

Collaborative Innovation Center of Chemistry for Energy Materials

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Fudan University

134

Collaborative Innovation Center of Chemistry for Energy Materials

Chinese Academy of Sciences

Sun Yat-sen University

Shanghai Stomatological Hospital

Jilin University

Shanghai Jiao Tong University

Sichuan University

University of Chinese Academy of Sciences

Tianjin University

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Surface curvature-induced oriented assembly of sushi-like Janus therapeutic nanoplatform for combined chemodynamic therapy

Journal of Nanobiotechnology (2023)

Yanming Ma Minchao Liu Mengmeng Hou Yufang Kou Wenxing Wang

Chemodynamic therapy (CDT) based on Fenton/Fenton-like reaction has emerged as a promising cancer treatment strategy. Yet, the strong anti-oxidation property of tumor microenvironment (TME) caused by endogenous glutathione (GSH) still severely impedes the effectiveness of CDT. Traditional CDT nanoplatforms based on core@shell structure possess inherent interference of different subunits, thus hindering the overall therapeutic efficiency. Consequently, it is urgent to construct a novel structure with isolated functional units and GSH depletion capability to achieve desirable combined CDT therapeutic efficiency.Herein, a surface curvature-induced oriented assembly strategy is proposed to synthesize a sushi-like novel Janus therapeutic nanoplatform which is composed of two functional units, a FeOOH nanospindle serving as CDT subunit and a mSiO2 nanorod serving as drug-loading subunit. The FeOOH CDT subunit is half covered by mSiO2 nanorod along its long axis, forming sushi-like structure. The FeOOH nanospindle is about 400 nm in length and 50 nm in diameter, and the mSiO2 nanorod is about 550 nm in length and 100 nm in diameter. The length and diameter of mSiO2 subunit can be tuned in a wide range while maintaining the sushi-like Janus structure, which is attributed to a Gibbs-free-energy-dominating surface curvature-induced oriented assembly process. In this Janus therapeutic nanoplatform, Fe3+ of FeOOH is firstly reduced to Fe2+ by endogenous GSH, the as-generated Fe2+ then effectively catalyzes overexpressed H2O2 in TME into highly lethal ·OH to achieve efficient CDT. The doxorubicin (DOX) loaded in the mSiO2 subunit can be released to achieve combined chemotherapy. Taking advantage of Fe3+-related GSH depletion, Fe2+-related enhanced ·OH generation, and DOX-induced chemotherapy, the as-synthesized nanoplatform possesses excellent therapeutic efficiency, in vitro eliminating efficiency of tumor cells is as high as ~ 87%. In vivo experiments also show the efficient inhibition of tumor, verifying the synthesized sushi-like Janus nanoparticles as a promising therapeutic nanoplatform.In general, our work provides a successful paradigm of constructing novel therapeutic nanoplatform to achieve efficient tumor inhibition.

Nanorod

10.1186/s12951-023-02138-0

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Black Titania Janus Mesoporous Nanomotor for Enhanced Tumor Penetration and Near-Infrared Light-Triggered Photodynamic Therapy

ACS Nano (2024)

Kexin Lv Mengmeng Hou Yufang Kou Hongyue Yu Mengli Liu

Thanks to their excellent photoelectric characteristics to generate cytotoxic reactive oxygen species (ROS) under the light-activation process, TiO2 nanomaterials have shown significant potential in photodynamic therapy (PDT) for solid tumors. Nevertheless, the limited penetration depth of TiO2-based photosensitizers and excitation sources (UV/visible light) for PDT remains a formidable challenge when confronted with complex tumor microenvironments (TMEs). Here, we present a H2O2-driven black TiO2 mesoporous nanomotor with near-infrared (NIR) light absorption capability and autonomous navigation ability, which effectively enhances solid tumor penetration in NIR light-triggered PDT. The nanomotor was rationally designed and fabricated based on the Janus mesoporous nanostructure, which consists of a NIR light-responsive black TiO2 nanosphere and an enzyme-modified periodic mesoporous organosilica (PMO) nanorod that wraps around the TiO2 nanosphere. The overexpressed H2O2 can drive the nanomotor in the TME under catalysis of catalase in the PMO domain. By precisely controlling the ratio of TiO2 and PMO compartments in the Janus nanostructure, TiO2&PMO nanomotors can achieve optimal self-propulsive directionality and velocity, enhancing cellular uptake and facilitating deep tumor penetration. Additionally, by the decomposition of endogenous H2O2 within solid tumors, these nanomotors can continuously supply oxygen to enable highly efficient ROS production under the NIR photocatalysis of black TiO2, leading to intensified PDT effects and effective tumor inhibition.

Penetration (warfare)

10.1021/acsnano.4c03652

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Unipolar Ionic Diode Nanofluidic Membranes Enabled by Stepped Mesochannels for Enhanced Salinity Gradient Energy Harvesting

Journal of the American Chemical Society (2024)

Yi Yang Shan Zhou Zirui Lv Chin‐Te Hung Zaiwang Zhao

Developing ionic diode membranes featuring asymmetric structures is in high demand for salinity gradient energy harvesting. These membranes offer benefits in mitigating ion concentration polarization, thereby promoting ion permeability. However, most reported works focus on the role of heterogeneous charge-based bipolar ionic diode membranes for ion concentration polarization suppression, with comparatively less attention given to maintaining ion selectivity. Herein, unipolar ionic diode nanofluidic mesoporous silica membranes featuring stepped mesochannels were developed via a micellar sequential oriented interfacial self-assembly strategy as a salinity gradient energy harvester. Due to the asymmetric mesochannels and unipolar structure (both sides carry negative charge), the ionic diode membranes exhibit a strong rectification ratio of ∼15.91 to facilitate unidirectional ion transport while maintaining excellent cation selectivity (cation transfer number of ∼0.85). Besides, the vertically aligned mesochannels significantly reduce ion transport resistance, generating a high ionic flux. Consequently, the unipolar ionic diode nanofluidic membranes demonstrate a power output of 5.88 W/m

Nanofluidics

10.1021/jacs.4c06949

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Versatile synthesis of uniform mesoporous superparticles from stable monomicelle units

Nature Protocols (2024)

Zaiwang Zhao Pengfei Zhang Yujuan Zhao Lipeng Wang Jie Zhang

10.1038/s41596-024-01073-0

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Streamlined Mesoporous Silica Nanoparticles with Tunable Curvature from Interfacial Dynamic-Migration Strategy for Nanomotors

Nano Letters (2021)

Yuzhu Ma Kun Lan Borui Xu Li Xu Linlin Duan

Streamlined architectures with a low fluid-resistance coefficient have been receiving great attention in various fields. However, it is still a great challenge to synthesize streamlined architecture with tunable surface curvature at the nanoscale. Herein, we report a facile interfacial dynamic migration strategy for the synthesis of streamlined mesoporous nanotadpoles with varied architectures. These tadpole-like nanoparticles possess a big streamlined head and a slender tail, which exhibit large inner cavities (75–170 nm), high surface areas (424–488 m2 g–1), and uniform mesopore sizes (2.4–3.2 nm). The head curvature of the streamlined mesoporous nanoparticles can be well-tuned from ∼2.96 × 10–2 to ∼5.56 × 10–2 nm–1, and the tail length can also be regulated from ∼30 to ∼650 nm. By selectively loading the Fe3O4 catalyst in the cavity of the streamlined silica nanotadpoles, the H2O2-driven mesoporous nanomotors were designed. The mesoporous nanomotors with optimized structural parameters exhibit outstanding directionality and a diffusion coefficient of 8.15 μm2 s–1.

Surface Modification

10.1021/acs.nanolett.1c01404

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Dual-Ligand Assisted Anisotropic Assembly for the Construction of NIR-II Light-Propelled Mesoporous Nanomotors

Journal of the American Chemical Society (2025)

Jia Jia Runfeng Lin Minchao Liu Mengmeng Hou Hongyue Yu

The advent of autonomous nanomotors presents exciting opportunities for nanodrug delivery. However, significant potential remains for enhancing the asymmetry of nanomotors and advancing the development of second near-infrared (NIR-II) light-propelled nanomotors capable of operating within deep tissues. Herein, we developed a dual-ligand assisted anisotropic assembly strategy that enables precise regulation of the interfacial energy between selenium (Se) nanoparticle and periodic mesoporous organosilica (PMO). This strategy facilitates the controllable anisotropic growth of PMO on the Se nanoparticle, leading to the formation of Se&PMO Janus nanohybrids. The exposure ratio of the Se subunit within the Janus nanohybrids can be finely tuned from 0% to 75%. Leveraging the transformability of the Se subunit, a variety of functional MxSe&PMO Janus nanocomposites (MxSe denotes metal selenide) were further derived. As a proof of concept, CuSe&PMO Janus nanohybrids, with NIR-II photothermal properties, were employed as NIR-II light-driven nanomotors. By precisely controlling the exposure ratio of the CuSe subunit within the Janus nanostructure, these CuSe&PMO nanomotors achieved optimal self-propulsion, thus enhancing cellular uptake and promoting deep tumor penetration. Furthermore, the high loading capacity and hydrophobic framework of the PMO subunit enabled the incorporation of hydrophobic disulfiram, thereby significantly boosting the efficacy of synergistic active-motion photothermal therapy.

10.1021/jacs.4c14011

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Imparting multi-functionality to covalent organic framework nanoparticles by the dual-ligand assistant encapsulation strategy

Nature Communications (2021)

Liang Chen Wenxing Wang Jia Tian Fanxing Bu Tiancong Zhao

Abstract The potential applications of covalent organic frameworks (COFs) can be further developed by encapsulating functional nanoparticles within the frameworks. However, the synthesis of monodispersed core@shell structured COF nanocomposites without agglomeration remains a significant challenge. Herein, we present a versatile dual-ligand assistant strategy for interfacial growth of COFs on the functional nanoparticles with abundant physicochemical properties. Regardless of the composition, geometry or surface properties of the core, the obtained core@shell structured nanocomposites with controllable shell-thickness are very uniform without agglomeration. The derived bowl-shape, yolk@shell, core@satellites@shell nanostructures can also be fabricated delicately. As a promising type of photosensitizer for photodynamic therapy (PDT), the porphyrin-based COFs were grown onto upconversion nanoparticles (UCNPs). With the assistance of the near-infrared (NIR) to visible optical property of UCNPs core and the intrinsic porosity of COF shell, the core@shell nanocomposites can be applied as a nanoplatform for NIR-activated PDT with deep tissue penetration and chemotherapeutic drug delivery.

10.1038/s41467-021-24838-7

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Citations (97)

Replenishing Cation-π Interactions for the Fabrication of Mesoporous Levodopa Nanoformulations for Parkinson Remission

ACS Nano (2024)

Min Guo Runfeng Lin Wenqing Xu Lihui Xu Minchao Liu

Directly assembling drugs into mesoporous nanoformulations will be greatly favored due to the combination of enhanced drug delivery efficiency and mesostructure-enabled nanobio interactions. However, such an approach is hindered due to the lack of understanding of polymer nanoparticles' formation mechanism, especially the relationship between polymerization, self-assembly, and the nucleation process. Here, by investigating the levodopa and dopamine polymerization process, we identify π-cation interaction as pivotal in the self-assembly and nucleation control of dopa molecules. Thus, through manipulation of the π-cation interaction, we present the direct assembly of a commercial drug, levodopa, into mesoporous nanoformulations. The synthesized nanospheres, approximately 200 nm in diameter, exhibit uniform mesopores of around 8 nm. These nanoformulations, abundant in mesopores, enhance chiral phenylalanine interaction with α-synuclein (Syn), curbing aggregation, safeguarding neurons, and alleviating Parkinson's pathology. When combating α-synuclein, the nanoformulation achieved ∼100% inhibition of protein aggregation and sustained neuron viability up to 300%. We believe that this study may advance mesoscale self-assembly knowledge, guiding future nanopharmaceutical developments.

10.1021/acsnano.4c09326

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Size and charge dual-transformable mesoporous nanoassemblies for enhanced drug delivery and tumor penetration

Chemical Science (2020)

Liang Chen Tiancong Zhao Mengyao Zhao Wenxing Wang Caixia Sun

Size and charge dual-transformable core@satellite structured nanoassemblies are developed to overcome multiple biological barriers in a drug delivery system.

Penetration (warfare)

Dual role

10.1039/c9sc06260b

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Citations (79)

Titanate nanotube-promoted chemical fixation of carbon dioxide to cyclic carbonate: a combined experimental and computational study

Catalysis Science & Technology (2015)

Aibing Chen Tiancong Zhao Hui Gao Limin Chen Jinzhu Chen

Titanate nanotubes are efficiently used as air- and water-tolerant, and recyclable Lewis acid catalysts for CO₂fixation to cyclic carbonate.

Carbon fixation

10.1039/c5cy01024a

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Citations (22)