Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN
Lida Tan1, Hui Su1, Jingtan Han1
1Department of Chemistry, and FQRNT Centre for Green Chemistry and Catalysis, McGill University, 801 Sherbrooke Street West, Montreal, QC, H3A 0B8, Canada.
Abstract:
Non-oxidative liquefaction of methane at room temperature and ambient pressure has long been a scientific "holy grail" of chemical research. Herein, we exploit an unprecedented catalytic transformation of methane exclusively to cyclohexane and hydrogen evolution through effective surface-hydrogen-transfer (SHT) at the heterojunctions boundary consisting of electron-rich platinum cluster (Pt) loaded on methane-activating gallium nitride (GaN) host. The experimental analysis demonstrates that the interface-induced overall reaction starts with methane aromatization to benzene and surface-bound hydrogen initiated by the Ga-N pairs, followed by the hydrogenation of benzene to cyclohexane with surface-bound hydrogen. The in-situ activated hydrogen at electron-rich metal Pt cluster is crucial for the hydrogenation and enables an outstanding selectivity (up to 92%) and productivity (41 μmol g-1) towards cyclohexane and hydrogen evolution concurrently at 300 °C, which is well-delivered after 5 recycling runs.
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