title: New route toward building active ruthenium nanoparticles on ordered mesoporous carbons with extremely high stability.
abstract: Creating highly active and stable metal catalysts is a persistent goal in the field of heterogeneous catalysis. However, a real catalyst can rarely achieve both of these qualities simultaneously due to limitations in the design of the active site and support. One method to circumvent this problem is to fabricate firmly attached metal species onto the voids of a mesoporous support formed simultaneously. In this study, we developed a new type of ruthenium catalyst that was firmly confined by ordered mesoporous carbons through the fabrication of a cubic Ia3d chitosan-ruthenium-silica mesophase before pyrolysis and silica removal. This facile method generates fine ruthenium nanoparticles (ca. 1.7 nm) that are homogeneously dispersed on a mesoporous carbonaceous framework. This ruthenium catalyst can be recycled 22 times without any loss of reactivity, showing the highest stability of any metal catalysts; this catalyst displays a high activity (23.3 mol(LA)h(-1)g(metal)(-1)) during the catalytic hydrogenation of levulinic acid (LA) when the metal loading is 6.1 wt%. Even at an ultralow loading (0.3 wt%), this catalyst still outperforms the most active known Ru/C catalyst. This work reveals new possibilities for designing and fabricating highly stable and active metal catalysts by creating metal sites and mesoporous supports simultaneously.
authors.affiliation: State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Changping, Beijing 102249, China.
authors.forename: Ying
authors.initials: Y
authors.lastname: Yang
authors.affiliation: X-ray Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Argonne, Illinois 60439, USA.
authors.forename: Chengjun
authors.initials: C
authors.lastname: Sun
authors.affiliation: X-ray Science Division, Argonne National Laboratory, 9700 S. Cass Ave., Argonne, Illinois 60439, USA.
authors.forename: Yang
authors.initials: Y
authors.lastname: Ren
authors.affiliation: State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Changping, Beijing 102249, China.
authors.forename: Shijie
authors.initials: S
authors.lastname: Hao
authors.affiliation: State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Changping, Beijing 102249, China.
authors.forename: Daqiang
authors.initials: D
authors.lastname: Jiang