Controllable synthesis of CuAlO_(2) via solid-phase method and its catalytic performance for methanol steam reforming to hydrogen

固相球磨法可控制备CuAlO_(2)及其甲醇重整制氢催化性能研究

This study explores the controllable synthesis of CuAlO_(2) using copper hydroxide and pseudo-boehmite powders as raw materials via a simple solid-phase ball milling method,along with its catalytic performance investigation in methanol steam reforming(MSR).Various catalysts were prepared under different conditions,such as calcination temperature,calcination atmosphere,and heating rate.Characterization techniques including BET,XRD,XPS,SEM and H2-TPR were employed to analyze the samples.The results revealed significant effects of calcination temperature on the phase compositions,specific surface area,reduction performance,and surface properties of the CA-T catalysts.Based on the findings,a synthesis route of CuAlO_(2) via the solid-phase method was proposed,highlighting the importance of high calcination temperature,nitrogen atmosphere,and low heating rate for CuAlO_(2) formation.Catalytic evaluation data demonstrated that CuAlO_(2) could catalyze MSR without pre-reduction,with the catalytic performance of CA-T catalysts being notably influenced by calcination temperature.Among the prepared catalysts,the CA-1100 catalyst exhibited the highest catalytic activity and stability.The findings of this study might be useful for the further study of the catalytic material for sustained release catalysis,including the synthesis of catalytic materials and the regulation of sustained release catalytic performance.

本工作以氢氧化铜和拟薄水铝石作为原料,采用固相球磨法可控合成了CuAlO_(2)缓释催化剂,并探究了其在甲醇水蒸气重整反应中的催化性能。重点研究了焙烧温度、焙烧气氛和加热速率对CuAlO_(2)缓释催化剂的结构影响。通过BET、XRD、XPS、SEM和H_(2)-TPR等表征技术分析,结果显示焙烧温度对CA-T催化剂的相组成、比表面积、还原性能和表面性质有显著影响;对比分析表明高焙烧温度、氮气气氛和低加热速率有利于CuAlO_(2)结构的生成。催化评价数据表明,CuAlO_(2)可以在无预还原条件下实现高性能的甲醇重整制氢反应,而催化剂反应性能与焙烧温度密切相关,在800-1200℃焙烧温度下,1100℃焙烧条件下制备的CA-1100催化剂表现出最佳的催化活性和稳定性。本研究的结果可为缓释催化材料的合成、缓释催化性能调控等的进一步深入研究提供有效的基础数据和理论支撑。