Pore Structure Modification of the Mixed Metal Oxides Derived from Co-Al Layered Double Hydroxides and Catalytic Performance Enhancement for Aerobic Oxidation of Benzyl Alcohol

The mixed metal oxides (MMOs) derived from layered double hydroxides (LDHs) are a typical class of porous materials and have attracted significant attention across various fields due to their high surface area, rich porous structures and various compositions. Regulating the pore structure of MMOs remains an urgent need because of the growing demand for numerous applications including adsorption, catalysis, and energy conversion. Controlling the lateral size of the lamellar crystals in the Co–Al LDH precursor allowed us to engineer the pore structure of Co–Al MMO, an architecture formed by the stacking of these lamellar flakes. The pore size distribution of the Co–Al MMO has been adjusted in the range from several nanometer to hundreds of nanometers. The sample with the optimized pore sizes exhibited a much higher catalytic reaction rate in the aerobic oxidation reaction of benzyl alcohol, about 4.2 times that of the control sample. Further research demonstrated that the high activity was favored by the improved mass transfer rate in the optimized pore architecture. Moreover, sodium silicate was employed as a cross-linking agent to enhance the cohesion within the secondary particles, which consist of stacked lamellar flakes. The resulting silicate-modified Co–Al MMO demonstrated significantly improved catalytic durability, maintaining stable performance over five consecutive reuse cycles—the performance that substantially exceeded that of its un-modified counterpart.