2022 Spring Meeting and 18th Global Congress on Process Safety Proceedings

(39c) Direct Methane Activation By Atomically Thin Platinum Nanolayers on Two-Dimensional Metal Carbides

Authors

Zhe Li, Iowa State University
Prabudhya Chowdhury, Purdue University
Zhenwei Wu, Purdue University
Tao Ma, Ames Laboratory
Johnny Zhuchen, Purdue University
Gang Wan, SLAC National Accelerator Laboratory
Tae-Hoon Kim, Department of Industrial Engineering, Lamar University
Peilei He, Iowa State University
Pratik Potdar, Purdue University
Lin Zhou, Ames Laboratory
Zhenhua Zeng, Purdue University
Xiulin Ruan, Purdue University
Jeffrey T. Miller, Purdue University
Jeffrey Greeley, Purdue University
Yue Wu, Iowa State University
Arvind Varma, Purdue University
Dapeng Jing, Department of Energy Ames Laboratory
Efficient and direct conversion of methane to value-added products has been a long-term challenge in shale gas applications. Here, we show that atomically thin nanolayers of Pt with a single or double atomic layer thickness, supported on a two-dimensional molybdenum titanium carbide (MXene), catalyse non-oxidative coupling of methane to ethane/ethylene (C2). Kinetic and theoretical studies, combined with in-situ spectroscopic and microscopic characterizations, demonstrate that Pt nanolayers anchored at the hexagonal close-packed sites of the MXene support can activate the first C–H bond of methane to form methyl radicals that favour desorption over further dehydrogenation and thus suppress coke deposition. At 750 °C and 7% methane conversion, the catalyst runs for 72 hours of continuous operation without deactivation and exhibits >98% selectivity towards C2 products, with a turnover frequency of 0.2–0.6 s−1. Our findings provide insights into the design of highly active and stable catalysts for methane activation and create a platform for developing atomically thin supported metal catalysts.