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Ni-Fe合金催化劑催化木質(zhì)素解聚

發(fā)布時(shí)間:2018-07-09 23:37

  本文選題:生物質(zhì) + 木質(zhì)素; 參考:《中國(guó)科學(xué)技術(shù)大學(xué)》2017年碩士論文


【摘要】:木質(zhì)素是來(lái)源于木質(zhì)纖維素的一種重要的可再生生物質(zhì)資源,可用于制備化學(xué)品和燃料。由于木質(zhì)素本身結(jié)構(gòu)的復(fù)雜性和穩(wěn)定使其難以有效利用。目前大量的制漿和造紙工業(yè)的木質(zhì)素沒(méi)有得到有效利用,僅有部分用于燃燒供能,造成了一定程度的環(huán)境污染。為了保護(hù)環(huán)境、實(shí)現(xiàn)可持續(xù)發(fā)展,催化轉(zhuǎn)化木質(zhì)素制備高附加值化學(xué)品成為了研究的熱點(diǎn)。木質(zhì)素轉(zhuǎn)化的研究眾多,但是進(jìn)展依然相對(duì)緩慢。目前主要的轉(zhuǎn)化方法包括堿催化解聚、酸催化解聚、熱化學(xué)轉(zhuǎn)化、加氫處理解聚,氧化解聚等。由于加氫處理解聚木質(zhì)素可以獲得低聚木質(zhì)素、酚類等有價(jià)值的化學(xué)品和制備烴類燃料,是目前研究的熱點(diǎn)和最有效的方法之一。但是,催化劑失活和解聚產(chǎn)物產(chǎn)率不高等依然是需要進(jìn)一步解決的問(wèn)題。木質(zhì)素主要由甲氧基苯丙醇單元組成,可以用于制備芳香化合物。因此,為了有效的解聚木質(zhì)素并保留芳香結(jié)構(gòu),我們制備了一系列的Ni-Fe/AC催化劑用于解聚木質(zhì)素。當(dāng)使用有機(jī)溶劑樺木木質(zhì)素被用于解聚時(shí),我們發(fā)現(xiàn)Ni1-Fe1/AC(Ni和Fe的比例為1:1)催化劑表現(xiàn)出了最好的催化效果。在225℃、2 MPa氫氣、6 h的反應(yīng)條件下,最高的單體產(chǎn)率可以達(dá)到23.2 wt%。GPC分析的結(jié)果也充分的證明了木質(zhì)素已經(jīng)獲得了有效的解聚。通過(guò)一系列的分析(XRD、HRTEM、H2-TPR和XPS表征),證明催化劑中存在鎳鐵和金的結(jié)構(gòu);谀P臀锏难芯,Ni1-Fe1/AC催化劑在醚鍵的氫解反應(yīng)中表現(xiàn)出了很高的反應(yīng)活性,并且能夠保留芳香環(huán)不被過(guò)度加氫,保留產(chǎn)物的芳向性。催化劑表現(xiàn)出的優(yōu)異的反應(yīng)活性可能要?dú)w因于鎳鐵合金結(jié)構(gòu)在催化過(guò)程中的協(xié)同效應(yīng)。將催化劑應(yīng)用于真實(shí)生物質(zhì)體系——樺木木屑的解聚反應(yīng)時(shí)也表現(xiàn)出了良好的反應(yīng)活性?偟膯误w產(chǎn)率可以達(dá)到39.5 wt%,并且PG和PS兩種產(chǎn)物的選擇性可以達(dá)到88%。
[Abstract]:Lignin is an important renewable biomass resource derived from lignocellulose, which can be used in the preparation of chemicals and fuels. Due to the complexity and stability of the lignin itself, the lignin is difficult to be used effectively. A certain degree of environmental pollution. In order to protect the environment and achieve sustainable development, catalytic conversion of lignin to the preparation of high value-added chemicals has become a hot spot. There are many studies on lignin conversion, but the progress is still relatively slow. The main methods of conversion include alkali catalytic depolymerization, acid catalytic depolymerization, thermochemical conversion, and hydrogenation treatment. Depolymerization, oxidative depolymerization, and so on. Due to the hydrogenation of depolymerization lignin to obtain oligomeric lignin, phenol and other valuable chemicals and the preparation of hydrocarbon fuels, it is one of the hotspots and most effective methods for the study. However, the problem that the deactivation of the catalyst and the yield of the depolymerization products are not high still need to be solved. The methoxy phenylpropanol unit can be used to prepare aromatic compounds. Therefore, in order to effectively depolymerization lignin and retain the aromatic structure, we have prepared a series of Ni-Fe/AC catalysts for depolymerization of lignin. When the use of organic solvents Betula lignin is used for depolymerization, we found that Ni1-Fe1/AC (the proportion of Ni and Fe is 1:1) catalysis. The best catalytic effect was shown. At 225 C, 2 MPa hydrogen and 6 h, the highest monomer yield could reach 23.2 wt%.GPC analysis. The results also proved that the lignin has been effectively depolymerization. A series of analysis (XRD, HRTEM, H2-TPR and XPS characterization) showed the presence of nickel iron and gold in the catalyst. Based on the study of the model, the Ni1-Fe1/AC catalyst shows a high reaction activity in the hydrosolution reaction of the ether bond, and can retain the aromatic ring not overhydrogenation and retain the aromatics of the product. The excellent activity of the catalyst may be attributed to the synergistic effect of the nickel iron alloy gold structure in the catalytic process. The chemical agent was also used in the depolymerization reaction of the real biomass system - birch wood chips. The total monomer yield can reach 39.5 wt%, and the selectivity of two products of PG and PS can reach 88%.
【學(xué)位授予單位】:中國(guó)科學(xué)技術(shù)大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:O643.36;O636.2

【參考文獻(xiàn)】

相關(guān)期刊論文 前4條

1 鄭明遠(yuǎn);龐紀(jì)峰;王愛(ài)琴;張濤;;纖維素直接催化轉(zhuǎn)化制乙二醇及其他化學(xué)品:從基礎(chǔ)研究發(fā)現(xiàn)到潛在工業(yè)應(yīng)用(英)[J];催化學(xué)報(bào);2014年05期

2 龍金星;徐瑩;王鐵軍;張興華;張琦;馬隆龍;李宇萍;;木質(zhì)素催化解聚與氫解[J];新能源進(jìn)展;2014年02期

3 宋奇;蔡嘉瑩;張俊杰;于維強(qiáng);王峰;徐杰;;Ni基催化劑上木質(zhì)素模型化合物苯基苯乙醚C O鍵的加氫裂解[J];催化學(xué)報(bào);2013年04期

4 趙冠鴻;鄭明遠(yuǎn);王愛(ài)琴;張濤;;磷化鎢催化轉(zhuǎn)化纖維素制乙二醇[J];催化學(xué)報(bào);2010年08期

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