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dual-responsive supramolecular photodynamic nanomedicine with activatable immunomodulation for enhanced antitumor therapy

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Acta Pharmaceutica Sinica B 2024年第2期14卷 765-780页

作者： Siqin He Lulu Wang Dongxu Wu Fan Tong Huan Zhao Hanmei Li Tao Gong Huile Gao Yang Zhou Key Laboratory of Tropical Biological Resources of Ministry of Education School of Pharmaceutical SciencesHainan UniversityHaikou 570200China Key Laboratory of Drug-Targeting and Drug Delivery System West China School of PharmacySichuan UniversityChengdu 610041China Revvity Inc. WalthamMA 02451USA School of Food and Biological Engineering Chengdu UniversityChengdu 610106China

A major challenge facing photodynamic therapy(PDT) is that the activity of the immuneinduced infiltrating CD8^(+)T cells is subject to the regulatory T lymphocytes(Tregs), leaving the tumor at risk of recurrence and metastasis after the initial ablation. To augment the antitumor response and reprogram the immunosuppressive tumor microenvironment(TME), a supramolecular photodynamic nanoparticle(DACss) is constructed by the host-guest interaction between demethylcantharidin-conjugated β-cyclodextrin(DMC-CD) and amantadine-terminated disulfide-conjugated FFVLGGGC peptide with chlorin e6 decoration(Ad-ss-pep-Ce6) to achieve intelligent delivery of photosensitizer and immunomodulator for breast cancer treatment. The acid-labile β-carboxamide bond of DMC-CD is hydrolyzed in response to the acidic TME, resulting in the localized release of DMC and subsequent inhibition of Tregs.The guest molecule Ad-ss-pep-Ce6 can be cleaved by a high level of intracellular GSH, reducing photosensitizer toxicity and increasing photosensitizer retention in the tumor. With a significant increase in the CTL/Treg ratio, the combination of Ce6-based PDT and DMC-mediated immunomodulation adequately achieved spatiotemporal regulation and remodeling of the TME, as well as improved primary tumor and in situ lung metastasis suppression with the aid of PD-1 antibody.

关键词： Photodynamic therapy Immunosuppressive microenvironment Immunomodulator dual-responsive Supramolecularassembly Checkpointblockade

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Glucose and MMP-9 dual-responsive hydrogel with temperature sensitive self-adaptive shape and controlled drug release accelerates diabetic wound healing

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Bioactive Materials 2022年第11期7卷 1-17页

作者： Wanyi Zhou Zhiguang Duan Jing Zhao Rongzhan Fu Chenhui Zhu Daidi Fan Shaanxi Key Laboratory of Degradable Biomedical Materials School of Chemical EngineeringNorthwest UniversityXi’an710069ShaanxiChina Shaanxi R&D Center of Biomaterials and Fermentation Engineering School of Chemical EngineeringNorthwest UniversityXi’an710069ShaanxiChina Biotech.&Biomed.Research Institute Northwest UniversityXi’an710069ShaanxiChina

Chronic diabetic wounds are an important healthcare challenge. High concentration glucose, high level of matrix metalloproteinase-9 (MMP-9), and long-term inflammation constitute the special wound environment of diabetic wounds. Tissue necrosis aggravates the formation of irregular wounds. All the above factors hinder the healing of chronic diabetic wounds. To solve these issues, a glucose and MMP-9 dual-response temperature-sensitive shape self-adaptive hydrogel (CBP/GMs@Cel&INS) was designed and constructed with polyvinyl alcohol (PVA) and chitosan grafted with phenylboric acid (CS-BA) by encapsulating insulin (INS) and gelatin microspheres con-taining celecoxib (GMs@Cel). Temperature-sensitive self-adaptive CBP/GMs@Cel&INS provides a new way to balance the fluid-like mobility (self-adapt to deep wounds quickly, approximately 37 ◦C) and solid-like elasticity (protect wounds against external forces, approximately 25 ◦C) of self-adaptive hydrogels, while simultaneously releasing insulin and celecoxib on-demand in the environment of high-level glucose and MMP-9. Moreover, CBP/ GMs@Cel&INS exhibits remodeling and self-healing properties, enhanced adhesion strength (39.65 ± 6.58 kPa), down-regulates MMP-9, and promotes cell proliferation, migration, and glucose consumption. In diabetic full-thickness skin defect models, CBP/GMs@Cel&INS significantly alleviates inflammation and regulates the local high-level glucose and MMP-9 in the wounds, and promotes wound healing effectively through the synergistic effect of temperature-sensitive shape-adaptive character and the dual-responsive system.

关键词： dual-responsive Temperature-sensitive Shape self-adaptive hydrogels Diabetic wound healing

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Integrated and dual-responsive lipopeptide nanovector with parallel effect to tumor and micro-environment regulation by efficient gene and drug co-delivery

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Chinese Chemical Letters 2023年第5期34卷 420-426页

作者： Xiaobing Chen Huan Yang Xu Song Hong Liang Yu Wei Jiao Lu Matthias Barz Rongrong Jin Yu Nie National Engineering Research Center for Biomaterials Sichuan UniversityChengdu 610064China Leiden Academic Center for Drug Research(LACDR) Leiden UniversityLeiden 2333 CCThe Netherlands Department of Pharmacy Sichuan Academy of Medical Sciences&Sichuan Provincial People's HospitalSchool of MedicineUniversity of Electronic Science and Technology of ChinaChengdu 610072China

The integrated lipopeptide(RVA)/gene complexes are fabricated with bi-directional regulation on tumor cells and micro-environment.After self-assembling and target coating modification,the poly(γ-glutamic acid)(γ-PGA)/RVA nano-vectors can sequentially respond to pH&redox stimuli,and guarantee efficient therapeutic gene delivery and control release of all-trans retinoic acid.The design provides a facile but promising strategy to treat refractory cancers.

关键词： Gene delivery Integrated co-delivery dual-responsive Lipopeptide Tumor micro-environment regulation

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pH and H2O2 dual-responsive carbon dots for biocatalytic transformation monitoring

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Chinese Chemical Letters 2019年第9期30卷 1635-1638页

作者： Wenxin Lv Xin Wang Jiahui Wu Haiyin Li Feng Li College of Chemistry and Pharmaceutical Sciences Qingdao Agricultural University

Development of sensitive biosensors for biocatalytic transformations monitoring is in high demand but remains a great challenge. It is ascribed to the current strategies that focused on the single metabolite detection, which may bring about the relatively low sensitivity and false diagnosis result. Herein, we report the design and fabrication of novel carbon dots(CDs) with strong orange light emission, pH and H2O2 dual-responsive characteristics. The fluorescence quenching of CDs by H+and H2O2 enables the highly sensitive detection of H+/H2O2-generating biocatalytic transformations. This is exemplified by the glucose oxidase-mediated catalytic oxidation reaction on glucose, in which H+and H2O2 would be formed. As compared to the case in which glucose is present, significant fluorescence reduction is detected, and the fluorescence intensity is negatively proportional to glucose concentration. Thus, highly sensitive detection of glucose was readily achieved with a detection limit down to 10.18 nmol/L. The prepared CDs not only realize the highly sensitive detection of glucose, but also allows the probing other substances by changing the enzymes, thus providing a versatile platform, and demonstrating good potential to be used for biocatalytic transformations effective monitoring.

关键词： Carbon dots dual-responsive pH H2O2 Glucose Biocatalytic transformations

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Novel robust cellulose-based foam with pH and light dual-response for oil recovery

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Frontiers of Materials Science 2018年第2期12卷 118-128页

作者： Qian WANG Guihua MENG Jianning WU Yixi WANG Zhiyong LIU Xuhong GUO School of Chemistry and Chemical Engineering Shihezi University/Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan Key Laboratory for Green Processing of Chemical Engineering of Xinjiang Bingtuan/Key Laboratory of Materials-Oriented Chemical Engineering of Xinjiang Uygur Autonomous Region/Engineering Research Center of Materials-Oriented Chemical Engineering of Xinjiang Bingtuan Shihezi 832003 China State Key Laboratory of Chemical Engineering East China University of Science and Technology Shanghai 200237 China

We fabricated pH and light dual-responsive adsorption materials which could induce the transition of surface wettability between hydrophobicity and hydrophilicity by using ATRPo The structure and morphology of adsorption materials were confirmed by ATR-FTIR, XPS, TGA and SEM. It showed that the modified cellulose （CE）- based foam was hydrophobic, which can adsorb a range of oils and organic solvents in water under pH = 7.0 or visible light irradiation （λ〉500 nm）. Meanwhile, the wettability of robust CE-based foam can convert hydrophobicity into hydrophilicity and underwater oleophobicity under pH = 3.0 or UV irradiation （λ = 365 nm）, giving rise to release oils and organic solvents. Most important of all, the adsorption and desorption processes of the modified CE-based foam could be switched by external stimuli. Furthermore, the modified CE-based foam was not damaged and still retained original performance after reversible cycle repeated for many times with variation of surface wettability. In short, it indicates that CE-based foam materials with switchable surface wettability are new responsive absorbent materials and have owned potential application in the treatment of oil recovery.

关键词： cellulose-based foam dual-responsive adsorption materials switchable wettability oil recovery

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