采用柠檬酸为络合剂,溶胶-凝胶法制备系列CeO_2-CuO/ZnO/Al_2O_3,在3.0 MPa压力和220~230℃反应条件下,甲苯二胺(TDA)和乙烯催化合成二乙基甲苯二胺(DETDA)为探针反应,考察其催化性能,其中CeO_2掺杂量为3%,催化活性最高。通过X射线衍射(...采用柠檬酸为络合剂,溶胶-凝胶法制备系列CeO_2-CuO/ZnO/Al_2O_3,在3.0 MPa压力和220~230℃反应条件下,甲苯二胺(TDA)和乙烯催化合成二乙基甲苯二胺(DETDA)为探针反应,考察其催化性能,其中CeO_2掺杂量为3%,催化活性最高。通过X射线衍射(XRD)、傅里叶红外光谱(FT-IR)、差热重量分析法(DTG-DTA)、核磁氢谱1 H NMR对CeO_2-CuO/ZnO/Al_2O_3、DETDA、TDA进行检测和表征,揭示了它们的微观结构和内在规律性。XRD检测发现CeO_2掺杂量增多,CeO_2-CuO/ZnO/Al_2O_3衍射峰强度增强,提高了晶化程度,金属原子存在协同效应,增多了活性中心。FT-IR揭示了DETDA内部化学键键型,拥有甲基、亚甲基的多取代芳胺。DTG-DTA检测出的质量变化与热效应两种信息,DETDA的DTG-DTA曲线在66.0、271.0℃存在二个吸热峰,分别为氨基脱离苯环、DETDA的分解产生。通过1 H NMR对DETDA、TDA检测,得到DETDA、TDA的氢原子的数目分别为18和10,分子中各个氢核对应所归属的吸收峰,分别和它们分子式中的氢原子数目吻合。CeO_2-CuO/ZnO/Al_2O_3催化合成DETDA,反应条件温和,工艺流程简单,容易实现高效率和连续化工业生产,因此具有广阔的发展前景。展开更多
以φ3 mm Al2O3作为主载体,采用浸渍与焙烧工艺,制备水煤气低温变换催化剂:CuO+ZnO/CeO2/Al2O3.利用X射线衍射(XRD)、扫描电子显微镜(SEM)、Raman散射光谱分别对催化剂的化学组成、表面形貌以及表面元素键合状态进行表征;对催化剂的水...以φ3 mm Al2O3作为主载体,采用浸渍与焙烧工艺,制备水煤气低温变换催化剂:CuO+ZnO/CeO2/Al2O3.利用X射线衍射(XRD)、扫描电子显微镜(SEM)、Raman散射光谱分别对催化剂的化学组成、表面形貌以及表面元素键合状态进行表征;对催化剂的水煤气变换反应(WGSR)活性进行测试.在对催化剂表面形貌进行数据挖掘的基础上,利用复杂网络方法对催化剂的表面形貌进行网络建模,并对其网络拓扑参数和同步性进行了计算.计算结果表明,CuO+ZnO/CeO2/Al2O3表面形貌网络度分布具有幂律分布特征;在催化WGSR以后,催化剂表面形貌网络同步性有所增强.展开更多
CeO2/ZnO nanocatalysts were prepared from the coupling route of homogeneous precipita-tion with microemulsion and the impregnation method. The catalytic performance of these two kinds of catalysts on the oxidative cou...CeO2/ZnO nanocatalysts were prepared from the coupling route of homogeneous precipita-tion with microemulsion and the impregnation method. The catalytic performance of these two kinds of catalysts on the oxidative coupling of methane with carbon dioxide was tested and compared; the frac-tal behavior of the nanocatalysts was analyzed using fractal theory. The CeO2/ZnO nanocatalysts had much higher activity than the catalysts prepared by impregnation method. There was no regular relation-ship between the average size of CeO2/ZnO nanocatalysts and their catalytic performance; however, the conversion of methane increased with the increase of the fractal dimension of CeO2/ZnO nanocatalysts.展开更多
文摘采用柠檬酸为络合剂,溶胶-凝胶法制备系列CeO_2-CuO/ZnO/Al_2O_3,在3.0 MPa压力和220~230℃反应条件下,甲苯二胺(TDA)和乙烯催化合成二乙基甲苯二胺(DETDA)为探针反应,考察其催化性能,其中CeO_2掺杂量为3%,催化活性最高。通过X射线衍射(XRD)、傅里叶红外光谱(FT-IR)、差热重量分析法(DTG-DTA)、核磁氢谱1 H NMR对CeO_2-CuO/ZnO/Al_2O_3、DETDA、TDA进行检测和表征,揭示了它们的微观结构和内在规律性。XRD检测发现CeO_2掺杂量增多,CeO_2-CuO/ZnO/Al_2O_3衍射峰强度增强,提高了晶化程度,金属原子存在协同效应,增多了活性中心。FT-IR揭示了DETDA内部化学键键型,拥有甲基、亚甲基的多取代芳胺。DTG-DTA检测出的质量变化与热效应两种信息,DETDA的DTG-DTA曲线在66.0、271.0℃存在二个吸热峰,分别为氨基脱离苯环、DETDA的分解产生。通过1 H NMR对DETDA、TDA检测,得到DETDA、TDA的氢原子的数目分别为18和10,分子中各个氢核对应所归属的吸收峰,分别和它们分子式中的氢原子数目吻合。CeO_2-CuO/ZnO/Al_2O_3催化合成DETDA,反应条件温和,工艺流程简单,容易实现高效率和连续化工业生产,因此具有广阔的发展前景。
基金National Natural Science Foundation of China(21076206)Natural Basic Research Program of China(973 Program,2010CB732302)National High Technology Research and Development Program(863 Program,2011AA050706)
文摘以φ3 mm Al2O3作为主载体,采用浸渍与焙烧工艺,制备水煤气低温变换催化剂:CuO+ZnO/CeO2/Al2O3.利用X射线衍射(XRD)、扫描电子显微镜(SEM)、Raman散射光谱分别对催化剂的化学组成、表面形貌以及表面元素键合状态进行表征;对催化剂的水煤气变换反应(WGSR)活性进行测试.在对催化剂表面形貌进行数据挖掘的基础上,利用复杂网络方法对催化剂的表面形貌进行网络建模,并对其网络拓扑参数和同步性进行了计算.计算结果表明,CuO+ZnO/CeO2/Al2O3表面形貌网络度分布具有幂律分布特征;在催化WGSR以后,催化剂表面形貌网络同步性有所增强.
文摘CeO2/ZnO nanocatalysts were prepared from the coupling route of homogeneous precipita-tion with microemulsion and the impregnation method. The catalytic performance of these two kinds of catalysts on the oxidative coupling of methane with carbon dioxide was tested and compared; the frac-tal behavior of the nanocatalysts was analyzed using fractal theory. The CeO2/ZnO nanocatalysts had much higher activity than the catalysts prepared by impregnation method. There was no regular relation-ship between the average size of CeO2/ZnO nanocatalysts and their catalytic performance; however, the conversion of methane increased with the increase of the fractal dimension of CeO2/ZnO nanocatalysts.
