Abstract
Highlights ★ Rattle-structured CuO/Co 3 O 4 @C was prepared via a hard template etching method. ★ CuO/Co 3 O 4 @C bifunctional catalysts for AB hydrolysis and methanolysis. ★ TOF values reach 18.8 and 26.8 min-1 for hydrolysis and methanolysis, respectively. ★ HGR is 4969.9 and 7078.3 mL·min-1 ·g-1 for hydrolysis and methanolysis, respectively. ★ The mechanism of AB hydrolysis and methanolysis on CuO/Co 3 O 4 @C catalyst was studied. Abstract: Engineering and fabricating cost-effective and high-performing bifunctional catalysts for ammonia borane (AB) hydrolysis and methanolysis is paramount for their commercial availability. A series of rattle-structured CuO/Co 3 O 4 @C microsphere bifunctional catalysts for AB hydrolysis and methanolysis were produced using a simple hard template etching approach. The CuO/Co 3 O 4 @C-4 (4 refers to designed the mole ratio of Cu/Co) exhibits the best activity with TOF of 18.8 and 26.8 mol H2 ·mol cat-1 ·min-1 for AB hydrolysis and methanolysis, respectively. It is discovered that the excellent performance is mainly attributed to its unique rattle structure and the synergetic effect between Co 3 O 4 and CuO. Kinetic isotope effect (KIE) experiments and infrared spectroscopy were applied to investigate AB hydrolysis and methanolysis reaction mechanisms. A suggested mechanism for AB methanolysis on rattle-structured CuO/Co 3 O 4 @C-4 is proposed based on the experiment results. This work could provide useful guidance for the construction of high-performance bifunctional catalysts for AB hydrolysis and methanolysis for hydrogen production.