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学者姓名:姚宇航
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Abstract :
Bioorthogonal catalysis mediated by abiotic transition metal catalysts (TMCs) is emerging as a momentum- gathering strategy for in situ generation of therapeutics. However, the unpredictable leakage and deposition of TMCs in living systems easily lead to nonspecific exposure of catalysts and concomitant off-target prodrug activation. Herein, we propose an enzyme-gated bioorthogonal catalytic nanoreactor constructed from hyaluronic acid (HA)-coated dendritic mesoporous silica nanoparticles (DMSNs), where the latter serves as a host for robustly immobilizing organometallic Ru(II) catalysts via covalent interactions. The covalent immobilization of catalysts within the nanoscaffold effectively avoids nonspecific metal leakage under biological conditions. Importantly, the grafted HA not only acts as a "gatekeeper" preventing unintended catalyst exposure in nontargeted tissues but also acts as a ligand targeting CD44 overexpressed cancer cells. Upon receptor-mediated endocytosis into tumor cells, HA is degraded by the overexpressed hyaluronidase-1, leading to the channel opening of the nanoreactors and hence gaining the accessibility of Ru(II) complexes to prodrugs. The therapeutic potency of this enzyme-gated nanoreactor in mediating site- specific activation of caged prodrugs was systematically demonstrated both in cellular settings and in tumor-bearing murine models. This enzyme-gated strategy enhances the efficacy of localized treatment while avoiding off-target prodrug activation, paving the way for advancing bioorthogonal catalysis for disease management in a safe and effective way.
Keyword :
bioorthogonal catalysis bioorthogonal catalysis cancer therapy cancer therapy catalyst immobilization catalyst immobilization enzyme-gated enzyme-gated prodrugs prodrugs
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GB/T 7714 | Guo, Yuheng , Jiang, Fang , Zhu, Xiaohui et al. An enzyme-gated bioorthogonal catalytic nanoreactor for tumor-specific prodrug activation [J]. | NANO RESEARCH , 2025 , 18 (2) . |
MLA | Guo, Yuheng et al. "An enzyme-gated bioorthogonal catalytic nanoreactor for tumor-specific prodrug activation" . | NANO RESEARCH 18 . 2 (2025) . |
APA | Guo, Yuheng , Jiang, Fang , Zhu, Xiaohui , He, Wen , Song, Sijie , Shou, Xuecen et al. An enzyme-gated bioorthogonal catalytic nanoreactor for tumor-specific prodrug activation . | NANO RESEARCH , 2025 , 18 (2) . |
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Control of phosphate capture and release is vital in environmental, biological, and pharmaceutical contexts. However, the binding of trivalent phosphate (PO43-) in water is exceptionally difficult due to its high hydration energy. Based on the anion coordination chemistry of phosphate, in this study, four charge-neutral tripodal hexaurea receptors (L1-L4), which were equipped with morpholine and polyethylene glycol terminal groups to enhance their solubility in water, were synthesized to enable the pH-triggered phosphate binding and release in aqueous solutions. Encouragingly, the receptors were found to bind PO43- anion in a 1 : 1 ratio via hydrogen bonds in 100 % water solutions, with L1 exhibiting the highest binding constant (1.2x103 M-1). These represent the first neutral anion ligands to bind phosphate in 100 % water and demonstrate the potential for phosphate capture and release in water through pH-triggered mechanisms, mimicking native phosphate binding proteins. Furthermore, L1 can also bind multiple bioavailable phosphate species, which may serve as model systems for probing and modulating phosphate homeostasis in biological and biomedical researches. A biomimetic charge-neutral anion receptor for reversible binding and release of highly hydrated phosphate in water image
Keyword :
Anion Coordination Chemistry Anion Coordination Chemistry Hydrogen Bond Hydrogen Bond Phosphate Binding in Water Phosphate Binding in Water Water-Soluble Anion Receptors Water-Soluble Anion Receptors
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GB/T 7714 | He, Maolin , Yao, Yuhang , Yang, Zihe et al. Biomimetic Charge-Neutral Anion Receptors for Reversible Binding and Release of Highly Hydrated Phosphate in Water [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (33) . |
MLA | He, Maolin et al. "Biomimetic Charge-Neutral Anion Receptors for Reversible Binding and Release of Highly Hydrated Phosphate in Water" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 63 . 33 (2024) . |
APA | He, Maolin , Yao, Yuhang , Yang, Zihe , Li, Boyang , Wang, Ji , Wang, Yanchao et al. Biomimetic Charge-Neutral Anion Receptors for Reversible Binding and Release of Highly Hydrated Phosphate in Water . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 63 (33) . |
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In situ monitoring microRNA (miRNA) expression in vivo holds immense potential for directly visualizing the occurrence and progression of tumors. However, the significant barrier to developing a probe that can overcome the low abundance of miRNAs while providing an output signal with unlimited tissue penetration depth remains formidable. In this study, we developed a DNA machine-based magnetic resonance imaging nanoprobe (MRINP) for amplified detection of miR-21 in vivo. The MRINP was constructed with superparamagnetic Fe3O4 nano- particles (NPs), paramagnetic Gd-DOTA complexes, and miR-21-activated DNA machines; the DNA machine was composed of hairpin DNAzyme (HD) strands serving as the DNAzyme walker and hairpin substrate (HS) strands serving as the track. Once uptake into tumor cells, the intracellular miR-21 specifically recognized and hybridized with the HD strand, restoring the activity of DNAzyme. Subsequently, the DNAzyme walker autonomously traveled on the surface of MRINP, and each step movement of the DNAzyme walker resulted in the cleavage of its substrate strands and the ensued release of the Gd-DOTA complex-labeled oligonucleotides, turning on the T1 signal of Gd-DOTA complexes for in situ imaging of miR-21 in tumor-bearing mice. This strategy would offer a promising approach for mapping tumor-specific biomarkers in vivo with unlimited penetration depth.
Keyword :
Biosensor Biosensor DNA machine DNA machine Magnetic resonance imaging Magnetic resonance imaging miR-21 detection miR-21 detection Tumor imaging Tumor imaging
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GB/T 7714 | Song, Sijie , Wang, Qi , Xie, Jiangao et al. A DNA machine-based magnetic resonance imaging nanoprobe for in vivo microRNA detection [J]. | TALANTA , 2024 , 281 . |
MLA | Song, Sijie et al. "A DNA machine-based magnetic resonance imaging nanoprobe for in vivo microRNA detection" . | TALANTA 281 (2024) . |
APA | Song, Sijie , Wang, Qi , Xie, Jiangao , Guo, Yuheng , He, Wen , Yao, Yuhang et al. A DNA machine-based magnetic resonance imaging nanoprobe for in vivo microRNA detection . | TALANTA , 2024 , 281 . |
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Microneedle patches for topical administration of photodynamic therapy (PDT) sensitizers are attractive owing to their safety, selectivity, and noninvasiveness. However, low-efficiency photosensitizer delivery coupled with the limitations of the hypoxic tumor microenvironment remains challenging. To overcome these issues, we developed an effective microneedle patch based on intermolecular electrostatic interactions within a photosensitizer matrix containing a zinc-containing porphyrin analogue, ZnBP (w). This design improved the mechanical strength of the microneedle patch and enhanced the photosensitizer loading efficiency in aqueous environments. A key feature of the system is efficient electron transfer between ZnBP (w) and NADH upon photoirradiation. Electrostatic interactions between ZnBP (w) and NADH were hypothesized to support initial binding and subsequent photoinduced electron transfer, disrupting NADH/NAD+ homeostasis and inducing tumor cell death. The developed microneedle patch demonstrated an antiangiogenesis effect in a vascular malformation model and an antitumor effect in a melanoma mouse model after transdermal administration. This study highlights the benefits of electrostatic interactions in designing microneedle PDT patches and their clinical potential, particularly in reducing systemic phototoxicity.
Keyword :
capillary malformation capillary malformation electrostatic interaction electrostatic interaction melanoma melanoma microneedle patch microneedle patch photodynamic therapy photodynamic therapy
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GB/T 7714 | Zhang, Hang , Xie, Wen-Chuan , Yao, Yuhang et al. Electrostatic Force-Enabled Microneedle Patches that Exploit Photoredox Catalysis for Transdermal Phototherapy [J]. | ACS APPLIED MATERIALS & INTERFACES , 2024 , 17 (2) : 3038-3051 . |
MLA | Zhang, Hang et al. "Electrostatic Force-Enabled Microneedle Patches that Exploit Photoredox Catalysis for Transdermal Phototherapy" . | ACS APPLIED MATERIALS & INTERFACES 17 . 2 (2024) : 3038-3051 . |
APA | Zhang, Hang , Xie, Wen-Chuan , Yao, Yuhang , Tang, Zi-Yi , Ni, Wen-Xiu , Wang, Bingwu et al. Electrostatic Force-Enabled Microneedle Patches that Exploit Photoredox Catalysis for Transdermal Phototherapy . | ACS APPLIED MATERIALS & INTERFACES , 2024 , 17 (2) , 3038-3051 . |
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