高选择性钯基催化剂的制备及其在氯代苯酚加氢脱氯反应中的应用

发布时间：2018-06-25 03:16

  本文选题：加氢脱氯 + 氯酚　； 参考：《兰州大学》2017年硕士论文

【摘要】：氯酚类化合物由于高毒性、抗生物降解性和强生物累积性等性质,严重危害到环境与生物体健康,这类化合物的安全处理已成为日益关注环境保护的一个重要的研究领域。催化加氢技术(HDC)由于其处理过程比较干净、相对比较便宜和有效性可用于在环境温度或接近于环境温度下广泛浓度的污染物的处理,因此研究Pd基催化剂在氯代苯酚的加氢脱氯反应中的催化性能具有重要意义。在本论文中,以碳纳米管(CNTs)、三乙酰丙酮铁(Fe(acac)3)和正硅酸乙酯(TEOs)制备了磁性介孔的二氧化硅管(MSNTs);通过3-氨基三乙氧基硅烷(3-APTES)将其表面氨基功能化;利用浸渍法把金属Pd负载到氨基功能化的磁性介孔二氧化硅管上制备出Pd基催化剂(Pd@NH2-MSNTs)。通过透射电子显微镜(TEM)、X射线光电子能谱仪(XPS)、X射线衍射仪(XRD)、振动探针式磁强计(VSM)、傅里叶变换红外光谱仪(FT-IR)和氮气的吸脱附等对催化剂进行表征和分析。将Pd@NH2-MSNTs用于常压和液相中的氯酚类的加氢脱氯及过度加氢生成环己酮的反应中,系统地研究了催化剂用量、反应温度、碱和不同载体等因素对催化剂活性的影响。研究结果表明催化剂在氯酚的加氢脱氯反应中表现出良好的催化性能,在60℃、常压和水作为溶剂的反应条件下,反应物的转化率为100%,环己酮的选择性高达99%,相比于别的非均相催化剂的最终产物为苯酚,该催化剂一锅法制备了环己酮。同时该磁性催化剂在外加磁场的条件下能从反应体系中很方便的分离出来,并且经七次循环使用其活性没有明显下降。
[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，

本文编号：2064300