State Environmental Protection Key Laboratory of Eco-Industry, Northeastern University, Shenyang, 110819, China.
National Frontiers Science Center for Industrial Intelligence and Systems Optimization, Northeastern University, Shenyang, 110819, China.
Environ Sci Pollut Res Int. 2024 Jul;31(35):48014-48026. doi: 10.1007/s11356-024-33959-7. Epub 2024 Jul 17.
Under the background of the continuous rise of CO annual emissions, the development of CO capture and utilization technology is urgent. This study focuses on improving the catalytic capacity of the catalyst for CO hydrogenation, improving the efficiency of CO conversion to methanol, and converting H into chemical substances to avoid the danger of H storage. Based on the concept of element sharing, the ASMZ (Aluminum Shares Metal Zeolite catalysts) series catalyst was prepared by combining the CuO-ZnO-AlO catalyst with the ZSM-5 zeolite using the amphoteric metal properties of the Al element. The basic structural properties of ASMZ catalysts were compared by XRD, FTIR, and BET characterization. Catalytic properties of samples were measured on a micro fixed-bed reactor. The catalytic mechanism of the catalyst was further analyzed by SEM, TEM, XPS, H-TPR, and NH-TPD. The results show that the ASMZ3 catalyst had the highest CO conversion rate (26.4%), the highest methanol selectivity (76.0%), and the lowest CO selectivity (15.3%) in this study. This is mainly due to the fact that the preparation method in this study promotes the exposure of effective weakly acidic sites and medium strength acidic sites (facilitating the hydrogenation of CO to methanol). At the same time, the close binding of Cu-ZnO-AlO (CZA) and ZSM-5 zeolite also ensures the timely transfer of catalytic products and ensures the timely play of various catalytic active centers. The preparation method of the catalyst in this study also provides ideas for the preparation of other catalysts.
在 CO 年排放量不断上升的背景下,CO 捕集与利用技术的发展迫在眉睫。本研究聚焦于提高 CO 加氢催化剂的催化性能,提高 CO 转化为甲醇的效率,并将 H 转化为化学物质,以避免 H 储存的危险。基于元素共享的概念,通过利用 Al 元素的两性金属性质,将 CuO-ZnO-AlO 催化剂与 ZSM-5 沸石结合,制备了 ASMZ(铝共享金属沸石催化剂)系列催化剂。通过 XRD、FTIR 和 BET 表征比较了 ASMZ 催化剂的基本结构性质。在微固定床反应器上测量了样品的催化性能。通过 SEM、TEM、XPS、H-TPR 和 NH-TPD 进一步分析了催化剂的催化机理。结果表明,在本研究中,ASMZ3 催化剂具有最高的 CO 转化率(26.4%)、最高的甲醇选择性(76.0%)和最低的 CO 选择性(15.3%)。这主要是由于本研究中的制备方法促进了有效弱酸性位和中等强度酸性位的暴露(有利于 CO 加氢制甲醇)。同时,Cu-ZnO-AlO(CZA)和 ZSM-5 沸石的紧密结合也确保了催化产物的及时转移,并确保了各种催化活性中心的及时发挥。本研究中催化剂的制备方法也为其他催化剂的制备提供了思路。