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基于琥珀酸衍生物为单体的聚酯的合成与表征

高分子材料科学与工程 2019年第11期35卷 17-22页

作者：程正载周佳丽刘盼盼谢聪王云胡海曾胜丁玲 Mario Gauthier 武汉科技大学化学与化工学院精细有机化工与有机材料研究所湖北武汉430081 煤转化与新型炭材料湖北省重点实验室湖北武汉430081 湖北科技学院湖北省非动力核技术协同创新中心湖北咸宁437100

以1,4-环己二酮-2,5-二甲酸二甲酯(DMSS)为起始原料,采用两步法成功制备了2,5-二甲氧基对苯二甲酸二甲酯(DMDMT)。分别以DMDMT和不同碳链的脂肪二醇为单体,在三氧化二锑的催化作用下,采用熔融共聚酯交换法合成了4种由脂肪族二元醇-芳香... 详细信息

以1,4-环己二酮-2,5-二甲酸二甲酯(DMSS)为起始原料,采用两步法成功制备了2,5-二甲氧基对苯二甲酸二甲酯(DMDMT)。分别以DMDMT和不同碳链的脂肪二醇为单体,在三氧化二锑的催化作用下,采用熔融共聚酯交换法合成了4种由脂肪族二元醇-芳香族二元酸构成的聚酯。经过溶解、沉淀、离心等分离手段,得到目标聚酯a^d。通过红外光谱、核磁共振氢谱、凝胶渗透色谱、差示扫描量热分析和热重分析对其进行表征和分析。聚酯a^d的PDI在1.95~2.70之间,数均相对分子质量(Mn)在10000~15200之间。研究了聚合物中分子主链柔顺性对聚合物的热性能的影响,其中,聚酯a的熔点(Tm)较高,达到90℃,其初始分解温度(T5%)高达363℃;随着脂肪族碳链的碳数增加,所合成的聚酯a^d的熔点和初始分解温度(T5%)下降,这为新型脂肪族-芳香族聚酯的分子设计与合成提供了有益的参考。

关键词： 2,5-二甲氧基对苯二甲酸二甲酯脂肪族-芳香族聚酯热性能熔融共聚酯交换法

Engineering homologous platelet-rich plasma,platelet-rich plasma-derived exosomes,and mesenchymal stem cell-derived exosomes-based dual-crosslinked hydrogels as bioactive diabetic wound dressings

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Bioactive Materials 2023年第10期28卷 74-94页

作者： Bianza Moise Bakadia Abeer Ahmed Qaed Ahmed Lallepak Lamboni Zhijun Shi Biampata Mutu Mukole Ruizhu Zheng Mazono Pierre Mbang Bi Zhang Mario Gauthier Guang Yang Department of Biomedical Engineering College of Life Science and TechnologyHuazhong University of Science and TechnologyWuhan430074China College of Life Science and Technology Key Laboratory of Molecular Biophysics of MOEHuazhong University of Science and TechnologyWuhanChina Institut Sup´erieur des Techniques M´edicales de Lubumbashi LubumbashiCongo Department of Molecular Medicine Biochemistry UnitUniversity of Pavi127100Pavi1Italy e Institut National de Recherche Biom´edicale Minist`ere de la Sant´eCongo Department of Chemistry University of WaterlooWaterlooOntarioN2L 3G1Canada

The management of diabetic wounds remains a critical therapeutic challenge. Platelet-rich plasma (PRP) gel, PRP-derived exosomes (PRP-Exos), and mesenchymal stem cell-derived exosomes (MSC-Exos) have demonstrated therapeutic potential in wound treatment. Unfortunately, their poor mechanical properties, the short half-lives of growth factors (GFs), and the burst release of GFs and exosomes have limited their clinical applications. Furthermore, proteases in diabetic wounds degrade GFs, which hampers wound repair. Silk fibroin is an enzyme-immobilization biomaterial that could protect GFs from proteases. Herein, we developed novel dual-crosslinked hydrogels based on silk protein (SP) (sericin and fibroin), including SP@PRP, SP@MSC-Exos, and SP@PRP-Exos, to promote diabetic wound healing synergistically. SP@PRP was prepared from PRP and SP using calcium gluconate/thrombin as agonist, while SP@PRP-Exos and SP@MSC-Exos were derived from exosomes and SP with genipin as crosslinker. SP provided improved mechanical properties and enabled the sustained release of GFs and exosomes, thereby overcoming the limitations of PRP and exosomes in wound healing. The dual-crosslinked hydrogels displayed shear-induced thinning, self-healing, and eradication of microbial biofilms in a bone-mimicking environment. In vivo, the dual-crosslinked hydrogels contributed to faster diabetic wound healing than PRP and SP by upregulating GFs expression, down-regulating matrix metalloproteinase-9 expression, and by promoting an anti-NETotic effect, angiogenesis, and re-epithelialization. Hence, these dual-crosslinked hydrogels have the potential to be translated into a new generation of diabetic wound dressings.

关键词： Platelet-rich plasma(PRP) Exosomes(Exos) Silk protein Dual-crosslinked hydrogel Diabetic wound

Preparation of Nitrogen-doped Carbon Dots from Coke Powder as a Fluorescent Chemosensor for Selective and Sensitive Detection of Cr (Ⅵ)

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Journal of Wuhan University of Technology(Materials Science) 2022年第6期37卷 1096-1104页

作者：孟娟 LI Shiqian 丁玲 ZHOU Chuang JIANG Rui ZHANG Qingtian CHENG Zhengzai gauthier mario HU Ya 伍林 School of Chemistry and Chemical Engineering Hubei Provincial Key Laboratory for New Processes of Ironmaking and Steel makingWuhan University of Science and TechnologyWuhan 430081China Fujian Universities and Colleges Engineering Research Center of Modern Facility Agriculture of Fujian University Fujian Polytechnic Normal UniversityFuqing 350300China Chemistry Department University of WaterlooWaterlooOntarioN2L 3G1Canada

The nitrogen-doped carbon dots(N-CDs)were prepared by using coke powder as carbon source and one-step hydrothermal method.The N-CDs were studied as a fluorescent chemosensor for determining Cr(Ⅵ)in water.The selective,sensitive,reproducibility and stability of as-prepared N-CDs were investigated.The morphology,composition and properties of N-CDs were characterized by a series of methods.The fluorescence quenching of N-CDs by Cr(Ⅵ)was explored.The experimental results reveal that the obtained N-CDs have great hydrophilicity and strong luminescence properties,which demonstrates the successful doping of nitrogen into the CDs.The surface-active groups and emission wavelength range of CDs increase due to the electronegativity and electron donor effect of doping N atom.Furthermore,the N-CDs exhibit good photochemical properties for the detection of Cr(Ⅵ),including a wide linear range from 0.3 to 200μM(R^(2)=0.9935)and a low detection limit of 0.10μM at the signal-to-noise ratio of 3(S/N=3).Moreover,the N-CDs as a sensor was used successfully for Cr(Ⅵ)detection in real water samples with recovery rates of 99.9%-110.6%.This sensor also shows highly reproducibility and stability.The N-CDs fluorescent chemical sensor may be a potential candidate for applying in the field of other fluorescent chemical sensing,catalysis,photoelectric devices and other fields.

关键词： carbon dots nitrogen doping preparation fluorescence detection Cr(Ⅵ)

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可降解含氮聚酯的合成与性能

化工新型材料 2022年第4期50卷 283-286页

作者：熊景程正载陈俊 Wandji Djouonkep Lesly Dasilva Seigu William Mawuko 孙欣贾如艳袁贝贝 Mario Gauthier 武汉科技大学化学与化工学院精细有机化工与有机材料研究所武汉430081 煤转化与新型炭材料湖北省重点实验室武汉430081

以N-(羧甲基)甘氨酸和对苯二酚二(2-羟乙基)醚为主要原料,三氧化二锑为催化剂,采用熔融聚合法,合成聚[N-(羧甲基)甘氨酸-对苯二酚二(2-羟乙基)醚]酯(P1)。采用FT-IR、1H-NMR对聚酯P1结构进行了表征;采用GPC、DSC、TGA测试其分子量和热性... 详细信息

以N-(羧甲基)甘氨酸和对苯二酚二(2-羟乙基)醚为主要原料,三氧化二锑为催化剂,采用熔融聚合法,合成聚[N-(羧甲基)甘氨酸-对苯二酚二(2-羟乙基)醚]酯(P1)。采用FT-IR、1H-NMR对聚酯P1结构进行了表征;采用GPC、DSC、TGA测试其分子量和热性能;并采用自然掩埋法,对其在土壤中的降解性能进行了研究。GPC测试结果表明,该聚酯具有较高的分子量,Mn为41500g/mol。TG结果显示,该聚酯有良好的热稳定性,起始热分解温度高于333℃。在自然土壤环境下,聚酯P1经过两年的降解,分子量下降20%,降解性能好,具有良好发展前景。

关键词：含氮聚酯N-(羧甲基)甘氨酸可降解熔融聚合

Degradable Polyesters based on Oxygenated Fatty Acid Monomer

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Journal of Wuhan University of Technology(Materials Science) 2022年第4期37卷 753-759页

作者：程正载 LI Yi Lesly Dasilva Wandji Djouonkep ZENG Sheng WANG Huan WANG Linfeng CAI Shuanpu LIU Panpan HU Hai YANG Yingao LI Jiaqi QIN Jisong Mario Gauthier Research Institute of Fine Organic Chemicals&Organic Materials at School of Chemistry and Chemical Engineering Wuhan University of Science and TechnologyWuhan 430081China Coal Conversion and New Carbon Materials Hubei Key Laboratory Wuhan University of Science and TechnologyWuhan 430081China Department of Petroleum Engineering Applied Chemistry in Oil and Gas FieldsYangtze UniversityWuhan 430100China Department of Chemistry University of Waterloo200 University Avenue WestWaterlooOntario N2L3G1Canada

A series of degradable polyesters was synthesized via melt polymerization of 3,6-dioxaoctane-1,8-dioic acid and five different diols,catalyzed by antimony trioxide(Sb_(2)O_(3)).The polymers were characterized by FT-IR and ^(1)H NMR spectroscopy,gel permeation chromatography(GPC)and differential scanning calorimetry(DSC)analysis.The polydispersity index(PDI=M_(w)/M_(n))of the polyesters ranged from 1.55 to 1.99,the weight-average molecular weight(M_(w))from 1.8×10^(4) to 3.2×10^(4) Da,the melting point from 63 to 123℃,and the highest decomposition temperature observed was 363℃.The influence of the structure of the polymer chain on hydrolytic degradability was investigated with tests performed at three different values of pH.The findings obtained provide useful insight for the molecular design and the synthesis of degradable polyesters.

关键词： degradable polyesters melt polymerization thermal properties aliphatic-aromatic polyester

Lewis酸催化三组分合成喹啉-2,4-二羧酸酯类化合物

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湖南大学学报（自然科学版） 2018年第6期45卷 133-138页

作者：程正载王云谢聪唐然王涵鼎丁玲刘锋波颜晓潮朱三勇 Mario Gauthier 武汉科技大学化学与化工学院精细有机化工与有机材料研究所湖北武汉430081 湖北科技学院湖北省非动力核技术协同创新中心湖北咸宁437100 弗罗里达大学化学系盖恩斯威尔32611

采用价廉易得的无水三氯化铝、三氯化铁、氯化铜等Lewis酸催化取代芳胺、乙醛酸乙酯和丙酮酸甲酯三组分一步反应,高效合成了4个喹啉-2,4-二羧酸酯类化合物.产物通过柱层析分离纯化,并采用FT-IR、~1H NMR、^(13)C NMR和元素分析等手段进... 详细信息

采用价廉易得的无水三氯化铝、三氯化铁、氯化铜等Lewis酸催化取代芳胺、乙醛酸乙酯和丙酮酸甲酯三组分一步反应,高效合成了4个喹啉-2,4-二羧酸酯类化合物.产物通过柱层析分离纯化,并采用FT-IR、~1H NMR、^(13)C NMR和元素分析等手段进行了结构表征.探讨了反应机理和取代芳胺的分子结构对反应的影响规律,为该类新颖化合物的分子设计与合成方法提供参考.该方法具有原料廉价易得、反应条件温和、原子经济性高、产率高等优点.

关键词：芳胺乙醛酸乙酯丙酮酸甲酯 Lewis酸喹啉衍生物

Microwave Synthesis of CdTe/TGA Quantum Dots and Their Thermodynamic Interaction with Bovine Serum Albumin

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Journal of Wuhan University of Technology(Materials Science) 2016年第6期31卷 1408-1414页

作者：丁玲 PENG Zeze SHEN Weizhou LIU Tao CHENG Zhengzai gauthier mario 梁峰 School of Chemistry and Chemical Engineering Coal Conversion and New Carbon Materials Hubei Key Laboratory Wuhan University of Science and Technology Wuhan 430081 China School of Electrical and Eletronic Engineering Huazhong University of Seience and Technology Wuhan 430074 China epartment of Chemistry University of Waterloo Ontario N2L 3G1 Canada

The thioglycollic acid（TGA） as a capping agent, CdTe/TGA quantum dots（QDs） with excellent properties were synthesized under microwave irradiation. The TGA/Cd/Te molar ratios, reaction time, temperature and p H are the crucial factors for properties of QDs. The QDs were characterized by UVvis absorption and fluorescence spectra, transmission electron microscopy and Fourier transform infrared spectroscopy. The experimental results show that when the p H value is 11.5 and molar ratio of TGA：Cd：Te is 1.2：1：0.4 at 100 ℃ heating for 15 min, the resulted QDs exhibit a high fluorescence quantum yield of 78%. The fluorescence full width at half maximum（FHMW） of QDs is around 23 nm. The products are spherical with average size of 3-5 nm. There is a strong coordination effect between TGA and Cd2＋. Moreover, the results of interaction between as-made QDs and bovine serum albumin（BSA） suggest that the QDs-BSA binding reaction is a static quenching. The negative values of free energy（△G〈0） suggest that the binding process is spontaneous, △H〈0 and △S〈0 show that hydrogen bonds and van der Waals interactions play a major role in the binding reaction between QDs and BSA.

关键词： microwave synthesis Cd Te/TGA quantum dots bovine serum albumin interaction thermodynamics

SENP7 overexpression protects cancer cells from oxygen and glucose deprivation and associates with poor prognosis in colon cancer

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Genes & Diseases 2022年第6期9卷 1419-1422页

作者： Francisco Gallardo-Chamizo Nieves Lara-Urena Juan F.Correa-Vazquez Jose C.Reyes Benoit R.gauthier mario Garcia-Dominguez Cell Dynamics and Signaling Department CABIMERCSICUniversidad de Sevilla-Universidad Pablo de Olavide-Junta de AndaluciaSeville 41092Spain Genome Biology Department CABIMERCSIC-Universidad de Sevilla-Universidad Pablo de Olavide-Junta de AndaluciaSeville 41092Spain Cell Therapy and Regeneration Department CABIMERCSIC-Universidad de Sevilla-Universidad Pablo de Olavide-Junta de AndaluciaSeville 41092Spain Centro de Investigacion Biomedica en Red de Diabetes y Enfermedades Metabo´licas Asociadas(CIBERDEM) Madrid 28029Spain

To the Editor,Constricted oxygen and glucose supplies are common conditions that healthy cells following a stress such an ischemic insult as well as cancer cells within a solid tumor need to overcome in order to survive.These conditions are a serious challenge for cells,which accurately measure the impact to make a life or death decision.In cancer cells,aberrant gene expression and/or protein regulation,frequently linked to appearing mutations,may confer selective advantages to survive under these adverse conditions.In the past years,cumulative evidence indicates that protein modification by covalent attachment of the Small Ubiquitin-like MOdifier(SUMO)plays a role in cell survival after oxygen and glucose deprivation(OGD).

关键词： cancer deprivation colon

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基于含硫单体的可降解聚酯的表征与性能

精细石油化工 2021年第5期38卷 65-69页

作者：陈俊程正载熊景 Wandji Djouonkep Lesly Dasilva Siegu William Mawuko 孙欣贾如艳袁贝贝 Mario Gauthier 武汉科技大学化学与化工学院精细有机化工与有机材料研究所湖北武汉430081 煤转化与新型炭材料湖北省重点实验室湖北武汉430081

以硫代二丙酸和间苯二酚二(2-羟乙基)醚为主要原料,Sb2O3为催化剂,通过熔融缩聚法合成了聚(硫代二丙酸-间苯二酚二(2-羟乙基)醚)酯。采用FT-IR、1H NMR,对聚酯的结构进行了表征;采用GPC、DSC、TGA测试其相对分子质量和热性能;并采用自... 详细信息

以硫代二丙酸和间苯二酚二(2-羟乙基)醚为主要原料,Sb2O3为催化剂,通过熔融缩聚法合成了聚(硫代二丙酸-间苯二酚二(2-羟乙基)醚)酯。采用FT-IR、1H NMR,对聚酯的结构进行了表征;采用GPC、DSC、TGA测试其相对分子质量和热性能;并采用自然掩埋法,对其在土壤中的降解性能进行了考察。结果表明:该新型含硫聚酯数均相对分子质量和重均相对分子质量分别为12634 g/mol和19708 g/mol、热分解5%温度为351.7℃,热分解50%温度为401.5℃,熔点为99.12℃,ΔHm为90.12 J/g,且在自然土壤环境下经过24个月的降解,聚酯P的失重率达到9.3%,具有较好的降解性能。

关键词：硫代二丙酸聚(硫代二丙酸-间苯二酚二(2-羟乙基)醚)酯熔融缩聚可降解聚酯