(廊坊師范學(xué)院 化學(xué)與材料科學(xué)學(xué)院，廊坊 065000)
摘 要: 采用高溫氧化、氫氣還原、氣相磷化法在SBA-15載體上分別制備了RuO2、Ru和RuP三類釕基納米催化劑，并將其應(yīng)用于催化氨硼烷水解制氫。通過場發(fā)射掃描電鏡、透射電鏡、X射線衍射、電感耦合等離子發(fā)射光譜儀對催化劑微觀形貌、物相、元素含量進(jìn)行分析；研究氨硼烷濃度、催化劑用量、反應(yīng)溫度和循環(huán)使用對催化劑性能的影響。結(jié)果表明：RuP催化活性最高，其次為Ru和RuO2。水解反應(yīng)相對于氨硼烷濃度和催化劑用量分別為零級和一級動力學(xué)關(guān)系，Ru催化下的表觀活化能低于RuP的。經(jīng)過四次循環(huán)使用后，Ru/SBA-15和RuP/SBA-15的催化活性均有所衰減。
關(guān)鍵字: 釕基納米粒子；氨硼烷；催化水解；制氫；動力學(xué)
（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
