Zhang Yali, Xie Xianglin, Yang Yunhan, Pal Manas, Dong Chen Xiao, Wu Zhangxiong
Particle Engineering Laboratory, School of Chemical and Environmental Engineering, and Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou City, Jiangsu Province 215123, People's Republic of China.
Department of Chemistry, School of Science, Indrashil University, Rajpur, Mehsana 382715, Gujarat, India.
J Colloid Interface Sci. 2024 Jun;663:749-760. doi: 10.1016/j.jcis.2024.02.180. Epub 2024 Feb 28.
Mesoporous aluminosilicates Al-SBA-15 with large pore sizes and suitable acid properties are promising substitutes to zeolites for catalytic cracking of bulky hydrocarbons without molecular diffusion limitation. The conventional processes to synthesize Al-SBA-15 are time-consuming and often suffer from low "framework" Al contents. Herein, Al-SBA-15 microspheres are synthesized using the rapid and scalable microfluidic jet spray drying technique. They possess uniform particle sizes (45-60 μm), variable surface morphologies, high surface areas (264-340 m/g), uniform mesopores (3.8-4.9 nm) and rich acid sites (126-812 μmol/g) and high acid strength. Their physicochemical properties are compared with the counterparts synthesized using traditional hydrothermal and evaporation-induced self-assembly methods. The spray drying technique results in a higher incorporation of aluminum (Al) atoms into the silica "framework" compared to the other two methods. The catalytic cracking efficiencies of 1,3,5-triisopropylbenzene (TIPB) on the Al-SBA-15 materials synthesized using the three different methods and nanosized ZSM-5 are compared. The optimal spray-dried Al-SBA-15 exhibits the best performance with 100 % TIPB conversion, excellent selectivity (about 75 %) towards the formation of deeply cracked products (benzene and propylene) and high stability. The catalytic performances of the spray-dried Al-SBA-15 with varying Si/Al ratios are also compared. The reasons for the different performances of the different materials are discussed, where the mesopores, high acid density and strength are observed to play the most critical role. This work might provide a basis for the synthesis of mesoporous rich metal-substituted silica materials for different catalytic applications.
具有大孔径和合适酸性的介孔硅铝酸盐Al-SBA-15是很有前景的沸石替代物,可用于催化裂解大分子烃而不受分子扩散限制。传统的合成Al-SBA-15的方法耗时且常常存在“骨架”铝含量低的问题。在此,采用快速且可扩展的微流控喷射喷雾干燥技术合成了Al-SBA-15微球。它们具有均匀的粒径(45 - 60μm)、可变的表面形态、高比表面积(264 - 340 m²/g)、均匀的介孔(3.8 - 4.9 nm)、丰富的酸位点(126 - 812 μmol/g)和高酸强度。将它们的物理化学性质与使用传统水热法和蒸发诱导自组装法合成的对应物进行了比较。与其他两种方法相比,喷雾干燥技术导致更多的铝(Al)原子掺入二氧化硅“骨架”中。比较了使用三种不同方法合成的Al-SBA-15材料以及纳米ZSM-5对1,3,5-三异丙基苯(TIPB)的催化裂解效率。最佳的喷雾干燥Al-SBA-15表现出最佳性能,TIPB转化率为100%,对深度裂解产物(苯和丙烯)的形成具有优异的选择性(约75%)和高稳定性。还比较了不同Si/Al比的喷雾干燥Al-SBA-15的催化性能。讨论了不同材料性能不同的原因,其中介孔、高酸密度和强度被认为起着最关键的作用。这项工作可能为合成用于不同催化应用的富含介孔的金属取代二氧化硅材料提供基础。