(廊坊师范学院 化学与材料科学学院，廊坊 065000)
摘 要: 采用高温氧化、氢气还原、气相磷化法在SBA-15载体上分别制备了RuO2、Ru和RuP三类钌基纳米催化剂，并将其应用于催化氨硼烷水解制氢。通过场发射扫描电镜、透射电镜、X射线衍射、电感耦合等离子发射光谱仪对催化剂微观形貌、物相、元素含量进行分析；研究氨硼烷浓度、催化剂用量、反应温度和循环使用对催化剂性能的影响。结果表明：RuP催化活性最高，其次为Ru和RuO2。水解反应相对于氨硼烷浓度和催化剂用量分别为零级和一级动力学关系，Ru催化下的表观活化能低于RuP的。经过四次循环使用后，Ru/SBA-15和RuP/SBA-15的催化活性均有所衰减。
关键字: 钌基纳米粒子；氨硼烷；催化水解；制氢；动力学
（College of Chemistry and Materials Science, Langfang Normal University, Langfang 065000, China）
Abstract:In this work, SBA-15 supported RuO2, Ru and RuP nanoparticles (NPs) were prepared via high temperature oxidation, hydrogen reduction and gas-phase phosphorization, respectively. The prepared Ru-based NPs were used as catalysts for ammonia borane (AB) hydrolysis to generate hydrogen. Typically, a series of characterization including field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), X-ray diffractometry (XRD) and inductively coupled plasma-atomic emission spectrometry (ICP-AES) were conducted to analyze the microscopic morphology, phase structure and chemical composition of the catalysts. The effects of AB concentration, catalyst amount, reaction temperature and recycling on the catalyst performance were investigated. The results show that RuP NPs present the highest catalytic activity, followed by Ru NPs and RuO2 NPs. Kinetic analyses indicate that AB hydrolysis catalyzed by the RuP/SBA-15 is zero-order with respect to AB concentration and first-order relative to catalyst concentration. Compared with the RuP NPs, catalysis hydrolysis of AB using the Ru NPs shows lower apparent activation energy. After recycling four times, catalytic activities of the Ru/SBA-15 and RuP/SBA-15 decrease to some extent.
Key words: hydrogen generation; Ru-based nanoparticles; ammonia borane; catalytic hydrolysis; kinetics
