METHANE LIQUEFACTION: Selective Conversion of Methane to Cyclohexane via Efficient Surface-Hydrogen-Transfer Catalyzed by GaN-Supported Platinum Clusters

Non-oxidative liquefaction of methane at room temperature and ambient pressure has long been a scientific “holy grail” of chemical research. In this report, we exploit an unprecedented catalytic transformation of methane exclusively to cyclohexane 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 interface-induced overall reaction starts with methane aromatization to benzene initiated by the Ga-N pairs, followed by hydrogenation of benzene to cyclohexane via hydrogen transfer. The in-situ activated hydrogen at electron-rich metal Pt cluster plays a key role for the hydrogenation and enables an outstanding selectivity (as high as 89 %) towards cyclohexane, which is well-delivered even after 5 recycling runs.

Isomerizations of a Pt4 cluster revealed by spatiotemporal microscopic analysis

We now report the first direct observation of the fluxional nature in which the four-atomic platinum cluster (Pt4) randomly walks through several isomers.