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高選擇性鈀基催化劑的制備及其在氯代苯酚加氫脫氯反應(yīng)中的應(yīng)用

發(fā)布時間:2018-06-25 03:16

  本文選題:加氫脫氯 + 氯酚; 參考:《蘭州大學(xué)》2017年碩士論文


【摘要】:氯酚類化合物由于高毒性、抗生物降解性和強生物累積性等性質(zhì),嚴重危害到環(huán)境與生物體健康,這類化合物的安全處理已成為日益關(guān)注環(huán)境保護的一個重要的研究領(lǐng)域。催化加氫技術(shù)(HDC)由于其處理過程比較干凈、相對比較便宜和有效性可用于在環(huán)境溫度或接近于環(huán)境溫度下廣泛濃度的污染物的處理,因此研究Pd基催化劑在氯代苯酚的加氫脫氯反應(yīng)中的催化性能具有重要意義。在本論文中,以碳納米管(CNTs)、三乙酰丙酮鐵(Fe(acac)3)和正硅酸乙酯(TEOs)制備了磁性介孔的二氧化硅管(MSNTs);通過3-氨基三乙氧基硅烷(3-APTES)將其表面氨基功能化;利用浸漬法把金屬Pd負載到氨基功能化的磁性介孔二氧化硅管上制備出Pd基催化劑(Pd@NH2-MSNTs)。通過透射電子顯微鏡(TEM)、X射線光電子能譜儀(XPS)、X射線衍射儀(XRD)、振動探針式磁強計(VSM)、傅里葉變換紅外光譜儀(FT-IR)和氮氣的吸脫附等對催化劑進行表征和分析。將Pd@NH2-MSNTs用于常壓和液相中的氯酚類的加氫脫氯及過度加氫生成環(huán)己酮的反應(yīng)中,系統(tǒng)地研究了催化劑用量、反應(yīng)溫度、堿和不同載體等因素對催化劑活性的影響。研究結(jié)果表明催化劑在氯酚的加氫脫氯反應(yīng)中表現(xiàn)出良好的催化性能,在60℃、常壓和水作為溶劑的反應(yīng)條件下,反應(yīng)物的轉(zhuǎn)化率為100%,環(huán)己酮的選擇性高達99%,相比于別的非均相催化劑的最終產(chǎn)物為苯酚,該催化劑一鍋法制備了環(huán)己酮。同時該磁性催化劑在外加磁場的條件下能從反應(yīng)體系中很方便的分離出來,并且經(jīng)七次循環(huán)使用其活性沒有明顯下降。
[Abstract]:Because of its high toxicity, biodegradability and strong bioaccumulation, chlorophenol compounds seriously harm to the environment and biological health. The safe treatment of these compounds has become an important research field of environmental protection. The catalytic hydrogenation (HDC) process is relatively inexpensive and efficient because of its cleaner treatment process, which can be used for the treatment of pollutants with a wide range of concentrations at or near ambient temperatures. Therefore, it is of great significance to study the catalytic performance of PD based catalyst in chlorophenol hydrodechlorination. In this thesis, magnetic mesoporous silicon dioxide (MSNTs) was prepared from carbon nanotubes (CNTs), ferric triacetylacetone (Fe (acac) 3) and tetraethyl orthosilicate (TEOs), and its surface was functionalized by 3-aminotriethoxy silane (3-APTES). PD based catalyst (PdNH2-MSNTs) was prepared by impregnating the metal onto the magnetic mesoporous silica tube. The catalysts were characterized and analyzed by transmission electron microscopy (TEM) X-ray photoelectron spectroscopy (XPS) X-ray diffraction (XRD) vibratory probe magnetometer (VSM) Fourier transform infrared spectroscopy (FT-IR) and nitrogen adsorption and desorption. PD @ NH2-MSNTs were used in hydrodechlorination and excessive hydrogenation of chlorophenols to produce cyclohexanone at atmospheric pressure and liquid phase. The effects of catalyst dosage, reaction temperature, alkali and different supports on the catalytic activity were systematically studied. The results show that the catalyst has good catalytic performance in the hydrodechlorination of chlorophenol, under the conditions of 60 鈩,

本文編號:2064300

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