3D Oxide‐Derived Ru Catalyst for Ultra‐Efficient Hydrogenation of Levulinic Acid to γ‐Valerolactone
Shanshan Wang, Zewen Zhuang, Xin Chen, Yu Wang, Xiaoxian Li, Mingde Yang, Yulong Wu, Qing Peng, Chen Chen, Yadong Li
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.