Zhang Hao, Muravev Valery, Liu Liang, Liutkova Anna, Simons Jérôme F M, Detlefs Blanka, Yang Huaizhou, Kosinov Nikolay, Hensen Emiel J M
Laboratory of Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, 5600 MB Eindhoven, The Netherlands.
European Synchrotron Radiation Facility, 71 avenue des Martyrs, CS 40220, 38043 Grenoble, France.
J Phys Chem Lett. 2023 Aug 3;14(30):6778-6783. doi: 10.1021/acs.jpclett.3c01179. Epub 2023 Jul 21.
Direct nonoxidative coupling is a promising route for methane upgrading, yet its commercialization is hindered by the lack of efficient catalysts. Pt/CeO catalysts with isolated Pt species have attracted an increasing amount of interest in recent years. Herein, we studied the catalytic role and evolution of isolated Pt centers on CeO prepared by flame spray pyrolysis under the harsh reaction conditions of nonoxidative methane coupling. During the reaction at 800 °C, the isolated Pt sites sinter, leading to a loss of the ethylene and ethane yield. The agglomerated Pt can be redispersed by using an regeneration strategy in oxygen. We found that isolated Pt centers are able to activate methane only at the initial reaction stage, and the CePt alloy acts as the active phase in the prolonged reaction.
直接非氧化偶联是甲烷升级的一条有前景的途径,然而其商业化受到缺乏高效催化剂的阻碍。近年来,具有孤立铂物种的Pt/CeO催化剂引起了越来越多的关注。在此,我们研究了在非氧化甲烷偶联的苛刻反应条件下,通过火焰喷雾热解制备的CeO上孤立铂中心的催化作用和演变。在800℃的反应过程中,孤立的铂位点烧结,导致乙烯和乙烷产率下降。通过在氧气中使用再生策略,团聚的铂可以重新分散。我们发现孤立的铂中心仅在反应初始阶段能够活化甲烷,而CePt合金在延长反应中作为活性相。