制备方法对Cu/Ce_(0.8)Zr_(0.2)O_(2)催化剂催化甲醇水蒸气重整制氢性能的影响  

Effects of preparation methods on catalytic performances of Cu/Ce_(0.8)Zr_(0.2)O_(2) catalysts for methanol steam reforming to produce hydrogen

作　　者：徐青文 柯举仓 李蕊 李鹏[1] 王凤霞 马清祥[1] 赵天生[1] XU Qingwen;KE Jucang;LI Rui;LI Peng;WANG Fengxia;MA Qingxiang;ZHAO Tiansheng(State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering,College of Chemistry and Chemical Engineering,Ningxia University,Yinchuan 750021,Ningxia,China;Analysis and Testing Center,Ningxia University,Yinchuan 750021,Ningxia,China)

机构地区：[1]宁夏大学化学化工学院省部共建煤炭高效利用与绿色化工国家重点实验室,宁夏银川750021 [2]宁夏大学测试分析中心,宁夏银川750021

出　　处：《低碳化学与化工》2024年第9期33-40,50,共9页Low-Carbon Chemistry and Chemical Engineering

基　　金：宁夏自然科学基金(2021AAC03108)。

摘　　要：制备方法会影响催化剂中Cu物种种类、分散性及其与载体之间的相互作用。分别采用沉积沉淀法、氨蒸法、浸渍法和共沉淀法制备了以Ce_(0.8)Zr_(0.2)O_(2)固溶体为载体、Cu负载量(质量分数)为15%的Cu/Ce_(0.8)Zr_(0.2)O_(2)催化剂。采用XRD、N_(2)物理吸/脱附、N_(2)O滴定和SEM等对催化剂的物相组成、织构性质、Cu分散度和微观结构等进行了表征,并采用固定床反应器评价了催化剂的甲醇水蒸气重整制氢催化性能。结果表明,与其他3种方法制备的Cu/Ce_(0.8)Zr_(0.2)O_(2)催化剂相比,采用沉积沉淀法制备的Cu/Ce_(0.8)Zr_(0.2)O_(2)催化剂(Cu/Ce_(0.8)Zr_(0.2)O_(2)-DP)具有相对最大的比表面积(82.5 m^(2)/g)和Cu比表面积(206.0 m^(2)/g),以及相对最高的Cu分散度(30.5%)。在温度为250℃、常压、n(去离子水):n(甲醇)为1.3:1.0和液时空速为6 mL/(g·h)的条件下反应24 h,Cu/Ce_(0.8)Zr_(0.2)O_(2)-DP表现出相对最优的催化性能,其甲醇转化率为95.2%,产氢速率为286.8 mmol/(g·h),CO选择性为0.86%。The preparation methods can affect the type and dispersion of Cu species,as well as the interaction between Cu species and supports in catalysts.Cu/Ce_(0.8)Zr_(0.2)O_(2) catalysts with Ce_(0.8)Zr_(0.2)O_(2) sosolid as the support and Cu loading(mass fraction) of 15% were prepared by deposition precipitation,ammonia evaporation,impregnation and co-precipitation methods,respectively.The phase compositions,texture properties,Cu dispersions and microstructures of the catalysts were characterized by XRD,N_(2) physical adsorption/desorption,N_(2O) titration,SEM,etc.And the catalytic performances of the catalysts for methanol steam reforming to produce hydrogen were evaluated in a fixed-bed reactor.The results show that compared with the Cu/Ce_(0.8)Zr_(0.2)O_(2) catalysts prepared by another three methods,the Cu/Ce_(0.8)Zr_(0.2)O_(2) catalyst(Cu/Ce_(0.8)Zr_(0.2)O_(2)-DP) prepared by deposition precipitation method has the largest specific surface area(82.5 m^(2)/g) and Cu specific surface area(206.0 m^(2)/g),as well as the highest Cu dispersion(30.5%).Under the reaction conditions of 250 ℃,atmospheric pressure,n(deionized water):n(methanol) of 1.3:1.0 and liquid space velocity of 6 mL/(g·h) for 24 h,Cu/Ce_(0.8)Zr_(0.2)O_(2)-DP shows relatively optimal catalytic performance with methanol conversion rate of 95.2%,hydrogen production rate of 286.8 mmol/(g·h) and CO selectivity of 0.86%.

关 键 词：甲醇水蒸气重整 Cu基催化剂 制备方法 铈锆固溶体 Cu分散度 

分 类 号：TQ426[化学工程]