本文選題：當(dāng)歸內(nèi)酯 + 雙金屬催化劑�。� 參考：《華東師范大學(xué)》2017年碩士論文

【摘要】：在多相催化反應(yīng)過程中使用負(fù)載型雙金屬催化劑通�？梢垣@得高于單金屬的原子經(jīng)濟(jì)性和高活性。在生物質(zhì)轉(zhuǎn)化中,α-當(dāng)歸內(nèi)酯(α-AL)作為一種新的生物質(zhì)平臺化合物,可用于制備多種具有應(yīng)用前景的化合物。本文圍繞α-AL加氫制備伽馬戊內(nèi)酯(GVL)的高效催化劑開展研究,考察了 Pd-NiO(Ni)雙金屬催化劑的結(jié)構(gòu)及組成等因素對加氫活性的影響,論文主要包括如下內(nèi)容:1、制備了一系列不同Ni負(fù)載量(2-40wt.%)的NiO/SiO2材料、并負(fù)載微量Pd(0.2 wt.%),考察了 NiO負(fù)載量及Ni物種價態(tài)在αα-當(dāng)歸內(nèi)酯釜式加氫反應(yīng)中的構(gòu)效關(guān)系。結(jié)果表明Pd-xNiO/SiO2系列催化劑可以在溫和條件下(室溫,0.3 MPa氫氣)高活性高選擇性催化α-AL加氫至GVL。在Ni負(fù)載量高于2%的Pd-xNi/SiO2催化劑中大量金屬Ni的存在抑制了 Pd納米粒子的加氫活性。Pd和NiO緊密結(jié)合形成的多相結(jié)構(gòu)為加氫活性中心。2、合成了一系列不同粒徑的NiO/SiO2載體,系統(tǒng)研究了不同Ni價態(tài)、粒徑的載體材料負(fù)載Pd后得到的Pd-NiO(Ni)雙金屬催化劑在不同溶劑中對于α-AL在固定床裝置加氫反應(yīng)的活性。結(jié)果表明,Pd-NiO/SiO2系列催化劑在H20和四氫呋喃(THF)中都表現(xiàn)出高加氫活性和穩(wěn)定性,并且表面的NiO表現(xiàn)出良好的抗積碳能力。通過在反應(yīng)器中原位還原獲得的Pd-Ni/SiO2在THF溶劑中隨著反應(yīng)的進(jìn)行而逐漸失活,催化劑活性降低程度和Ni的粒徑大小密切相關(guān)。相比較而言,雙金屬催化劑在水相體系中表現(xiàn)出良好的穩(wěn)定性。H2O作為一種綠色溶劑比非質(zhì)子溶劑THF在該反應(yīng)中具有更好的應(yīng)用前景。
[Abstract]:The atom economy and high activity of supported bimetallic catalyst are usually higher than that of single metal in heterogeneous catalytic reaction.偽 -Angelica lactone (偽 -ALL), as a new biomass platform compound, can be used to prepare many promising compounds in biomass conversion.In this paper, the efficient catalyst for the preparation of gamma-pentanolactone (GVLL) from 偽 -AL hydrogenation was studied. The effects of the structure and composition of Pd-NiO- Ni) bimetallic catalyst on the hydrogenation activity were investigated.The main contents of this paper are as follows: 1. A series of NiO/SiO2 materials with different Ni loading amounts (2-40wt.t) have been prepared, and a small amount of Pd(0.2 wt. has been loaded. The structure-activity relationships of the NiO loading amount and the valence state of Ni species in 偽 -Angelica lactone hydrogenation reaction have been investigated.The results show that Pd-xNiO/SiO2 series catalysts can catalyze the hydrogenation of 偽 -AL to GVL under mild conditions (0. 3 MPa hydrogen at room temperature) with high activity and high selectivity.The presence of a large amount of metal Ni in the Pd-xNi/SiO2 catalyst with Ni loading of more than 2% inhibited the hydrogenation activity of PD nanoparticles. The multiphase structure formed by the close combination of PD and NiO was formed as the hydrogenation active center. A series of NiO/SiO2 carriers with different particle sizes were synthesized.The activity of Pd-NiO- Ni) bimetallic catalysts with different Ni valence and particle size for 偽 -AL hydrogenation in fixed bed was studied in different solvents.The results showed that Pd-NiO / Sio _ 2 series catalysts exhibited high hydrogenation activity and stability in H20 and THF, and the surface NiO exhibited good resistance to carbon deposition.The Pd-Ni/SiO2 obtained by in situ reduction in the reactor was gradually deactivated in THF solvent, and the decrease of catalyst activity was closely related to the particle size of Ni.In comparison, the bimetallic catalyst exhibited good stability in aqueous system. H2O as a green solvent had a better application prospect than the non-proton solvent THF in the reaction.
【學(xué)位授予單位】：華東師范大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2017
【分類號】：O621.251

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