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JOURNAL OF CATALYSIS · 2022 · IF 8.047

Atomically dispersed Pt sites on porous metal–organic frameworks to enable dual reaction mechanisms for enhanced photocatalytic hydrogen conversion

Hao Zhang,Qiuye Li,Bowen Li,Bo Weng,Zhihong Tian,Jianjun Yang,Johan Hofkens,Feili Lai,Tianxi Liu

We report a porous metal–organic framework loaded with single Pt atoms, namely PCN-222(Pt) nanorods, which are prepared by the self-assembly of Pt-metalized tetrakis(4-carboxyphenyl)porphyrin ligand with a Zr 6 cluster. The mass-loading of Pt in the synthesized PCN-222(Pt) is up to 4.67%, and can be accurately controlled by using an in-situ reaction strategy. Remarkably, the PCN-222(Pt) exhibits a highly efficient photocatalytic hydrogen production rate of 614 μmol g -1 h −1 , which is 7.4 times higher than that of PCN-222 (an isostructural sample to PCN-222(Pt) without coordinated Pt ions in the porphyrin rings). The apparent quantum efficiency of PCN-222(Pt) reaches up to 1.049% at 420 nm. Electron paramagnetic resonance spectra confirm the as-formed intermediate Zr III , obtained from the reduction of Zr IV species, participates in the photocatalytic reaction. Density functional theory calculations demonstrate the positive role that single Pt atoms in PCN-222(Pt) play in optimizing the corresponding hydrogen binding energy. The existence of this dual reaction mechanism in PCN-222(Pt) greatly and synergistically boosts the photocatalytic H 2 production activity.

研究领域: 材料科学 · 催化 · 光催化 · 能量转换
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Advanced Healthcare Materials · 2024 · IF 10

An Oxidative Stress Nano-Amplifier for Improved Tumor Elimination and Combined Immunotherapy

Wei Zhang,Yijun Ran,Mi Yang,Yaqin Hu,Zhigang Wang,Yang Cao,Haitao Ran

Amplifying oxidative stress to disrupt intracellular redox homeostasis can accelerate tumor cell death. In this work, an oxidative stress amplifier (PP@T) is prepared for enhanced tumor oxidation therapy to reduce tumor growth and metastases. The nano-amplifier has been successfully constructed by embedding MTH1 inhibitor (TH588) in the PDA-coated porphyrin metal–organic framework PCN-224. The controllable-released TH588 is demonstrated from pores can hinder MTH1-mediated damage-repairing process by preventing the hydrolysis of 8-oxo-dG, thereby amplifying oxidative stress and exacerbating the oxidative DNA damage induced by the sonodynamic therapy of PP@T under ultrasound irradiation. Furthermore, PP@T can effectively induce immunogenic cell death to trigger systemic anti-tumor immune response. When administered in combination with immune checkpoint blockade, PP@T not only impedes the progression of the primary tumor but also achieves obvious antimetastasis in breast cancer murine models, including orthotopic and artificial whole-body metastasis models. Furthermore, the nanoplatform also provides photoacoustic imaging for in vivo treatment guidance. In conclusion, by amplifying oxidative stress and reactive oxygen species sensitized immunotherapy, this image-guided nanosystem shows potential for highly specific, effective combined therapy against tumor cells with negligible side-effects to normal cells which will provide a new insight for precise tumor treatment.

CAS / MDL: 62-31-7
研究领域: 肿瘤学 · 生物医学工程 · 免疫治疗 · 纳米技术 · 癌症治疗
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CATALYSIS TODAY · 2021 · IF 6.766

Construction of hexanuclear Ce(III) metal−porphyrin frameworks through linker induce strategy for CO2 capture and conversion

Liangliang Zhang,Yang Feng,Huihui He,Yang Liu,Jiena Weng,Peng Zhang,Wei Huang

In this article, we report a series of hexanuclear rare-earth MOFs based on Ce (III) and 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin, namely Ce-PCN-224, with a new zln topology through linker induce strategy. Ce-PCN-224 exhibits permanent porosity, high water and thermal stabilities, and the ability to adsorb dye molecules in the aqueous environment. Moreover, after post-metallation with Fe, Co, and Ni, Ce-PCN-224(Fe) and Ce-PCN-224(Co) were proved to be efficient heterogeneous catalysts for the cycloaddition of CO 2 with epoxides, attributed to the combination of multiple Lewis acidic sites.

研究领域: 材料科学 · 化学工程 · 环境科学 · 催化
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SENSORS AND ACTUATORS B-CHEMICAL · 2023 · IF 8.4

A colorimetric biosensor to track Trop-2 status of tumor cells for diagnosis of breast cancer

Tianyu Zeng,Shuai Wu,Qizhi Liang,Hai Shi,Jue Gong,Ningjun Duan,Wei Li,Genxi Li,Yongmei Yin

The emergence of antibody-drug conjugates (ADCs) targeting trophoblast cell-surface antigen-2 (Trop-2) has reshaped the therapeutic landscape of advanced breast cancer. Accurate profiling of the Trop-2 status of tumor cells can facilitate the identification of patients who will benefit from Trop-2-targeting therapy; however limited analytical method has hindered this process. In this study, we have proposed a specific and sensitive biosensor for visual tracking of the Trop-2 status of breast cancer cells based on tetrahedral DNA nanostructure (TDN)-decorated Fe-based metal-organic framework nanoparticles (TDN-PCN-222 (Fe)). In the design, a dual-aptamer-assisted biomimetic capture strategy shows high capture efficiency while maintaining the viability and original phenotype of captured cells, ensuring the accurate profiling of the Trop-2 status. Meanwhile, by using the high intrinsic peroxidase activity and excellent targeting ability of Trop-2-specific aptamer-linked TDN-PCN-222 (Fe), specific detection of Trop-2-positive tumor cells can be achieved with a limit of detection (LOD) of 10 cells/mL, and the Trop-2 status of tumor cells can be visually tracked. Moreover, the proposed biosensor has been successfully used for tracking the Trop-2 status of tumor cells in breast cancer tissues, suggesting that our method has great promise for clinical applications.

CAS / MDL: 79-43-6 54827-17-7
研究领域: 生物技术 · 癌症生物学 · 纳米技术 · 分子诊断
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-18 · IF 14.7

Biodegradable oxygen-evolving metalloantibiotics for spatiotemporal sono-metalloimmunotherapy against orthopaedic biofilm infections

Su Zheng,Xu Dongdong,Hu Xianli,Zhu Wanbo,Kong Lingtong,Qian Zhengzheng,Mei Jiawei,Ma Ruixiang,Shang Xifu,Fan Wenpei,Zhu Chen

Pathogen-host competition for manganese and intricate immunostimulatory pathways severely attenuates the efficacy of antibacterial immunotherapy against biofilm infections associated with orthopaedic implants. Herein, we introduce a spatiotemporal sono-metalloimmunotherapy (SMIT) strategy aimed at efficient biofilm ablation by custom design of ingenious biomimetic metal-organic framework (PCN-224)-coated MnO 2 -hydrangea nanoparticles (MnPM) as a metalloantibiotic. Upon reaching the acidic H 2 O 2 -enriched biofilm microenvironment, MnPM can convert abundant H 2 O 2 into oxygen, which is conducive to significantly enhancing the efficacy of ultrasound (US)-triggered sonodynamic therapy (SDT), thereby exposing bacteria-associated antigens (BAAs). Moreover, MnPM disrupts bacterial homeostasis, further killing more bacteria. Then, the Mn ions released from the degraded MnO 2 can recharge immune cells to enhance the cGAS-STING signaling pathway sensing of BAAs, further boosting the immune response and suppressing biofilm growth via biofilm-specific T cell responses. Following US withdrawal, the sustained oxygenation promotes the survival and migration of fibroblasts, stimulates the expression of angiogenic growth factors and angiogenesis, and neutralizes excessive inflammation. Our findings highlight that MnPM may act as an immune costimulatory metalloantibiotic to regulate the cGAS-STING signaling pathway, presenting a promising alternative to antibiotics for orthopaedic biofilm infection treatment and pro-tissue repair.

研究领域: 生物医学工程 · 材料科学 · 免疫学 · 骨科 · 传染病
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JOURNAL OF RARE EARTHS · 2025 · IF 7.2

Dye-sensitized rare-earth-doped nanoparticles and MOF heterostructures for enhanced NIR-II fluorescence imaging and synergistic photothermal and photodynamic therapy

Ming Qian,Jiarui Du,Qichuan Jiang,Wei Tao,Jiayi Zhang,Liang Gong

Early diagnosis and treatment of cancer are key problems for effective cancer therapy. Therefore, the development of multifunctional materials that can integrate imaging and therapeutic functions is of great importance. Lanthanide-doped nanoparticles@metal-organic frameworks (Ln-NPs@MOFs) offer an unprecedented opportunity to address this challenge, by combining the imaging capabilities of rare earth-doped nanoparticles with the photosensitizing properties of MOFs for photodynamic therapy (PDT). Here, we report a near-infrared (NIR) light-responsive nanoparticle based on a zirconium-porphyrin metal-organic framework (PCN-224) for synergistic photothermal and photodynamic therapy. Tetra(4-carboxyphenyl)porphyrin (TCPP) that constitutes the MOF framework serves as a natural photosensitizer, enabling efficient photodynamic therapy through Förster resonance energy transfer (FRET). The dye indocyanine green (ICG) was loaded into the MOF pores to sensitize the Ln nanoparticles, enhancing the upconversion fluorescence by 41 times and the downconversion fluorescence by 5 times, which is beneficial to the biological efficacy for imaging diagnosis. Meanwhile, ICG, a traditional photothermal agent, also imparts photothermal therapy capabilities to the system. Furthermore, the encapsulation of cancer cell membranes not only enhances biocompatibility but also improves the material's targeting towards cancer cells, thereby greatly enhancing the therapeutic effect. This dual-functional material provides a promising platform for the integration of cancer diagnosis and therapy.

研究领域: 生物医学工程 · 纳米医学 · 癌症诊疗一体化 · 光学成像 · 光疗
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