3D Oxide‐Derived Ru Catalyst for Ultra‐Efficient Hydrogenation of Levulinic Acid to γ‐Valerolactone

Abstract

Abstract γ‐valerolactone (GVL) is a key value‐added chemical catalytically produced from levulinic acid (LA), an important biomass derivative platform chemical. Here an ultra‐efficient 3D Ru catalyst generated by in situ reduction of RuZnO x nanoboxes is reported; the catalyst features a well‐defined structure of highly dispersed in situ oxide‐derived Ru (IOD‐Ru) clusters (≈1 nm in size) spatially confined within the 3D nanocages with rich mesopores, which guarantees a maximized atom utilization with a high exposure of Ru active sites as well as a 3D accessibility for substrate molecules. The IOD‐Ru exhibits ultrahigh performance for the hydrogenation of LA into GVL with a record‐breaking turnover frequency (TOF) up to 59400 h −1 , 14 times higher than that of the ex situ reduction of RuZnO x nanoboxes catalyst. Structural characterizations and theoretical calculations collectively indicate that the defect‐rich and coordination‐unsaturated IOD‐Ru sites can boost the activation of the carbonyl group in LA with a significantly lowered energy barrier of hydrogenation.