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/Co3O4@C microsphere bifunctional catalysts for AB hydrolysis and methanolysis were produced using a simple hard template etching approach. The CuO/Co3O4@C-4 (4 refers to designed the mole ratio of Cu/Co) exhibits the best activity with TOF of 18.8 and 26.8 molH2·molcat-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 Co3O4 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/Co3O4@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.

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