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Nanochaperones Based on Hydrophobic Interaction and Coordination Inhibit Protein Misfolding and Fibrillation

Chinese Journal of Polymer Science 2024年第11期42卷 1710-1718,I0009页

作者： Hui Wang Lin-Lin Xu Lin-Qi Shi Ru-Jiang Ma key laboratory of Functional Polymer Materials of Ministry of Education Institute of Polymer ChemistryState Key Laboratory of Medicinal Chemical BiologyFrontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China Haihe laboratory of Sustainable chemical Transformations Tianjin300192China

Amyloidosis is characterized by the deposition of fibrillar aggregates,with a specific peptide or protein as the primary component,in affected tissues or *** proliferation and deposition of amyloid fibrils can cause organismal dysfunction and lethal pathological outcomes associated with *** this study,a nanochaperone(nChap-NA)was developed to inhibit protein misfolding and fibrillation by simulating the function of natural molecular *** nanochaperone was prepared by self-assembly of two block copolymers PEG-b-PCL and PCL-b-P(NIPAM-co-AANTA),which had a phase-separated surface consisting of hydrophobic PNIPAM microdomains with coordinative NTA(Zn)moieties and hydrophilic PEG *** hydrophobic interaction of the PNIPAM microdomain and the coordination of NTA(Zn)synergistically work together to effectively trap the amyloid monomer and block its fibrillation *** and human islet amyloid polypeptide(hIAPP)were used as model proteins to investigate the nanochaperone's inhibition of amyloid misfolding and *** was proved that the nanochaperone could stabilize the natural conformation of the trapped insulin and hIAPP,and effectively inhibit their *** vivo study demonstrated that the nanochaperone could effectively preserve the bioactivity of insulin and reduce the cytotoxicity caused by hIAPP *** study may provide a promising strategy for the prophylactic treatment of amyloidosis.

关键词： Nanochaperone Amyloidosis Insulin hIAPP Inhibit fibrillation

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An on-chip intestine-liver model for multiple drugs absorption and metabolism behavior simulation

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Science China Chemistry 2018年第2期61卷 236-242页

作者： Mingsha Jie Haifeng Lin Ziyi He Hanyang Liu Haifang Li Jin-Ming Lin state key laboratory of chemical Resource Engineering Beijing University of Chemical Technology Department of Chemistry Beijing Key Laboratory of Microanalytical Methods and Instrumentation Key Laboratory of Bioorganic Phosphorus Chemistry & Chemical Biology Ministry of Education Tsinghua University

A double-layer microfluidic chip integrated with a hollow fiber(HF)was developed to reconstitute the intestine-liver functionality for studying the absorption and metabolism of combination ***-2 cells were inoculated in the HF cavity at the top of the serpentine channel to simulate the intestinal tissue for drug absorption and transport studied,and Hep G2 cells,seeded in the bottom chamber,were used to mimic the liver for metabolism-related *** and dacarbazine were selected for combination drug therapy and its effects on cell viability,hepatotoxicity,and cell cycle arrest under drug-conditioned culture were *** results suggested that the combined concentration below-100μg/m L had no significant inhibitory effect on Hep G2 cell viability,and therefore Hep G2 cells maintained their drug metabolism *** the drug concentration was increased above 250μg/m L,Hep G2 cells underwent *** of metabolites by mass spectrometry proved the effective metabolism in the microchip *** dynamic,co-culture microchip successfully provided a podium for long-term observation of absorption,transport,and metabolism of combination drugs,and could be an effective in vitro simulation model for further clinical research.

关键词： intestine-liver model combination drug microchip metabolite behavior

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A Dynamic Covalent Bonding-based Nanoplatform for Intracellular Co-Delivery of Protein Drugs and Chemotherapeutics with Enhanced Anti-Cancer Effect

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Chinese Journal of Polymer Science 2024年第5期42卷 559-569,I0005页

作者： Sai-Nan Liu Jia-Hui Meng Li-Yun Cui Hua Chen Lin-Qi Shi Ru-Jiang Ma key laboratory of Functional Polymer Materials of Ministry of Education Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer MaterialsState Key Laboratory of Medicinal Chemical BiologyFrontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China Haihe laboratory of Sustainable chemical Transformations Tianjin300192China

Efficient intracellular delivery of protein drugs is critical for protein *** combination of protein drugs with chemotherapeutics represents a promising strategy in enhancing anti-cancer ***,co-delivery systems for efficient delivery of these two kinds of drugs are still lacking because of their different ***,we show a well-designed delivery system based on dynamic covalent bond for efficient intracellular co-delivery of ribonuclease A(RNase A)and doxorubicin(DOX).Two polymers,PEG-b-P(Asp-co-AspDA)and PAE-b-P(Asp-co-AspPBA),and two 2-acetylphenylboronic acid(2-APBA)-functionalized drugs,2-APBA-RNase A and 2-APBA-DOX,self-assemble into mixed-shell nanoparticles(RNase A/DOX@MNPs)via dynamic phenylboronic acid(PBA)-catechol bond between PBA and dopamine(DA)*** PBA-catechol bond endows the nanoparticles with high stability and excellent stimulus-responsive drug release *** the slight acidic environment at tumor tissue,RNase A/DOX@MNPs are positively charged,promoting their *** cellular uptake into endosome,further protonation of PAE chains leads to the rupture of endosomes because of the proton sponge effect and the cleavage of PBA-catechol bond promotes the release of two *** cytoplasm,the high level of GSH removed the modification of 2-APBA on *** restored RNase A and DOX show a synergistic and enhanced antic-cancer *** system may be a promising platform for intracellular co-delivery of protein drugs and chemotherapeutics.

关键词： Drug co-delivery Combination therapy Dynamic covalent bond

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Molecular Hydrogels with Esterase-like Activity

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Chinese Journal of Chemistry 2013年第4期31卷 494-500页

作者： Chengbiao Yang Huaimin Wang Dongxia Li Ling Wang state key laboratory of medicinal chemical biology and College of Pharmacy Nankai University Tianiin 300071 China College of Life Sciences Nankai University Tianjin 300071 China

The development of molecular hydrogels that can be applied for mimicking bioactive molecules attracts exten- sive interests of researchers in fields of self-assembly. In this study, we reported on several molecular hydrogels based on naphthylacetic acid-peptides containing L-histidine formed by the heating-cooling process. All hydrogels exhibited higher activity to hydrolyze 4-nitrophenyl acetate （4-NPA） than the free L-histidine probably due the high density of L-histidine residue at the surface of self-assembled nanofibers. To calculate the 4-NPA hydrolysis rates, the Michaelis-Menten enzyme kinetics model was made. Among these gels, the gel of Nap-GFFYGHY possesses the highest enzyme activity of making the ester bond cleavage, which is approximately 25 times higher than that of the control （free L-histidine and Nap-GFFYGYY）. These results indicate that molecular hydrogels with self-assembled nanofibers have great potential for the generation of self-assembled multivalent materials.

关键词： self-assembly hydrogel artificial enzyme

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Deciphering the role of ultra-low-loaded rhodium in NiFe-MIL-53 for superior oxygen evolution reaction

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Journal of Energy Chemistry 2025年第01期 77-86页

作者： Jinzhi Jia Jinhua Zhang Kailu Guo Lanyue Zhang Gening Du Hao You Junfeng Huang Mudong Tu Hua Li Yong Peng Wei Dou Cailing Xu state key laboratory of Applied Organic Chemistry College of Chemistry and Chemical Engineering School of Materials and Energy Lanzhou University College of Chemistry and chemical Engineering Luoyang Normal University

Designing highly active and stable electrocatalysts of oxygen evolution reaction （OER） is one of the crucial *** this study,a novel OER electrocatalyst,NiFe-MIL-53 modified with ultra-low rhodium（Rh@NiFe-MIL-53）,is successfully prepared via the hydrothermal ***-situ Raman spectroscopy and electrochemical impedance spectroscopy reveal that the doped Rh accelerates the phase transformation of NiFe-MIL-53 and the in-situ formed Rh@NiFeOOH is the actual active *** importantly,the enhanced reversibility of electrochemical reconstruction between NiFeOOH and NiFe（OH）2after doping Rh is beneficial for improving the electrochemical stability of the catalyst.X-ray photoelectron spectroscopy spectra show the strong electronic interaction between single-atom Rh and Ni/Fe in Rh@***,theoretical calculations confirm that the integration of single-atom Rh into the NiFeOOH successfully reduces the band gap,regulates the d-band center （εd）,accelerates the charge transfer,and optimizes the adsorption behavior of oxygen-containing intermediates,thereby lowering the energy barrier of rate-determining ***,the optimized Rh@NiFe-MIL-53 exhibits excellent OER activity （240 mV） with a small Tafel slope of 48.2 mV dec-1and long-term durability (over1270 h at 10 m A cm-2and 110 h at 200 mA cm-2).This work presents a new perspective on designing highly efficient OER electrocatalysts.

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Precursor-involved and Conversion Rate-controlled Self-assembly of a ＇Super Gelator＇ in Thixotropic Hydrogels for Drug Delivery

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Chinese Journal of Chemistry 2012年第8期30卷 1781-1787页

作者：区彩文王怀民杨志谋陈敏生 Guangzhou Medical University GuangzhouGuangdong 510182China state key laboratory of medicinal chemical biology and College of Life Sciences Nankai UniversityTianjin 300071China

Enzymatic hydrogelation is a totally different process to the heating-cooling gelation process, in which the pre- cursors of the gelators can be involved during the formation of self-assembled structures. Using thixotropic hy- drogels formed by a super gelator as our studied system, we demonstrated that the enzyme concentration/conversion rate of enzymatic reaction had a strong influence on the morphology of resulting self-assembled nanostructures and the property of resulting hydrogels. The principle demonstrated in this study not only helps to understand and elucidate the phenomenon of self-assembly triggered by enzymes in biological systems, but also offers a unique methodology to control the morphology of self-assembled structures for specific applications such as controlled drug re- lease.

关键词： self-assembly hydrogel enzymatic reaction

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Design, synthesis and systematic evaluation of all possible cyclic dinucleotides (CDNs) that activate human stimulator of interferon genes (STING) variants

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Science China Chemistry 2020年第4期63卷 534-545页

作者： Zheng-Hua Wang Can-Can Zhao Qiang-Zhe Zhang Chuan-Lin Wang Hang Zhang De-Jun Ma Da-Wei Wang Xin Wen Lu-Yuan Li Zhen Xi state key laboratory of Elemento-organic Chemistry Department of Chemical BiologyCollege of ChemistryNankai UniversityTianjin 300071China state key laboratory of medicinal chemical biology and College of Pharmacy Tianjin Key Laboratory of Molecular Drug ResearchNankai UniversityTianjin 300071China Collaborative Innovation Center of chemical Science and Engineering(Tianjin) Tianjin 300071China National Pesticide Engineering Research Center(Tianjin) Tianjin 300071China

Cyclic dinucleotides(CDNs) are known to activate stimulator of interferon genes(STING) and induce type I interferon responses, therefor possess great potentials to be of immunotherapeutic value for cancers and infectious diseases. However, the existence of different single nucleotide polymorphism(SNP) of human STING(hSTING) gene poses an obstacle to achieve broad-spectrum activation by CDNs. We reported here the design and synthesis of a total of 36 CDNs, representing all structural variations, that contain four bases(A, G, C, U) and two linkage directions(2′-5′-linked and 3′-5′-linked phosphodiester).Through systematic evaluation of IFN-β induction with a dual-luciferase reporter assay, we discovered that wild type hSTING and two isoforms(HAQ and AQ) showed strong response while hSTING-R232 H and R293 Q exhibited the relatively weak response to CDNs stimulation. For the first time, we found that the c[G(2′,5′)U(2′,5′)] showed excellent activity against all five hSTING variants even equivalent to the endogenous ligand c[G(2′,5′)A(3′,5′)]. Furthermore, we have also demonstrated that 3′-3′CDNs with two 3′-5′ phosphodiesters showed higher serum and hydrolase stability than 2′-2′ CDNs with two 2′-5′ phosphodiesters and 2′-3′ CDNs with one 2′-5′ and one 3′-5′ phosphodiester. It is very interesting to note that 2′-2′ CDNs has been found for the first time to show strong activity. These findings will stimulate our exploration for the new functional role of CDNs, and provide guidelines to design CDNs based hSTING targeted drugs.

关键词： cyclic dinucleotides(CDNs) stimulator of interferon genes(STING) pyrimidine CDNs interferonβ ecto-nucleotide pyrophosphatase/phosphodiesterase 1(ENPP1)

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Anti-Sca-1 antibody-functionalized vascular grafts improve vascular regeneration via selective capture of endogenous vascular stem/progenitor cells

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Bioactive Materials 2022年第10期7卷 433-450页

作者： He Wang Mengmeng Xing Weiliang Deng Meng Qian Fei Wang Kai Wang Adam C.Midgley Qiang Zhao state key laboratory of medicinal chemical biology Haihe Laboratory of Sustainable Chemical TransformationsKey Laboratory of Bioactive Materials(Ministry of Education)Frontiers Science Center for Cell ResponsesCollege of Life SciencesNankai UniversityTianjinChina

Small-diameter vascular grafts fabricated from synthetic biodegradable polymers exhibit beneficial mechanical properties but often face poor regenerative *** tissue engineering approaches have been employed to improve tissue regeneration in vascular grafts,but there remains a requirement for a new generation of synthetic grafts that can orchestrate the host response to achieve robust vascular *** stem/progenitor cells(SPCs)are mostly found in quiescent niches but can be activated in response to injury and participate in endothelium and smooth muscle regeneration during neo-artery ***,we developed a functional vascular graft by surface immobilization of stem cell antigen-1(Sca-1)antibody on an electrospun poly(ε-caprolactone)graft(PCL-Sca-1 Ab).PCL-Sca-1 Ab promoted capture and retainment of Sca-1+SPCs in *** rat abdominal aorta replacement models,PCL-Sca-1 Ab stimulated in vivo recruitment of Sca-1+SPCs,and drove SPCs differentiation towards vascular cell *** origin of infiltrated Sca-1+SPCs was further investigated using a bone marrow transplantation mouse model,which revealed that Sca-1+SPCs originating from the resident tissues and bone marrow contributed to rapid vascular regeneration of vascular *** data indicated that PCL-Sca-1 Ab vascular grafts may serve as a useful strategy to develop next generation cell-free vascular grafts.

关键词： Small-diameter vascular grafts Surface modification Stem cell antigen-1(Sca-1)antibody Vascular stem/progenitor cells(SPCs) Tissue regeneration

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Atractylenolide-I covalently binds to CYP11B2,selectively inhibits aldosterone synthesis, and improves hyperaldosteronism

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Acta Pharmaceutica Sinica B 2022年第1期12卷 135-148页

作者： Wenjuan Liu Zhenqiang Li Simeng Chu Xiaoyao Ma Xiaoying Wang Min Jiang Gang Bai state key laboratory of medicinal chemical biology College of Pharmacy and Tianjin Key Laboratory of Molecular Drug ResearchNankai UniversityTianjin 300353China Tianjin University of Traditional Chinese Medicine Tianjin 300193China

Hyperaldosteronism is a common disease that is closely related to endocrine hypertension and other cardiovascular diseases. Cytochrome P450 11 B2(CYP11 B2), an important enzyme in aldosterone(ALD) synthesis, is a promising target for the treatment of hyperaldosteronism. However, selective inhibitors targeting CYP11 B2 are still lacking due to the high similarity with CYP11 B1. In this study,atractylenolide-I(AT-I) was found to significantly reduce the production of ALD but had no effect on cortisol synthesis, which is catalyzed by CYP11 B1. chemical biology studies revealed that due to the presence of Ala320, AT-I is selectively bound to the catalytic pocket of CYP11 B2, and the C8/C9 double bond of AT-I can be epoxidized, which then undergoes nucleophilic addition with the sulfhydryl group of Cys450 in CYP11 B2. The covalent binding of AT-I disrupts the interaction between heme and CYP11 B2 and inactivates CYP11 B2, leading to the suppression of ALD synthesis;AT-I shows a significant therapeutic effect for improving hyperaldosteronism.

关键词： Aldosterone CYP11B2 Hyperaldosteronism Atractylenolide-I Selective inhibitor

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Photochemical and Electrochemical Carbon Dioxide Utilization with Organic Compounds

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Chinese Journal of Chemistry 2018年第7期36卷 644-659页

作者： Yu Cao Xing He Ning Wang Hong-Ru Li Liang-Nian He state key laboratory and Institute of Elemento-Organic Chemistry College of Chemistry Collaborative Innovation Center of Chemical Science and Engineering Nankai University Tianjin 300071 China state key laboratory of medicinal chemical biology and Tianjin key laboratory of Molecular Drug Research College of Pharmacy Nankai University Tianjin 300071 China

In the last few years, photochemical and electrochemical CO2 transformations have attracted increasing attention in response to topical interest in renewable energy and green chemistry. The present minireview offers an overview about the current approaches for the photochemical and electrochemical carbon dioxide fixation with organic compounds. Valuable products, including carboxylic acids and heterocyclic compounds, are accessible through carboxylation and carboxylative cyclization, respectively. In photochemical and electrochemical processes, photo- or electro-induced radical ions or other high-energy organic compounds are considered as key intermediates to react with CO2. Besides, activation of CO2 to produce radical anion has also been reported.

关键词： carbon dioxide carboxylative cyclization electrochemistry photocatalysis sustainable chemistry

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