Ke Quanli, Sun Tianjun, Wei Xiaoli, Guo Ya, Wang Shudong
Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian, 116023, P. R. China.
University of Chinese Academy of Sciences, 19A Yuquan Road, Beijing, 100049, P. R. China.
ChemSusChem. 2017 Nov 9;10(21):4207-4214. doi: 10.1002/cssc.201701162. Epub 2017 Oct 17.
Boron and copper heteroatoms were successfully incorporated into the frameworks of high-silica RHO zeolite by adopting a bulky alkali-metal-crown ether (AMCE) complex as the template. These heteroatom-doped zeolites show both larger micropore surface areas and volumes than those of their aluminosilicate analogue. Proton-type RHO zeolites were then applied for the separation of CO /CH /N mixtures, as these zeolites have weaker electric fields and, thus, lower heats of adsorption. The adsorption results showed that a balance between working capacity and adsorption heat could be achieved for these heteroatom-doped zeolites. Ideal adsorbed solution theory predictions indicate that these zeolites should have high selectivities even for remarkably dilute sources of CO . Finally, the heteroatom-substituted zeolites, especially the boron-substituted one, could be thermally regenerated rapidly at 150 °C after full hydration and maintained high regenerability for up to 30 cycles; therefore, they are potential candidates for trace CO removal under humid conditions.
通过采用大体积碱金属冠醚(AMCE)配合物作为模板,硼和铜杂原子成功地掺入到高硅RHO沸石骨架中。这些杂原子掺杂的沸石比其铝硅酸盐类似物具有更大的微孔表面积和体积。质子型RHO沸石随后被应用于CO/CH/N混合物的分离,因为这些沸石具有较弱的电场,因此吸附热较低。吸附结果表明,这些杂原子掺杂的沸石可以在工作容量和吸附热之间实现平衡。理想吸附溶液理论预测表明,即使对于非常稀的CO源,这些沸石也应该具有高选择性。最后,杂原子取代的沸石,尤其是硼取代的沸石,在完全水合后可以在150℃下快速热再生,并在高达30个循环中保持高再生性;因此,它们是潮湿条件下痕量CO去除的潜在候选材料。