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Near-infrared light-controllable bufalin delivery from a black phosphorus-hybrid supramolecular hydrogel for synergistic photothermal-chemo tumor therapy

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Nano Research 2021年第11期14卷 3988-3998页

作者： Jiaqi He Guoqin Chen Peng Zhao Caiwen Ou Cardiology Department of Panyu Central Hospital Guangzhou University of Chinese MedicineGuangzhou510006China Guangdong Provincial Key Laboratory of New Drug Screening School of Pharmaceutical SciencesSouthern Medical UniversityGuangzhou510515China Guangdong Provincial Key Laboratory of Shock and Microcirculation Zhujiang Hospital of Southern Medical UniversitySouthern Medical UniversityGuangzhou510280China

Bufalin is efficacious in treating various tumors, however, the clinical application of which is restricted by the myocardial toxicity. Developing a smart synergetic delivery system is widely considered as a promising therapeutic strategy. To address this issue, a black phosphorus hybrid polypeptides hydrogel was designed to highly load bufalin, and achieved near-infrared (NIR)-controllable drug release with synergistic photothermal-chemo therapeutic effect. Black phosphorus nanosheets (BPNSs) and bufalin were co-loaded in temperature-sensitive supramolecular hydrogel to receive smart hybridization (BP-bufalin@SH). With NIR irradiation (1 W·cm−2), BP-bufalin@SH exhibited a rapid and large temperature increase and released bufalin via light-controllable manner, with which the side effects of bufalin were greatly decreased. Combined with photothermal-chemo therapeutic effect, BP-bufalin@SH could collapse the mitochondrial transmembrane potential resulting in the irreversible apoptosis of tumor cells, and realize a highly efficient in vivo tumor elimination with good biosafety and biocompatibility. This work provides a new hydrogel platform for controlling bufalin release, and thus further promotes the practical application on antitumor therapy.

关键词： photothermal-chemo synergic therapy bufalin black phosphorus nanosheets supramolecular hydrogel

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Antibacterial conductive self-healable supramolecular hydrogel dressing for infected motional wound healing

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Science China Chemistry 2022年第11期65卷 2238-2251页

作者： Rui Yu Zhenlong Li Guoying Pan Baolin Guo Key Laboratory of Shaanxi Province for Craniofacial Precision Medicine Research College of StomatologyXi’an Jiaotong UniversityXi'an 710049China State Key Laboratory for Mechanical Behavior of Materials Frontier Institute of Science and TechnologyXi’an Jiaotong UniversityXi'an710049China

Wounds on stretchable parts of the human body cause prolonged suffering and involve more severe healing processes than wounds on stationary parts. However, they have received insufficient attention compared with other types of chronic wounds. In this study, a novel supramolecular gelatin(GT) hydrogel composed of GT-graft-aniline tetramer and quaternized chitosan was presented. The hydrogel was crosslinked by monoaldehyde β-cyclodextrin via host-guest interaction and dynamic Schiff base and was free from permanent covalent bonds, heavy metals, and oxidants. Given its dynamic feature, the hydrogel exhibited flexibility, self-healing, and tissue adhesiveness and well adapted to motion wounds. Moreover, the hydrogel was bioactive with conductivity, antioxidant property, hemostatic effect, antibacterial, and photothermal effect(the killing ratio for methicillinresistant Staphylococcus aureus(MRSA) was higher than 99.8% after 5 min of near-infrared irradiation) and exhibited ondemand removability. In the full-thickness MRSA-infected motional wound healing experiment, this novel hydrogel exhibited a significantly enhanced wound healing efficacy with a fast wound closure ratio(about 99.0% for 14 days), mild inflammatory response, high level of collagen deposition, and enhanced re-epithelialization by downregulating interleukin-6 and CD68 and upregulating vascular endothelial growth factor. The results indicated that this hydrogel has great potential in wound healing and skin tissue engineering and serves as an inspiration for the design of supramolecular biomaterials.

关键词： supramolecular hydrogel self-healing tissue adhesion joint wound

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Drug-peptide supramolecular hydrogel boosting transcorneal permeability and pharmacological activity via ligand-receptor interaction

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Bioactive Materials 2022年第4期7卷 420-429页

作者： Lin Chen Jie Deng Ailing Yu Yuhan Hu Bo Jin Pengyuan Du Jianhong Zhou Lei Lei Yuan Wang Serhii Vakal Xingyi Li Institute of Biomedical Engineering School of Ophthalmology&OptometryEye HospitalWenzhou Medical University270 Xueyuan RoadWenzhou325027PR China Key Laboratory of Diagnosis and Treatment of Severe Hepato-Pancreatic Diseases of Zhejiang Province The First Affiliated HospitalWenzhou Medical UniversityWenzhou325027PR China Structural Bioinformatics Laboratory BiochemistryÅbo Akademi UniversityTurku20541Finland

Boosting transcorneal permeability and pharmacological activity of drug poses a great challenge in the field of ocular drug *** the present study,we propose a drug-peptide supramolecular hydrogel based on anti-inflammatory drug,dexamethasone(Dex),and Arg-Gly-Asp(RGD)motif for boosting transcorneal permeability and pharmacological activity via the ligand-receptor *** drug-peptide(Dex-SA-RGD/RGE)supramolecular hydrogel comprised of uniform nanotube architecture formed spontaneously in phosphate buffered saline(PBS,pH=7.4)without external *** storage at 4℃,25℃,and 37℃ for 70 days,Dex-SA-RGD in hydrogel did not undergo significant hydrolysis,suggesting great long-term *** comparison to Dex-SA-RGE,Dex-SA-RGD exhibited a more potent in vitro anti-inflammatory efficacy in lipopolysaccharide(LPS)-activated RAW 264.7 macrophages via the inhibition of nuclear factorкB(NF-κB)signal *** importantly,using drug-peptide supramolecular hydrogel labeled with 7-nitro-2,1,3-benzoxadiazole(NBD),the Dex-SA-K(NBD)RGD showed increased performance in terms of integrin targeting and cellular uptake compared to Dex-SA-K(NBD)RGE,as revealed by cellular uptake *** topical instillation in rabbit’s eye,the proposed Dex-SA-K(NBD)RGD could effectively enhance the transcorneal distribution and permeability with respect to the Dex-SA-K(NBD)***,our findings demonstrate the performance of the ligand-receptor interaction for boosting transcorneal permeability and pharmacological activity of drug.

关键词： Active transport Integrin supramolecular hydrogel Ocular retention Corneal permeability

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Bioinspired self-assembly supramolecular hydrogel for ocular drug delivery

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Chinese Chemical Letters 2021年第12期32卷 3936-3939页

作者： Xianglian Li Hui Liu Ailing Yu Dan Lin Zhishu Bao Yuqin Wang Xingyi Li Institute of Biomedical Engineering School of Ophthalmology OptometryEye HospitalWenzhou Medical UniversityWenzhou 325027China

Based on a recent report concerning endogenous agents(i.e., pyridoxal phosphate, adenosine triphosphate, adenosine monophosphate, folinic acid) that modulate the oligomerization of apoptosis-associated speck-like protein(ASC) via the peptide epitope of KKFKLKL, we rationally designed and synthesized a nonapeptide(Nap FFKKFKLKL), which can co-assemble with dexamethasone sodium phosphate(Dexp) to generate a Nap FFKKFKLKL/Dexp supramolecular hydrogel for ocular drug *** Nap FFKKFKLKL/Dexp hydrogel formed instantly after the complexation of Nap FFKKFKLKL with Dexp in aqueous solution. The formed supramolecular hydrogels were thoroughly characterized by transmission electron microscopy(TEM), fluorescent spectrum, circular dichroism(CD) spectra and rheology. The peptide concentration significantly affected the in vitro release behavior of Dexp from the supramolecular hydrogel, and the higher peptide concentration resulted in the slower drug *** a single intravitreal injection, the proposed Nap FFKKFKLKL/Dexp hydrogel displayed good intraocular biocompatibility without having an adverse impact on the retinal architecture and eyesight functions during one month of follow-up. Using an experimental autoimmune uveitis(EAU) rat model,we demonstrated that the resulting Nap FFKKFKLKL/Dexp hydrogel had potent capacity to alleviate the intraocular inflammation and retain the morphology of retinal architecture. Overall, the resulting Nap FFKKFKLKL/Dexp hydrogel may be a promising drug carrier system to treat various posterior disorders(i.e., uveitis).

关键词： supramolecular hydrogel Self-assembly Drug delivery Ocular disorder

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Cascaded amplification of intracellular oxidative stress and reversion of multidrug resistance by nitric oxide prodrug based-supramolecular hydrogel for synergistic cancer chemotherapy

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Bioactive Materials 2021年第10期6卷 3300-3313页

作者： Jimin Zhang Meigui Deng Xiaoguang Shi Chuangnian Zhang Xiongwei Qu Xiuli Hu Weiwei Wang Deling Kong Pingsheng Huang Hebei Key Laboratory of Functional Polymers National-Local Joint Engineering Laboratory for Energy Conservation of Chemical Process Integration and Resources UtilizationSchool of Chemical Engineering and TechnologyHebei University of TechnologyTianjin300130China Tianjin Key Laboratory of Biomaterial Research Institute of Biomedical EngineeringChinese Academy of Medical Sciences and Peking Union Medical CollegeTianjin300192China State Key Laboratory of Medicinal Chemical Biology College of Life SciencesNankai UniversityTianjin300071China

*** Chemotherapy is the traditional treatment for clinical cancer patient[1,2].However,the therapeutic effect is often severely limited by the multidrug resistance(MDR)[3,4],which was commonly mediated by inactivating drugs,increasing efflux,stimulating DNA repair mechanisms,and/or activating detoxification pathways[5-7].Recent studies are committing to develop reasonable strategies for intervention of the molecular pathways mediating MDR,of which P-glycoprotein(P-gp)has been widely investigated[8].So far,several kinds of P-gp inhibitors,including verapamil[9],vitamin E[10],cyclosporin A[11],and small interfering RNA(siRNA)[12].

关键词： NO prodrug supramolecular hydrogel Oxidative stress Multidrug resistance Synergistic therapy

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Penetrating efficiency of supramolecular hydrogel eye drops:Electrostatic interaction surpasses ligand-receptor interaction

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Chinese Chemical Letters 2024年第11期35卷 419-422页

作者： Zhibin Ren Shan Li Xiaoying Liu Guanghao Lv Lei Chen Jingli Wang Xingyi Li Jiaqing Wang National Engineering Research Center of Ophthalmology and Optometry School of Ophthalmology and Optometry&Biomedical EngineeringEye HospitalWenzhou Medical UniversityWenzhou 325027China

The low drug bioavailability of eye drops challenges the therapy of ocular disorders with high *** of solutions is to extend the corneal retention and enhance the penetration of drug into *** we synthesize two fluorophore-conjugated peptide based analogs rich in positive charges(i.e.,NBDFFKK)and with a specific ligand(i.e.,NBD-FFRGD),respectively,to visualize their performances in vitro and in *** peptides both can self-assemble into supramolecular hydrogels with the microstructure of *** in vitro experiments exhibit that two peptides are both uniformly distributed in cytoplasm,and the intracellular amount of peptide rich in positive charges is significantly larger than that of peptide with a specific *** living corneal fluorescence shows that two peptides enter the corneal stroma within 15 min,and the peptide rich in positive charges is accumulated more extensively throughout the entire cornea,revealing that the supramolecular hydrogel eye drops penetrate the cornea more efficiently via electrostatic interaction than that via ligand-receptor *** work,as a comparative study of supramolecular hydrogel eye drops on penetrating efficiency,indicates a possible direction for the design of eye drops with efficient corneal penetration.

关键词： supramolecular hydrogel Eye drop Electrostatic interaction Ligand-receptor interaction Corneal penetration

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Autocatalytic strategy for tuning drug release from peptide-drug supramolecular hydrogel

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Chinese Chemical Letters 2023年第10期34卷 204-208页

作者： Yuqin Wu Tian Xia Xiaohui Ma Lei Lei Lulu Du Xiaoning Xu Xiangyi Liu Yueting Shi Xingyi Li Deqing Lin Institute of Biomedical Engineering School of Ophthalmology&Optometry and Eye HospitalWenzhou Medical UniversityWenzhou 325027China

Peptide-drug conjugates(PDCs) composed of peptide, spacer and drug have gained extensive attention in the field of drug delivery owing to its precise control over the drug payload and architecture. However,the achievement of controllable and rapid drug release at targeted site by PDCs is still a great challenge for pharmaceutist. Herein, we introduced the histidine residue into PDCs to generate a supramolecular hydrogel via a p H-trigger strategy, which exhibited an autocatalytic effect to precisely tune drug release from PDCs hydrogel. Using indomethacin(Idm) as model drug, various PDCs(Y(Idm)EEH, Y(Idm)EEK and Y(Idm)EER) were synthesized and their self-assembling properties were investigated in terms of critical aggregation concentration(CAC), transmission electron microscopy(TEM) and rheometer. Introduction of histidine residue into PDCs presented a robust catalytic activity on the ester hydrolysis of p-nitrophenyl acetate in aqueous solution, as well conferred the autocatalytic capacity to hydrolyze the PDCs into active parent drug(Idm). Overall, we reported an autocatalytic activity of histidine residue to precisely tune drug release from PDCs hydrogels.

关键词： Peptide-drug conjugates supramolecular hydrogel Autocatalysis Hydrolysis Drug release

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Application of supramolecular hydrogel in supercapacitors: Opportunities and challenges

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Aggregate 2024年第5期5卷 159-180页

作者： Wenshi Xu Aibing Chen College of Chemical and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuangChina

Supercapacitors(SCs)are studied and used in variousﬁelds due to their high power density,fast charging/discharging rate,as well as long cycle *** to other traditional electrode and electrolyte materials,supramolecular hydrogels have great advantages in the application of SCs due to their excellent *** covalent bonds,supramolecular systems are assembled through dynamic reversible bonds,including host–guest interactions,ion interactions,electrostatic interactions,hydrogen bonding,coordination interactions,*** resulting supramolecular hydrogels show some special functions,such as stretching,compression,adhesion,self-healing,stimulus responsiveness,etc.,making them strong candidates for the next generation of energy storage *** paper reviews the representative progress of electrodes,electrolytes,and SCs based on supramolecular ***,the properties of supramolecular hydrogels,such as conductivity,exten-sibility,compressibility and elasticity,self-healing,frost resistance,adhesion,andﬂexibility,are also reviewed to highlight the key role of excellent properties of hydro-gel materials in *** addition,this article also discusses the challenges faced by current technologies,hoping to continue promoting future research in thisﬁeld.

关键词： electrode electrolyte noncovalent interactions supercapacitors supramolecular hydrogel

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Influence of supramolecular Chiral hydrogel on Cellular Behavior of Endothelial Cells Under High-Glucose-Induced Injury

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Journal of Shanghai Jiaotong university(Science) 2021年第1期26卷 17-24页

作者： CAI Weijie HAMUSHAN Musha ZHAO Changli CHENG Pengfei ZHONG Wanrun HAN Pei Department of Orthopedics the Sixth People’s Hospital Affiliated to Shanghai Jiao Tong UniversityShanghai 200233China School of Materials Science and Engineering Shanghai Jiao Tong UniversityShanghai 200240China

In order to manage the impaired wound healing of diabetic chronic wounds induced by high-glucose-damaged endothelial cells,a glucose-induced injured endothelial cell model is established in this research to explore the regulatory effects of a supramolecular chiral hydrogel on injured endothelial *** behaviors of endothelial cells under different culture conditions are evaluated by CCK-8,5-ethynyl-2′-deoxyuridine(EdU)staining,adhesion,and Transwell *** expression levels of angiogenesis-related markers,including nitric ox-ide,endothelial nitric oxide synthase(eNOS),and vascular endothelial growth factor(VEGF),are also assessed by enzyme-linked immune sorbent assay(ELISA)and the polymerase chain reaction(PCR).The results demonstrate that the left-handed chirality of the supramolecular chiral hydrogel can promote cell proliferation and enhance the adhesion and migration ability of impaired endothelial ***,enhanced nitric oxide synthesis and elevated expression of eNOS and VEGF are observed in cells in the left-handed chiral ***,the left-handed supramolecular chiral hydrogel can regulate the cellular behavior of high-glucose-injured endothelial cells,including cell proliferation,adhesion,migration,and angiogenesis,offering the potential to promote diabetic wound healing.

关键词： chirality supramolecular hydrogel diabetes endothelial cells wound healing

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Construction and Properties of the Me_(10)Q[5]/2,7-diaminofluorenedihydrochloride supramolecular hydrogel

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贵州大学学报（自然科学版） 2024年第6期41卷 19-25页

作者： GUO Haning GAO Ruihan TAO Zhu School of Chemistry and Biological Engineering University of Science and Technology BeijingBeijing 100083China Key Laboratory of Macrocyclic and supramolecular Chemistry of Guizhou Province Guiyang 550025China

Compared to traditional polymer hydrogels,supramolecular hydrogels exhibits superior reversibility and stimulus response due to the instantaneous and reversible nature of non-covalent *** this paper,we utilized the host-guest exclusion interaction between Decamethylcucurbit[5]uril(Me_(10)Q[5])and the 2,7-diaminofluorenedihydrochloride(DAF·HCl)to construct a Q[n]-based hydrogel *** composition,structure,and properties of the hydrogel were compre-hensively characterized using rheometer,nuclear magnetic resonance,scanning electron *** cost-effective and straightforward hydrogel synthesis method paves the way for the scalable production of practical and commercially viable Q[n]-based hydrogels.

关键词： decamethylcucurbituril 2,7-diaminofluorenedihydrochloride supramolecular hydrogel host-guest exclusion interaction

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