Ru/g-C₃N₄催化NaBH₄水解产氢性能研究

Performance of Ru/g-C₃N₄ Catalyst for Hydrogen Generation from Hydrolysis of Sodium Borohydride

摘要: 本文以RuCl₃∙xH₂O与NaH₂PO₂∙H₂O为原料，g-C₃N₄为载体，采用水热还原法制备了Ru/g-C₃N₄催化剂，考察了载体种类、载体前驱体三聚氰胺水热时间、Ru负载量、次亚磷酸钠浓度和水热还原时间对制备的Ru催化剂催化硼氢化钠产氢性能的影响。结果表明，在g-C₃N₄-0、二氧化硅、二氧化锆、氧化铝、硅藻土载体中，g-C₃N₄-0作载体Ru催化剂催化硼氢化钠水解产氢的速率最快。当次亚磷酸钠的浓度为0.099 mol∙L⁻¹，水热还原温度为180℃，水热还原时间为10 h，钌负载量50%，载体前驱体三聚氰胺不进行水热，制备的Ru/g-C₃N₄-0催化剂催化硼氢化钠产氢性能最好，活化能为35.30 kJ∙mol⁻¹，TOF为67.70 min⁻¹。

Abstract: In this study, a Ru/g-C₃N₄ catalyst was synthesized via a hydrothermal reduction method using RuCl₃·xH₂O and NaH₂PO₂·H₂O as precursors, with g-C₃N₄ serving as the support. The influence of various factors on the catalytic performance of Ru/g-C₃N₄ was systematically investigated, including the type of support, hydrothermal treatment time of the support precursor (melamine), Ru loading amount, sodium hypophosphite concentration, and hydrothermal reduction time. The results demonstrated that among the supports evaluated—such as g-C₃N₄-0, SiO₂, ZrO₂, Al₂O₃, and diatomite, the Ru catalyst supported on g-C₃N₄-0 exhibited the highest hydrogen generation rate from the hydrolysis of sodium borohydride. When the concentration of sodium hypophosphite was 0.099 mol∙L⁻¹, the hydrothermal reduction temperature was 180˚C, and the hydrothermal reduction time was 10 h, the ruthenium loading capacity was 50%, the hydrothermal time of the carrier precursor melamine was 0 h, the prepared Ru/g-C₃N₄-0 catalyst had the best catalytic performance for hydrogen production of sodium borohydride. The activation energy is 35.30 kJ∙mol⁻¹ and the TOF is 67.70 min⁻¹.