Highly Effective Cu/AEI Zeolite Catalysts Contribute to Continuous Conversion of Methane to Methanol
Peipei Xiao, Yong Wang, K. Nakamura, Yao Lu, Trees De Baerdemaeker, Andrei‐Nicolae Parvulescu, Ulrich Müller, Dirk De Vos, Xiangju Meng, Feng‐Shou Xiao, Weiping Zhang, Bernd Marler, Ute Kolb, Ryota Osuga, Maiko Nishibori, Hermann Gies, Toshiyuki Yokoi
Abstract
High Resolution Image Download MS PowerPoint Slide A robust catalyst that can continuously and effectively produce methanol from methane is exceedingly desired. Cu-containing zeolite catalysts were widely used in direct oxidative methane to methanol reactions, and the local structure of the Cu species was one of the key factors to influence the reaction performance. It has been considered that dicopper was a highly active species, and its implementation was thoroughly dependent on the Al pairs in the zeolite framework. Therefore, to obtain a highly effective Cu-exchanged AEI zeolite catalyst, the synthesis of the AEI zeolite with a high proportion of Al pairs was an important premise. Herein, AEI zeolite was successfully synthesized from ferrierite (FER) zeolite via the interzeolite conversion (IZC) method. The use of FER zeolite realized a high proportion of Al pairs, leading to the fabrication of abundant dicopper-containing AEI. In addition, the high thermal stability of the AEI zeolite enabled us to adjust the framework Al distribution and the acidic properties by postcalcination. Thus, the prepared Cu/AEI zeolite with plentiful dicopper species exhibited a distinctive catalytic performance in the continuous conversion of methane to methanol at 350 °C; a state-of-the-art methanol productivity of 40.8 μmol·g –1 ·min –1 (2448 μmol·g –1 ·h –1 ) with a 45% selectivity and long-term reaction stability was achieved.