新型多金属氧酸盐催化剂的设计合成及催化过氧化氢氧化淀粉性能的研究

发布时间：2018-07-08 09:21

本文选题：生物质 + 淀粉　；参考：《东北师范大学》2017年硕士论文

【摘要】：近年来,人们对全球变暖以及化石燃料减少等问题的日益关注,促使科学家们不遗余力的研究以更绿色的、有效的、可持续发展的方式通过以可再生能源为原料加以一定的技术手段生产化学品和燃料。其中,生物质资源作为自然界中广泛存在的可再生资源,近年来全球科研工作者对其的研究热情与日俱增。淀粉是一种绿色可再生并大量存在的生物质资源,科研工作者们利用不同的技术手段对其进行变性处理后,可以按照人们的需求得到不同应用范围的变性淀粉。氧化淀粉是变性淀粉的一种,是由淀粉经过部分氧化而得到的,在日常生活以及不同行业生产中有着广泛的应用。在氧化淀粉多种的生产工艺中,以过氧化氢为氧化剂的绿色环保无污染的生产工艺被广泛的应用。近年来,多金属氧酸盐(POMs)因为其具有独特的化学催化活性以及绿色环保等特性而被广泛关注,亦被大量应用于化学催化领域。POMs具有很强的氧化还原性和强Br?nsted酸性,在生物质转化研究中有着重要的应用前景。基于此,本论文开展了以下工作:1、制备了H_5PMo_(10)V_2O40/MCM-41催化剂,通过ICP-AES、FT-IR、XRD、31P固体核磁、DR UV-Vis、TEM等测试方法对其组成和结构进行了分析表征。对PMo_(10)V_2/MCM-41催化过氧化氢氧化淀粉反应进行了系统研究,并通过优化反应确定最佳反应条件为:反应温度80°C;反应时间8 h;水含量2 mL;过氧化氢含量4.0 mL;催化剂用量为5 mg。在该反应条件下氧化程度高达0.58 mol CO2H per 100 g。催化效果较为理想,催化剂经过简单处理后亦可重复使用。2、制备了H_5PMo_(10)V_2O40/SBA-15催化剂,通过ICP-AES、FT-IR、XRD、31P固体核磁、DR UV-Vis、TEM等测试方法对其组成和结构进行了分析表征。对PMo_(10)V_2/SBA-15催化过氧化氢氧化淀粉反应进行了系统研究,并通过优化反应确定最佳反应条件为:反应温度80°C;反应时间9 h;过氧化氢使用量4.0 mL;水含量1.5 m L;催化剂用量为5 mg。在该反应条件下氧化程度高达0.59 mol CO2H per 100 g。催化效果较为理想,催化剂回收后亦可重复使用。3、合成了一种超分子化合物(H_3O)_2(HINA)_2[PMo_(11)VO_(40)].15.5H_2O。通过单晶X-射线结构分析确定了其结构。并通FT-IR、DR UV-Vis、热重分析等表征手段对其结构和性质进行了进一步的研究。对该超分子化合物作为催化过氧化氢氧化淀粉反应进行了系统研究,并通过优化反应确定最佳反应条件为:反应温度80°C,反应时间7 h,水含量2 m L,过氧化氢含量4.0 mL,催化剂用量为4 mg。在该反应条件下氧化程度高达0.60 mol CO2H per 100 g。催化效果十分理想.。
[Abstract]:In recent years, increasing attention to global warming and the reduction of fossil fuels has prompted scientists to spare no effort to study greener and more effective. The way of sustainable development is to produce chemical and fuel by using renewable energy as raw material. Among them, biomass resources, as a renewable resource widely existing in nature, have attracted increasing enthusiasm from researchers all over the world in recent years. Starch is a kind of green renewable and abundant biomass resources. After denaturing it with different technical means, researchers can get different range of modified starch according to people's needs. Oxidized starch is a kind of modified starch, which is obtained by partial oxidation of starch. It is widely used in daily life and production in different industries. In many production processes of oxidized starch, hydrogen peroxide as oxidant is widely used in green environmental protection and no pollution production. In recent years, polyoxometalates (poss) have been widely concerned because of their unique chemical catalytic activity and green environmental protection, and have been widely used in the field of chemical catalysis, such as strong redox and strong Brnsted acidity. It has an important application prospect in biomass conversion research. Based on this, the following work was carried out in this thesis: 1, HK5PMo10 / MCM-41 catalyst was prepared, and its composition and structure were analyzed and characterized by ICP-AESS-FT-IRT-XRDN31P solid state magnetic resonance (NMR) -DR UV-Vis-Tem method. The catalytic reaction of PMo10 / MCM-41 to oxidize starch by hydrogen peroxide was studied systematically. The optimum reaction conditions were determined as follows: reaction temperature 80 掳C; reaction time 8 h; water content 2 mL; hydrogen peroxide content 4.0 mL; amount of catalyst 5 mg. The oxidation degree was as high as 0.58 mol CO2H per 100g. H5PMo10 V _ 2O _ (10) V _ 2O _ (40) / SBA-15 catalyst was prepared, and its composition and structure were characterized by ICP-AESFT-IRT-XRD31P solid state NMR UV-Vis-TEM method. The catalytic reaction of PMo10 V _ (10) V _ 2O _ 2 / SBA-15 on the oxidation of starch with hydrogen peroxide was studied systematically. The optimum reaction conditions were determined as follows: reaction temperature 80 掳C; reaction time 9 h; hydrogen peroxide usage 4.0 mL; water content 1.5 mL; and catalyst dosage 5 mg. The oxidation degree was as high as 0.59 mol CO2H per 100g. A supramolecular compound (H _ s _ 3O) _ 2 (China) _ 2 [PMo_ (11) VO( 40)] .15.5H _ 2O was synthesized. The structure was determined by X-ray structure analysis of single crystal. The structure and properties of FT-IRN Dr were further studied by FTIR-IR-Dr and thermogravimetric analysis. The supramolecular compound was used as catalyst for the oxidation of starch by hydrogen peroxide. The optimum reaction conditions were determined as follows: reaction temperature 80 掳C, reaction time 7 h, water content 2 mL, hydrogen peroxide content 4.0 mL, catalyst dosage 4 mg. The oxidation degree was as high as 0.60 mol CO2H per 100g. The catalytic effect is very ideal.
【学位授予单位】：东北师范大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：O643.36;O636.12

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