In this work, a dual-catalyst bed reactor packed with the combination of hierarchical nanosheet HZSM-35 (Hi-NZ35) zeolite and CuZnAl catalyst was proposed to realize more efficient ethanol synthesis from dimethyl ether (DME) and syngas (CO+H₂). The nanosheet ZSM-35 (NZ35) zeolite was prepared via a direct hydrothermal synthesis route and the CuZnAl catalyst was prepared by co-precipitation method. Moreover, a series of Hi-NZ35_x zeolites were obtained from NZ35 zeolite by further treatment with varied NaOH aqueous solution using hydrothermal process (“x” means the NaOH solution concentration of 0.2-0.6 M). The catalysts properties, such as crystallinity, porosity, acidity, morphology and composition, were characterized by X-ray diffraction (XRD), N₂ adsorption-desorption, NH₃ temperature-programmed desorption (NH₃-TPD), H₂ temperature-programmed reduction (H₂-TPR), scanning electron microscope (SEM) and energy dispersive spectroscopy (EDS). It was found that Hi-NZ35_0.4 zeolite was more effective to obtain hierarchical porosity with mesopore volume up to 0.131 cm³ g⁻¹. For single DME carbonylation reaction, the NZ35 zeolite exhibited superior catalytic activity (32.2%) and stability compared with conventional ZSM-35 (CZ35) zeolite. Furthermore, improved catalytic activity (42.0%) was observed on Hi-NZ35_0.4 zeolite owing to its abundant mesoporous structure. This result revealed that the hierarchical porosity of zeolite could effectively promote the catalytic performance of zeolite for DME carbonylation reaction. For the ethanol synthesis using the optimized catalysts combination of Hi-NZ35_0.4 zeolite and CuZnAl catalyst, the DME conversion was about 47.2% with higher ethanol productivity of 840.2 mmol kg⁻¹ h⁻¹.

在这项工作中，提出了一种由分层纳米片HZSM-35（Hi-NZ35）沸石和CuZnAl催化剂组合填充的双催化剂床反应器，以实现由二甲醚（DME）和合成气（CO + H ₂）更加高效的乙醇合成。）。通过直接水热合成途径制备纳米片ZSM-35（NZ35）沸石，并通过共沉淀法制备CuZnAl催化剂。此外，通过使用水热法用变化的NaOH水溶液进一步处理从NZ35沸石获得一系列Hi-NZ35 _x沸石（“ x”表示0.2-0.6M的NaOH溶液浓度）。通过X射线衍射（XRD），N ₂表征了催化剂的性质，如结晶度，孔隙率，酸度，形态和组成。吸附-脱附，NH _3程序升温脱附（NH ₃ -TPD），H _2程序升温还原（H ₂ -TPR），扫描电子显微镜（SEM）和能量色散光谱（EDS）。结果发现，Hi-NZ35 _0.4沸石更有效地获得分级孔隙率，中孔体积最大为0.131 cm ³  g ^-1。对于单一DME羰基化反应，与传统的ZSM-35（CZ35）沸石相比，NZ35沸石具有优异的催化活性（32.2％）和稳定性。此外，在Hi-NZ35 _0.4上观察到改善的催化活性（42.0％）沸石由于其丰富的介孔结构。该结果表明，沸石的分级孔隙率可以有效地促进沸石对DME羰基化反应的催化性能。对于使用Hi-NZ35 _0.4沸石和CuZnAl催化剂的优化催化剂组合的乙醇合成，DME转化率为约47.2％，乙醇产率更高，为840.2 mmol kg ^-1  h ^-1。