摘要
A convenient, high-density and low-cost hydrogen supply technology is essential to hydrogen energy system by providing hydrogen to fuel cell component. Magnesium silicide (Mg 2 Si) can be a good hydrolysis candidate due to its low cost and ability of releasing hydrogen gas during hydrolysis process. However, previous studies have demonstrated that Mg 2 Si could easily produce large amount of silanes during hydrolysis reaction, which may cause serious problem of explosive danger when in contact with air. Here it is the first time that Mg 2 Si was used for generation of hydrogen by a simple and convenient one-step hydrolysis reaction. In this study, hydrolysis kinetics and mechanisms of Mg 2 Si in NH 4 Cl and NH 4 F solutions were investigated. The silanes could be almost completely turned into hydrogen by introduction of fluorine ion during the hydrolysis reaction of Mg 2 Si, leading to very low silanes content in the produced hydrogen. The kinetic studies indicated that when the concentration of the NH 4 F solution increased to 13.0%, the hydrogen generation rate and the reaction yield were improved significantly and reached the best performance, producing 466 mL g −1 H 2 in 10 min and 616 mL g −1 H 2 in 30 min at 25 °C. The activation energy was calculated to be 37.3 ± 0.8 kJ mol −1 . Furthermore, the hydrogen yield and the hydrolysis rate of Mg 2 Si can be further improved by high-energy ball milling. After ball milling for 2 and 5 h, the hydrogen generation yield in 30 min increased to 698 and 771 mL g −1 , respectively, and the activation energy was decreased to 23.9 ± 0.6 kJ mol −1 and 12.9 ± 0.1 kJ mol −1 , respectively. The results revealed that NH 4 F can be a promising reagent for promoting the hydrolysis of Mg 2 Si for onsite hydrogen supply.
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