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新型多金屬氧酸鹽催化劑的設(shè)計(jì)合成及催化過氧化氫氧化淀粉性能的研究

發(fā)布時間:2018-07-08 09:21

  本文選題:生物質(zhì) + 淀粉 ; 參考:《東北師范大學(xué)》2017年碩士論文


【摘要】:近年來,人們對全球變暖以及化石燃料減少等問題的日益關(guān)注,促使科學(xué)家們不遺余力的研究以更綠色的、有效的、可持續(xù)發(fā)展的方式通過以可再生能源為原料加以一定的技術(shù)手段生產(chǎn)化學(xué)品和燃料。其中,生物質(zhì)資源作為自然界中廣泛存在的可再生資源,近年來全球科研工作者對其的研究熱情與日俱增。淀粉是一種綠色可再生并大量存在的生物質(zhì)資源,科研工作者們利用不同的技術(shù)手段對其進(jìn)行變性處理后,可以按照人們的需求得到不同應(yīng)用范圍的變性淀粉。氧化淀粉是變性淀粉的一種,是由淀粉經(jīng)過部分氧化而得到的,在日常生活以及不同行業(yè)生產(chǎn)中有著廣泛的應(yīng)用。在氧化淀粉多種的生產(chǎn)工藝中,以過氧化氫為氧化劑的綠色環(huán)保無污染的生產(chǎn)工藝被廣泛的應(yīng)用。近年來,多金屬氧酸鹽(POMs)因?yàn)槠渚哂歇?dú)特的化學(xué)催化活性以及綠色環(huán)保等特性而被廣泛關(guān)注,亦被大量應(yīng)用于化學(xué)催化領(lǐng)域。POMs具有很強(qiáng)的氧化還原性和強(qiáng)Br?nsted酸性,在生物質(zhì)轉(zhuǎn)化研究中有著重要的應(yīng)用前景;诖,本論文開展了以下工作:1、制備了H_5PMo_(10)V_2O40/MCM-41催化劑,通過ICP-AES、FT-IR、XRD、31P固體核磁、DR UV-Vis、TEM等測試方法對其組成和結(jié)構(gòu)進(jìn)行了分析表征。對PMo_(10)V_2/MCM-41催化過氧化氫氧化淀粉反應(yīng)進(jìn)行了系統(tǒng)研究,并通過優(yōu)化反應(yīng)確定最佳反應(yīng)條件為:反應(yīng)溫度80°C;反應(yīng)時間8 h;水含量2 mL;過氧化氫含量4.0 mL;催化劑用量為5 mg。在該反應(yīng)條件下氧化程度高達(dá)0.58 mol CO2H per 100 g。催化效果較為理想,催化劑經(jīng)過簡單處理后亦可重復(fù)使用。2、制備了H_5PMo_(10)V_2O40/SBA-15催化劑,通過ICP-AES、FT-IR、XRD、31P固體核磁、DR UV-Vis、TEM等測試方法對其組成和結(jié)構(gòu)進(jìn)行了分析表征。對PMo_(10)V_2/SBA-15催化過氧化氫氧化淀粉反應(yīng)進(jìn)行了系統(tǒng)研究,并通過優(yōu)化反應(yīng)確定最佳反應(yīng)條件為:反應(yīng)溫度80°C;反應(yīng)時間9 h;過氧化氫使用量4.0 mL;水含量1.5 m L;催化劑用量為5 mg。在該反應(yīng)條件下氧化程度高達(dá)0.59 mol CO2H per 100 g。催化效果較為理想,催化劑回收后亦可重復(fù)使用。3、合成了一種超分子化合物(H_3O)_2(HINA)_2[PMo_(11)VO_(40)].15.5H_2O。通過單晶X-射線結(jié)構(gòu)分析確定了其結(jié)構(gòu)。并通FT-IR、DR UV-Vis、熱重分析等表征手段對其結(jié)構(gòu)和性質(zhì)進(jìn)行了進(jìn)一步的研究。對該超分子化合物作為催化過氧化氫氧化淀粉反應(yīng)進(jìn)行了系統(tǒng)研究,并通過優(yōu)化反應(yīng)確定最佳反應(yīng)條件為:反應(yīng)溫度80°C,反應(yīng)時間7 h,水含量2 m L,過氧化氫含量4.0 mL,催化劑用量為4 mg。在該反應(yīng)條件下氧化程度高達(dá)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 擄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 擄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 擄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.
【學(xué)位授予單位】:東北師范大學(xué)
【學(xué)位級別】:碩士
【學(xué)位授予年份】:2017
【分類號】:O643.36;O636.12

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