张文珂, 刘军辉, 李冰, 李梦婷, 李想, 许爱荣. NaOH(碱)诱导Co/MoO3重构催化氨硼烷水解释氢[J]. 燃料化学学报(中英文). DOI: 10.3724/2097-213X.2024.JFCT.0002
引用本文: 张文珂, 刘军辉, 李冰, 李梦婷, 李想, 许爱荣. NaOH(碱)诱导Co/MoO3重构催化氨硼烷水解释氢[J]. 燃料化学学报(中英文). DOI: 10.3724/2097-213X.2024.JFCT.0002
ZHANG Wenke, LIU Junhui, LI Bing, LI Mengting, LI Xiang, XU Airong. Co/MoO3 reconfiguration induced by NaOH (alkali) for hydrogen generation from catalytic hydrolysis of ammonia borane[J]. Journal of Fuel Chemistry and Technology. DOI: 10.3724/2097-213X.2024.JFCT.0002
Citation: ZHANG Wenke, LIU Junhui, LI Bing, LI Mengting, LI Xiang, XU Airong. Co/MoO3 reconfiguration induced by NaOH (alkali) for hydrogen generation from catalytic hydrolysis of ammonia borane[J]. Journal of Fuel Chemistry and Technology. DOI: 10.3724/2097-213X.2024.JFCT.0002

NaOH(碱)诱导Co/MoO3重构催化氨硼烷水解释氢

Co/MoO3 reconfiguration induced by NaOH (alkali) for hydrogen generation from catalytic hydrolysis of ammonia borane

  • 摘要: 本研究以MoO3为载体通过液相还原法制备了Co/MoO3催化剂,用于催化氨硼烷水解释氢反应。Co/MoO3催化剂在无NaOH(碱)加入的体系中没有催化活性,不能催化氨硼烷水解释放氢气,而在有NaOH(碱)加入的体系中表现出优异的催化释氢性能。对Co/MoO3催化剂的组成结构在反应前后变化情况的表征分析表明,Co/MoO3催化剂中的组分是Co和Mo的无定形态存在的物质,非晶态的结构导致了在氨硼烷水解释氢反应中没有催化活性。在NaOH(碱)诱导作用下,Co/MoO3催化剂的组成结构由无定形态转变为针状Co(OH)2分散在片状堆叠的MoO3上的结构。NaOH(碱)的诱导重构作用使Co/MoO3催化剂在氨硼烷水解释氢反应中由没有催化活性转变为可以在15 min内使氨硼烷完全脱氢。

     

    Abstract: The development of clean fuel sources based on renewable energy is one of the most significant subjects to replace fossil fuels. Hydrogen is considered as an attractive green fuel and a promising efficient energy carrier for future applications. Ammonia borane is an excellent hydrogen-storage material for fuel cells. The hydrolysis of ammonia borane by using heterogeneous catalysts is a secure and promising way to produce hydrogen in mild conditions. The noble metal-based catalysts usually present outstanding activity, while high cost and rarity limit their further application. In recent years, economical non-noble metal-based catalysts have been developed for catalytic hydrolysis of AB. Co, Ni and Cu have been widely used as the active metals, which presented the higher catalytic activity for hydrogen evolution. Co-based catalyst is an excellent candidate to catalyze the AB dehydrogenation reaction, and various Co-based catalysts were designed to improve the dehydrogenation rate. The structure-activity relationship of catalysts is the key to study the catalytic mechanism in heterogeneous catalysis. The reduction method was adopted to prepare the Co/MoO3 catalyst by using MoO3 as support for catalytic hydrolysis of ammonia borane to release hydrogen. The Co/MoO3 catalyst showed no catalytic activity in the system without NaOH (alkali), and could not catalyze the hydrolysis of ammonia borane to release hydrogen. However, the Co/MoO3 catalyst exhibited excellent catalytic performance by adding NaOH (alkali) into the reaction system. The catalysts prepared by the liquid phase reduction method using other common materials as the carrier do not have this characteristic. Different concentrations or types of bases can make the Co/MoO3 catalyst change from no catalytic activity to higher catalytic activity. The characterization analysis of the compositional structure of the Co/MoO3 catalyst was carried out by XRD, SEM and TEM before and after the hydrolysis reaction, and the results indicated that the components of Co/MoO3 catalyst were amorphous substances of Co and Mo, and their amorphous structure resulted in no catalytic activity during ammonia borane hydrolysis. By the induction affection of NaOH (alkali), the structure of the Co/MoO3 catalyst transformed from amorphous state to needle-like dispersion of Co(OH)2 on stacked MoO3 sheets. The induced reconstruction effect of NaOH (alkali) enabled the catalyst to exhibit excellent performance in for H2 generation from ammonia borane hydrolysis, and the H2 generation reaction can complete within 15 minutes. This work provides a deep insight into the structure-activity relationship and structure reconstruction of catalysts during the heterogeneous catalytic reaction.

     

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