Abstract
The oxidation state of an active metal is vital in the hydrolysis of NaBH4 for rapid hydrogen generation since the electron-rich and electron-deficient sites facilitate BH4− and H2O adsorption. Herein, we systematically design a tunable oxidation state of Co in Co3O4 by in situ N-doing using the combination of melamine (M) and urea (U) as nitrogen precursors during thermal treatment. The oxidation state of Co was tuned via electronic interaction between N and Co. This interaction was optimized by varying the amount of N doping and calcination temperature. The types of heterocyclic nitrogen, mainly pyridinic- and graphitic-N, and their carbon matrix content are critical in controlling the Co oxidation state. Various Co2+/Co3+ ratios showed a different catalytic performance, and the catalytic activity reached its peak at the highest ratio of 2.74 due to the synergetic effect of the maximum adsorption of BH4− and H2O by Co2+ and Co3+, respectively. Consequently, an excellent hydrogen generation rate (2042 mL g−1 min−1) was achieved with a low activation energy of 46.9 kJ mol−1 of M2.5U10Co3O4-400. Hence, N doping from a dual N source significantly enhanced the hydrogen performance compared to the reported cobalt-based catalyst. Furthermore, M2.5U10Co3O4-400 is highly recyclable, implying its stability and practical application.
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