When Pt nanoparticles meet oxygen-deficient Co3O4: Enabling superior performance towards on-demand hydrogen generation from hydrolytic dehydrogenation of dimethylamine borane

Abstract

The regulation of the metal-support interaction in heterogeneous catalysts can promote the activation of reactants, which is beneficial for the hydrolytic dehydrogenation reaction. Herein, the hydrolytic dehydrogenation of dimethylamine borane (DMAB) is systematically studied on the oxygen vacancy (Ov) enriched Pt-Co3O4 heterogeneous catalyst with the metal-support interaction. It is found that the metallic Pt site facilitates the adsorption of DMAB molecules and the Ov on Co3O4 support as an electron-rich center cooperates with the adjacent Pt site to dissociate water molecules. The in situ Raman and attenuated total reflectance (ATR)-Fourier transform infrared (FTIR) spectroscopy reveal the effective activation and cleavage of the O-H in water and the B-H in DMAB over the Pt-Co3O4 catalyst. The optimal Pt-Co3O4 catalyst exhibits the extraordinary activity for the catalytic hydrolysis of DMAB at 303 K, delivering a high specific hydrogen generation rate (64063 mL min−1 gpt−1) and a competitive turnover frequency (TOF, 23880 molH2 molPt−1 h−1). This performance outperforms most of the reported heterogeneous catalysts for DMAB dehydrogenation. More importantly, the Pt-Co3O4 catalyst achieves the desirable on-demand hydrogen production by using special chemical switches. This finding provides the fundamental understanding of metal-oxide systems with the collaborative interfacial catalysis for boosting DMAB dehydrogenation.