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A Robust Self-healing Polyurethane Elastomer Enabled by Tuning the Molecular Mobility and Phase Morphology through disulfide bonds

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Chinese Journal of Polymer Science 2021年第10期39卷 1299-1309,I0007页

作者： Hai-Tao Wu Bi-Qiang Jin Hao Wang Wen-Qiang Wu Zhen-Xing Cao Zhao-Yang Yuan Yue Huang Wei-Hang Li Guang-Su Huang Lu-Sheng Liao Jin-Rong Wu State Key Laboratory of Polymer Materials Engineering College of Polymer Science and EngineerngSichuan UniversityChengdu 610065China Guangdong Provincial Key Laboratory of Natural Rubber Processing Agricultural Products Processing Research Institute of Chinese Academy of Tropical Agricultural SciencesZhanjiang 524001China

Elastomers with outstanding strength,toughness and healing efficiency are highly promising for many emerging fields.However,it is still a challenge to integrate all these beneficial features in one elastomer.Herein,an asymmetric alicyclic structure adjacent to aromatic disulfide was tactfully introduced into the backbone of polyurethane(PU)elastomer.Specifically,such elastomer(PU-HPS)was fabricated by polycondensing polytetramethylene ether glycol(PTMEG),isophorone diisocyanate(IPDI)and p-hydroxydiphenyl disulfide(HPS)via one-pot method.The molecular mobility and phase morphology of PU-HPS can be tuned by adjusting the HPS content.Consequently,the dynamic exchange of hydrogen and disulfide bonds in the hard segment domains can also be tailored.The optimized sample manifests outstanding tensile strength(46.4 MPa),high toughness(109.1 MJ/m^(3)),high self-healing efficiency after fracture(90.3%),complete scratch recovery(100%)and good puncture resistance.Therefore,this work provides a facile strategy for developing robust self-healing polymers.

关键词： Self-healing Polyurethane disulfide bonds Chain mobility Phase morphology

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“Pincer movement”:Reversing cisplatin resistance based on simultaneous glutathione depletion and glutathione S-transferases inhibition by redox-responsive degradable organosilica hybrid nanoparticles

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Acta Pharmaceutica Sinica B 2022年第4期12卷 2074-2088页

作者： Boyi Niu Yixian Zhou Kaixin Liao Ting Wen Sixian Lao Guilan Quan Xin Pan Chuanbin Wu School of Pharmaceutical Sciences Sun Yat-sen UniversityGuangzhou 510006China College of Pharmacy Jinan UniversityGuangzhou 510632China

The therapeutic efficacy of cisplatin has been restricted by drug resistance of cancers.Intracellular glutathione(GSH)detoxification of cisplatin under the catalysis of glutathione S-transferases(GST)plays important roles in the development of cisplatin resistance.Herein,a strategy of“pincer movement”based on simultaneous GSH depletion and GST inhibition is proposed to enhance cisplatin-based chemotherapy.Specifically,a redox-responsive nanomedicine based on disulfide-bridged degradable organosilica hybrid nanoparticles is developed and loaded with cisplatin and ethacrynic acid(EA),a GST inhibitor.Responding to high level of intracellular GSH,the hybrid nanoparticles can be gradually degraded due to the break of disulfide bonds,which further promotes drug release.Meanwhile,the disulfide-mediated GSH depletion and EA-induced GST inhibition cooperatively prevent cellular detoxification of cisplatin and reverse drug resistance.Moreover,the nanomedicine is integrated into microneedles for intralesional drug delivery against cisplatin-resistant melanoma.The in vivo results show that the nanomedicine-loaded microneedles can achieve significant GSH depletion,GST inhibition,and consequent tumor growth suppression.Overall,this research provides a promising strategy for the construction of new-type nanomedicines to overcome cisplatin resistance,which extends the biomedical application of organosilica hybrid nanomaterials and enables more efficient chemotherapy against drug-resistant cancers.

关键词： Cancer therapy Cisplatin Drug resistance Glutathione depletion Glutathione Stransferases disulfide bonds Organosilica hybrid nanoparticles Ethacrynic acid

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Engineering Reversible Hydrogels for 3D Cell Culture and Release Using Diselenide Catalyzed Fast disulfide Formation

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Chinese Journal of Chemistry 2022年第13期40卷 1578-1584,I0002页

作者： Yueying Han Cheng Liu Huaping Xu Yi Cao Collaborative Innovation Center of Advanced Microstructures National Laboratory of Solid State MicrostructureKey Laboratory of Intelligent Optical Sensing and ManipulationMinistry of EducationDepartment of PhysicsNanjing UniversityNanjingJiangsu 210093China Jinan Microecological Biomedicine Shandong Laboratory JinanShandong 250021China Key Lab of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China

Hydrogels crosslinked by dynamic covalent bonds can effectively mimic the viscoelastic properties of native extracellular matrix and have been widely explored for 3D cell culture.disulfide is one of the most common dynamic bonds in biological systems whose formation and cleavage are catalyzed by a set of dedicated enzymes.However,in vitro formation of disulfide bonds is a slow process and requires harsh catalysts.Therefore,it is difficult to use disulfide crosslinked hydrogels for cell culture.n this work,we show that disulfide bonds can be formed by thiol-diselenide(Dise)exchange under blue light llumination.This reaction is fast,reversible,and biocompatible.Moreover,residual diselenide in the hydrogel network can also accelerate thiol-disulfide exchange reactions leading to faster cell release from the hydrogels upon the addition of thiol-containing agents.We anticipate that disulfide crosslinked hydrogels catalyzed by diselenide can find broad biomedical applications,such as cell culture,celldelivery,and drug-controlled release.

关键词： disulfide bonds Diselenide bonds Photocatalysis Gels Cellencapsulation

Spectroscopic Analysis on the Effect of Temperature on Kunitz Domain 1 of Human Tissue Factor Pathway Inhibitor-2

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Acta Biochimica et Biophysica Sinica 2007年第6期39卷 406-412页

作者： Chenqi ZHANG~(1#), Desheng KONG~(2#), Xingang LIU~1, Xiaomin YAN~1, Linsen DAI~(1*), and Duan MA~(2*) 1 Center of Analysis and Measurement, Fudan University, Shanghai 200433, China 2 Key Laboratory of Molecular Medicine. Ministry of Education, Fudan University, Shanghai 200032, China Center of Analysis and Measurement Fudan UniversityShanghai 200433 China Key Laboratory of Molecular Medicine Ministry of Education Fudan UniversityShanghai 200032 China.

The conformation of Kunitz domain 1 of human tissue factor pathway inhibitor-2 (hTFPI-2/KD1) has been studied by Fourier transform infrared spectroscopy, circular dichroism, and Raman spectroscopy. It was found that hTFPI-2/KD1 contained approximately 17% s-helices, 24% β-strands, 46% random coils, 13% β-turns, and two kinds of disulfide bonds (ggg and tgt) at 25℃. The detailed conformational changes of the heated protein observed by Fourier transform infrared spectroscopy, circular dichroism and Raman spectroscopy revealed that hTFPI-2/KD1 was thermally stable. However, KD1 could form an intermediate form at high temperature, then return to its normal conformation when the temperature was lowered. Activity assays also showed that hTFPI-2/KD1 was able to keep its inhibitory activity on plasmin after being heated to 80℃ for 5min.

关键词： hTFPI-2/KD1 conformation disulfide bonds thermal stability structure and function

Addition of phenolic compounds to bread: antioxidant benefits and impact on food structure and sensory characteristics

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Food Production, Processing and Nutrition

Food Production, Processing and Nutrition 2021年第1期3卷 314-325页

作者： Yesica A.Czajkowska–González Emilio Alvarez–Parrilla Nina del Rocío Martínez–Ruiz Alma A.Vázquez–Flores Marcela Gaytán–Martínez Laura Ade la Rosa Departament of Chemical Biological Sciences Institute of Biomedical SciencesUniversidad Autónoma de Ciudad JuárezAnillo Envolvente del PRONAF y Estocolmos/nC.P.32310 Cd.JuárezMéxico Programa de Posgrado en Alimentos del Centro de la República(PROPAC) Research and Graduate Studies in Food ScienceSchool of ChemistryUniversidad Autónoma de QuerétaroCentro UniversitarioCerro de las Campanas S/NC.P.76010 Santiago de QuerétaroMexico

The use of flours or phenolic extracts obtained from non-traditional sources or agri-food industry by-products has been a strategy used to formulate new bakery products with characteristics of a functional food.However,phenolic compounds present great structural diversity,as well as the ability to interact in a complex way with the macromolecules that constitute the bread matrix.Therefore,the addition of these flours,extracts or pure compounds produces various effects on the microstructure of bread,and several of its sensory properties.This is mainly due to interactions between phenolic compounds and gluten proteins.The objective of this review is to analyze some of the most recent published works on the addition of phenolic compounds in wheat bread to identify the type of positive and negative effects that have been observed and how they can be related to the physicochemical interactions between phenolic compounds and the macromolecules that constitute the food matrix,mainly gluten.The effect of monomeric and polymeric phenolic compounds on the strength of these interactions and on the properties of dough and bread are discussed.

关键词： condensed tannins hydrolysable tannins phenolic acids gluten food rheology food texture protein-phenolic interactions disulfide bonds non-covalent interactions

Evidence for the Existence of Cross-Linked Intermediates during Unfolding and Refolding of CK in UGGE

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Tsinghua Science and Technology 2001年第3期6卷 206-211页

作者：王希成谢成杨建周海梦 Department of Biological Sciences and Biotechnology Tsinghua University Beijing 100084 China

Urea gradient gel electrophoresis (UGGE) is an important technique for studying the conformation changes of proteins during denaturation. This paper reports on an investigation of the unfolding and refolding of creatine kinase (CK) by UGGE. The native and denatured CK underwent electrophoresis in polyacrylamide gels containing a linear 08 mol/L gradient of urea perpendicular to the direction of migration. The results showed that unfolding and refolding of CK is a relatively rapid process. The denatured enzyme could refold to a conformation with activity during electrophoresis at low urea concentrations, indicating that denaturation in urea is reversible. More importantly, both the native and denatured CK were separated into multiple parallel bands through UGGE, but the bands decreased significantly when mercaptoethanol was added to the samples. The results suggest that various kinds of unfolding and refolding intermediates were formed during UGGE, which are assumed to be oligomers with disulfide bonds between peptide chains. Urea/SDS (sodium dodecylsulphate) polyacrylamide two dimensional electrophoresis proved that these unfolding and refolding intermediates formed during UGGE were oligomers which were composed of different number of subunits cross linked by disulfide bonds. The results indicate that the unfolding and refolding of CK are relatively rapid processes with some cross linked intermediates with disulfide bonds during unfolding and refolding of the enzyme. 

关键词： creatine kinase unfolding and refolding urea gradient gel electrophoresis intermediate disulfide bonds

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