Selective conversion of methane to cyclohexane and hydrogen via efficient hydrogen transfer catalyzed by GaN supported platinum clusters

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.