超氧化物歧化酶及过氧化氢酶模拟物的研究

发布时间：2018-06-07 23:10

本文选题：超氧化物歧化酶模拟 + 过氧化氢酶模拟　；参考：《武汉工程大学》2015年硕士论文

【摘要】：超氧化物歧化酶和过氧化氢酶是人体内两种重要的抗氧化酶。可以有效的清除人体细胞代谢过程中产生的O2-·,·OH,H2O2等氧化物种。而人类代谢过程中产生的氧自由基等物种不能被及时清除会导致人体衰老和疾病的产生。因此将这些酶类应用到疾病治疗,延缓衰老,保健美容等方面上对人体的健康与幸福生活有具有重要意义。但是天然酶存在分子量大,细胞透过性差,易失活,提取困难,成本高的特点,因此合成具有天然抗氧化酶功能的模拟物变得尤为重要。将二氧化硅作为活性组分的载体,有望得到高活性,稳定性好,易回收的模拟物。本论文设计并合成了以二氧化硅纳米颗粒为核,以多胺及水杨醛希夫碱、甲硫氨酸希夫碱还原产物修饰其表面的纳米颗粒作为模拟物。首先探讨了用四乙氧基硅烷(TEOS)为原料在催化剂氨水作用下,反应条件如TEOS滴加速度、反应时间及溶剂的种类对形成的硅纳米颗粒尺寸和形貌的影响,接着以合成的纳米颗粒为核进行了下面的工作:(1)以3-氯丙基三乙氧基硅烷(ACTES)作为硅烷偶联剂,将二乙烯三胺(DETA)和三乙烯四胺(TETA)接枝到二氧化硅微球表面,再与Mn2+、Cu2+反应得到负载Mn2+、Cu2+的二氧化硅纳米颗粒。对该类型模拟物的SOD和CAT活性进行了研究,接枝DETA的纳米颗粒Si O2/ACTES/DETA/Mn2+和Si O2/ACTES/DETA/Cu2+的SOD活性单位IC50都为0.026 g·L-1,Si O2/ACTES/DETA/Mn2+的CAT活性初始反应速率为1.59′10-6,转化率为66%,Si O2/ACTES/DETA/Cu2+的CAT活性初始反应速率为6.7′10-7 mol(O2)·s-1,转化率为35%,接枝了TETA的纳米颗粒Si O2/ACTES/TETA/Mn2+的SOD活性单位IC50为0.007 g·L-1,Si O2/ACTES/TETA/Cu2+的SOD活性单位IC50为0.003 g·L-1,Si O2/ACTES/DETA/Mn2+的CAT活性初始反应速率为3.06′10-6,转化率为82%,Si O2/ACTES/DETA/Cu2+的CAT活性初始反应速率为1.56′10-6 mol(O2)·s-1,转化率为53%;(2)以3-氯丙基三乙氧基硅烷(ACTES)作为硅烷偶联剂,合成含Mn、Cu的水杨醛希夫碱修饰的二氧化硅纳米颗粒。对该类型模拟物SOD和CAT活性进行了研究,Si O2/ACTES/r-HL/Mn2+的SOD活性单位IC50为0.0051 g·L-1,Si O2/ACTES/r-HL/Cu2+的SOD活性单位IC50为0.0048 g·L-1,Si O2/ACTES/r-HL/Mn2+的CAT活性初始反应速率为2.17′10-6,转化率为85%,Si O2/ACTES/r-HL/Cu2+的CAT活性初始反应速率为1.03′10-6 mol(O2)·s-1,转化率为50%;(3)以3-氯丙基三乙氧基硅烷(ACTES)作为硅烷偶联剂,合成含Mn、Cu的甲硫氨酸希夫碱修饰的二氧化硅纳米颗粒。对该类型模拟物SOD和CAT活性进行了研究,ACTES/r-HL/Mn2+的SOD活性单位IC50为0.0041 g·L-1,ACTES/r-HL/Cu2+的SOD活性单位IC50为0.0012 g·L-1,ACTES/r-HL/Mn2+的CAT活性初始反应速率为3.53′10-6,转化率为90%,ACTES/r-HL/Cu2+的CAT活性初始反应速率为2.72′10-6mol(O2)·s-1,转化率为67%;本论文中对各步产物进行了IR,TGA,SEM及EDS等表征。比较并讨论了各种纳米颗粒模拟物活性的影响因素。结果表明:(1)用多胺将Mn、Cu负载于纳米颗粒上的模拟物同时具有SOD和CAT活性;(2)含Mn、Cu的水杨醛希夫碱修饰的二氧化硅纳米颗粒具有较高的SOD和CAT活性;(3)含Mn、Cu的甲硫氨酸希夫碱修饰的二氧化硅纳米颗粒同时具有SOD和CAT双活性。
[Abstract]:Superoxide dismutase (SOD) and catalase are two important antioxidant enzymes in the human body. They can effectively remove O2-, OH, H2O2 and other oxidizing species produced during the metabolic process of human cells, and the oxygen free radicals produced in human metabolism can not be removed in time and cause human aging and disease. Enzymes are of great significance to the health and happy life of the human body in the treatment of disease, delaying senility and health care. However, the natural enzyme has the characteristics of large molecular weight, poor cell transmission, easy to inactivate, difficult extraction and high cost. Therefore, it becomes particularly important to synthesize the mimics with the function of natural antioxidant enzymes. Two oxygen is used. As a carrier of active components, silicon carbide is expected to be highly active, stable and easy to recover. This paper has designed and synthesized nano particles with silica nanoparticles as core, polyamines and salicylaldehyde Schiff base and methionine Schiff base reduction products as the simulants. First, the four ethoxy silane was discussed. TEOS) the effect of the reaction conditions such as the acceleration of TEOS drop, the reaction time and the kind of solvent on the size and morphology of the formed silicon nanoparticles under the action of the catalyst ammonia water, and then the following work is carried out with the synthesized nanoparticles as the core: (1) the 3- chlorpropyl triethoxy silane (ACTES) is used as the silane coupling agent, and the two ethylene three amine is used. (DETA) and three ethylene four amine (TETA) grafted onto the surface of silica microspheres, and then reacted with Mn2+ and Cu2+ to obtain the silica nanoparticles loaded with Mn2+ and Cu2+. The activity of SOD and CAT of this type of analogue was studied. The grafting DETA nanoparticles Si O2/ACTES/DETA/Mn2+ and Si activated units were 0.026 The initial reaction rate of CAT activity of Si O2/ACTES/DETA/Mn2+ is 1.59 '10-6, the conversion rate is 66%. The initial reaction rate of CAT activity of Si O2/ACTES/DETA/Cu2+ is 6.7' 10-7 mol (O2) s-1, and the conversion rate is 35%. The unit IC50 was 0.003 G. L-1, the initial reaction rate of CAT activity of Si O2/ACTES/DETA/Mn2+ was 3.06 '10-6, the conversion rate was 82%, the initial reaction rate of CAT activity of Si O2/ACTES/DETA/Cu2+ was 1.56' 10-6 mol (O2). The conversion rate was 53%. (2) chlorpropyl triethoxylsilane was used as silane coupling agent to synthesize salicylaldehyde Schiff The activity of SOD and CAT in this type of analogue was studied. The SOD active unit IC50 of Si O2/ACTES/r-HL/Mn2+ was 0.0051 G. L-1. The SOD active unit IC50 of Si O2/ACTES/r-HL/Cu2+ was 0.0048. The initial reaction rate was 2.17 '10-6 and the conversion rate was 85%. The initial reaction rate of CAT activity of TES/r-HL/Cu2+ was 1.03 '10-6 mol (O2). S-1 and the conversion rate was 50%. (3) 3- chloro propyl triethoxy silane (ACTES) was used as silane coupling agent to synthesize silica nanoparticles modified by methionine Schiff base containing Mn and Cu. The SOD and CAT activities of this type of mimics were studied. The sex unit IC50 is 0.0041 G. L-1, and the SOD active unit IC50 of ACTES/r-HL/Cu2+ is 0.0012 G. L-1. The initial reaction rate of ACTES/r-HL/Mn2+'s CAT activity is 3.53 '10-6, the conversion rate is 90%, ACTES/r-HL/Cu2+ CAT activity initial reaction rate is 2.72'. The conversion rate is 67%. S and other characterization. Compare and discuss the influence factors of the activity of various nano particle simulants. The results show: (1) the mimics of Mn, Cu loaded on the nanoparticles with polyamines have both SOD and CAT activity simultaneously; (2) the silica nanoparticles containing the salicylaldehyde Schiff base containing Mn and Cu have higher SOD and CAT activity; (3) Mn, Cu methionine Schiff base modified silica nanoparticles also have SOD and CAT double activity.
【学位授予单位】：武汉工程大学
【学位级别】：硕士
【学位授予年份】：2015
【分类号】：O613.72;TB383.1

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