Carbon neutrality initiative has stimulated the development of the sustainable methodologies for hydrogen generation and safe storage. Aqueous-phase reforming methanol and H2O (APRM) has attracted the particular interests for their high gravimetric density and easy availability. Thus, to efficiently release hydrogen and significantly suppress CO generation at low temperatures without any additives is the sustainable pursuit of APRM. Herein, we demonstrate that the dual-active sites of Pt single-atoms and frustrated Lewis pairs (FLPs) on porous nanorods of CeO2 enable the efficient additive-free H2 generation with a low CO (0.027%) through APRM at 120 °C. Mechanism investigations illustrate that the Pt single-atoms and Lewis acidic sites cooperatively promote the activation of methanol. With the help of a spontaneous water dissociation on FLPs, Pt single-atoms exhibit a significantly improved reforming of *CO to promote H2 production and suppress CO generation. This finding provides a promising path towards the flexible hydrogen utilizations.
© 2022. The Author(s).