期刊
JOURNAL OF COLLOID AND INTERFACE SCIENCE
卷 646, 期 -, 页码 25-33出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcis.2023.04.181
关键词
Ammonia borane; Hydrogen generation; Hydrolysis; Mott-Schottky effect; Heterostructure
In this study, a robust Ru-Co3O4 catalyst was designed using the Mott-Schottky effect to induce favorable charge rearrangement, resulting in an optimal Ru-Co3O4 heterostructure that exhibited outstanding catalytic activity for the hydrolysis of ammonia borane (AB) with high hydrogen generation rate and turnover frequency.
Developing efficient catalysts for the dehydrogenation of ammonia borane (AB) is important for the safe storage and controlled release of hydrogen, but it is a challenging task. In this study, we designed a robust Ru-Co3O4 catalyst using the Mott-Schottky effect to induce favorable charge rearrangement. The self-created electron-rich Co3O4 and electron-deficient Ru sites at heterointerfaces are indispensable for the activation of the B-H bond in NH3BH3 and the O-H bond in H2O, respectively. The synergistic electronic interaction between the electron-rich Co3O4 and electron-deficient Ru sites at the heterointerfaces resulted in an optimal Ru-Co3O4 heterostructure that exhibited outstanding catalytic activity for the hydrolysis of AB in the presence of NaOH. The hetero-structure had an extremely high hydrogen generation rate (HGR) of 12238 mL min-1 gcat-1 and an expected high turnover frequency (TOF) of 755 molH2 molRu-1 min-1 at 298 K. The activation energy needed for the hydrolysis was low (36.65 kJ mol-1). This study opens up a new avenue for the rational design of high-performance cat-alysts for AB dehydrogenation based on the Mott-Schottky effect.
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