Direct Non‐Oxidative Methane Conversion in a Millisecond Catalytic Wall Reactor

• Published in: Angewandte Chemie International Edition 2019-05, Vol.58 (21), p.7083-7086
• Main Authors: Oh, Su Cheun, Schulman, Emily, Zhang, Junyan, Fan, Jiufeng, Pan, Ying, Meng, Jianqiang, Liu, Dongxia
• Format: Article
• Language: English
• Subjects: Alkenes; Catalytic converters; Coke; Conversion; Durability; Endothermic reactions; Flow velocity; Gas flow; heterogeneous catalysis; iron; Methane; methane conversion; natural gas; Organic chemistry; Reactor materials; Reactors; Selectivity; supported catalysts; Technology; Viability
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.201903000

Direct non‐oxidative methane conversion (DNMC) has been recognized as a single‐step technology that directly converts methane into olefins and higher hydrocarbons. High reaction temperature and low catalyst durability, resulting from the endothermic reaction and coke deposition, are two main challenges. We show that a millisecond catalytic wall reactor enables stable methane conversion, C2+ selectivity, coke yield, and long‐term durability. These effects originate from initiation of the DNMC on a reactor wall and maintenance of the reaction by gas‐phase chemistry within the reactor compartment. The results obtained under various temperatures and gas flow rates form a basis for optimizing the process towards lighter C2 or heavier aromatic products. A process simulation was done by Aspen Plus to understand the practical implications of this reactor in DNMC. High carbon and thermal efficiencies and low cost of the reactor materials are realized, indicating the technoeconomic viability of this DNMC technology. Wall to wall: The upgrade of CH4 by direct non‐oxidative methane conversion is facilitated by a Fe/SiO2 millisecond catalytic wall reactor. The reactor design results in stable methane conversion, C2+ selectivity, coke yield, and long‐term durability.