Modulating Pt States through Hydroxyl Control for Low-Temperature Aqueous Phase Reforming of Methanol
Yuyao Yang, Xuan Bie, Xiaoying Qi, Yongqing Xu, Qinghai Li, Yanguo Zhang, Hui Zhou
Abstract
Aqueous phase reforming of methanol (APRM) offers a method for releasing H 2 from the liquid phase, by which H 2 can be stored in methanol safely. It is an efficient way to design high-performance catalysts by controlling the hydroxyl (OH) groups, but its mechanism for affecting the APRM is still unclear. Herein, we loaded Pt on three types of Al 2 O 3 (nanopolyhedron, nanosheet, and nanorod Al 2 O 3 ) with different OH contents and types. Among them, Pt/nanorod Al 2 O 3 exhibited the highest H 2 production rate of 20.4 μmol g –1 s –1 with 96.6% H 2 selectivity at a low temperature of 190 °C. This was attributed to the roles of hydroxyl groups in modulating Pt states. On nanopolyhedron, nanosheet, and nanorod Al 2 O 3, the bonding of Pt with O atoms became more favorable as the dehydroxylation happened. In particular, on nanorod Al 2 O 3, the dehydroxylation process generated a high density of five-coordinated Al (Al V ) sites, facilitating the dispersion and anchoring of Pt particles. Moreover, the special OH groups (hydrogen bond donor) on nanorod Al 2 O 3 promoted Pt particle reduction via the movement of electrons. Ultimately, the results demonstrated the influence of OH groups on the dispersion and reduction of active metals, offering perspectives for designing catalysts for APRM through hydroxyl control.