采用两步水热晶化法合成了Cu-SBA-15介孔分子筛,并且用XRD、N2吸附、FT-IR、TEM以及UV-vis对所合成的样品进行了表征。结果表明,Cu-SBA-15具有高度有序的介孔结构和均一的孔径分布。部分铜离子进入了分子筛骨架,部分铜离子以八面体配位...采用两步水热晶化法合成了Cu-SBA-15介孔分子筛,并且用XRD、N2吸附、FT-IR、TEM以及UV-vis对所合成的样品进行了表征。结果表明,Cu-SBA-15具有高度有序的介孔结构和均一的孔径分布。部分铜离子进入了分子筛骨架,部分铜离子以八面体配位环境与骨架硅相连均匀分布在孔壁上。Cu-SBA-15(含铜6.0%)在催化氧化水溶液中4-硝基苯酚的反应中具有良好的催化活性,主要考察了H2O2初始浓度、催化剂用量、处理温度等因素对4-硝基苯酚氧化效果的影响。在4-硝基苯酚初始浓度为200 mg L 1、H2O2初始浓度为1.2 g L 1、在60℃的条件下处理100 min,4-硝基苯酚去除率达100%,TOC去除率可达82.4%。展开更多
以二乙烯三胺基丙基三甲氧基硅烷为偶联剂,采用后期修饰方法,制备出氨基修饰SBA-15(SBA代表University of California,Santa Barbara,USA)。利用扫描电镜、傅立叶红外光谱仪、N2吸附-脱附对其结构进行表征。以修饰后的SBA-15为吸附剂,...以二乙烯三胺基丙基三甲氧基硅烷为偶联剂,采用后期修饰方法,制备出氨基修饰SBA-15(SBA代表University of California,Santa Barbara,USA)。利用扫描电镜、傅立叶红外光谱仪、N2吸附-脱附对其结构进行表征。以修饰后的SBA-15为吸附剂,对水中Cu2+的吸附过程进行了动力学与热力学探讨。结果表明:修饰后的SBA-15是一种理想的铜吸附剂,pH值适应范围较宽(3~6),吸附平衡时间较短(120 min),最大吸附量可达37.94 mg/g。修饰后SBA-15对Cu2+吸附动力学符合拟二阶动力学方程,吸附过程可分为三个阶段且不只受内扩散控制。Langmuir吸附模型和Dubinin-Radushkevich(D-R)吸附模型能更好地描述了Cu2+在修饰后SBA-15上的吸附行为,其吸附平均活化能E值分别为-16.44,-17.05,-17.20 kJ/mol,表明该吸附过程为表面络合。热力学参数表明吸附过程是自发、吸热、混乱度增加的过程,升温有利于吸附。展开更多
A series of Ni/SBA-15 catalysts with 5wt% to 15wt% Ni content as well as a series of 12.5%Ni/Cu/SBA-15 catalysts with 1% to 10% copper content were prepared by the impregnation method. The catalytic performance for pa...A series of Ni/SBA-15 catalysts with 5wt% to 15wt% Ni content as well as a series of 12.5%Ni/Cu/SBA-15 catalysts with 1% to 10% copper content were prepared by the impregnation method. The catalytic performance for partial oxidation of methane was investigated in a continuous flow microreactor under atmospheric pressure. The textural and chemical properties of the catalysts were characterized by XRD, TEM, BET and Hz-TPR techniques. The results indicated that the catalysts modified with Cu promoter showed better performance than those without modification. For the 12.5%Ni/2.5%/Cu/SBA-15 catalyst, at 850 ℃ the conversion of CH4 reached 97.9% and the selectivity of CO and H2 reached 98.0% and 96.0%, respectively. In XRD patterns of the Ni/Cu/SBA-15 catalyst with 7.5 to 10% Cu contents there were CuO characteristic peaks beside NiO characteristic peaks. The mesoporous structure of SBA-15 was retained in all of the catalysts. TPR analysis of the catalysts revealed that a strong interaction between Ni, Cu promoter and SBA-15 support may be existed. This interaction enhanced significantly the redox properties of the catalysts resulting in the higher catalytic activity.展开更多
合成了以N-甲基咪唑为配体,Cu为活性中心的络合金属多相催化剂Cu(I)-NHC-SBA-15。通过1H-NMR、13CNMR、有机元素分析和FTIR对各步合成反应产物结构经行了鉴定;用SEM、N2吸附脱附等方法对催化剂进行了表征;用ICP测定了催化剂Cu含量。对...合成了以N-甲基咪唑为配体,Cu为活性中心的络合金属多相催化剂Cu(I)-NHC-SBA-15。通过1H-NMR、13CNMR、有机元素分析和FTIR对各步合成反应产物结构经行了鉴定;用SEM、N2吸附脱附等方法对催化剂进行了表征;用ICP测定了催化剂Cu含量。对催化剂催化2,4-二甲氧基溴苯还原脱溴活性进行了测试。在反应时间为24 h,通过正交实验和单因素实验,考察了催化剂用量、反应温度、还原剂用量等因素对脱溴率的影响,并确定了最佳反应条件:催化剂用量为0.05 g、水合肼用量为2 m L、反应温度为80℃,脱溴效果较好,脱溴率达到98.5%。对催化剂重复使用进行了初步研究。对催化反应动力学进行了初步研究,结果表明,该多相催化反应是由表面反应速度控制,并符合一级动力学反应。对反应机理进行了初步探讨。展开更多
文摘采用两步水热晶化法合成了Cu-SBA-15介孔分子筛,并且用XRD、N2吸附、FT-IR、TEM以及UV-vis对所合成的样品进行了表征。结果表明,Cu-SBA-15具有高度有序的介孔结构和均一的孔径分布。部分铜离子进入了分子筛骨架,部分铜离子以八面体配位环境与骨架硅相连均匀分布在孔壁上。Cu-SBA-15(含铜6.0%)在催化氧化水溶液中4-硝基苯酚的反应中具有良好的催化活性,主要考察了H2O2初始浓度、催化剂用量、处理温度等因素对4-硝基苯酚氧化效果的影响。在4-硝基苯酚初始浓度为200 mg L 1、H2O2初始浓度为1.2 g L 1、在60℃的条件下处理100 min,4-硝基苯酚去除率达100%,TOC去除率可达82.4%。
基金supported by the National Basic Research Program of China (Project No. 2005CB221405)the National "863" Project of China (No.2006AA10Z425)
文摘A series of Ni/SBA-15 catalysts with 5wt% to 15wt% Ni content as well as a series of 12.5%Ni/Cu/SBA-15 catalysts with 1% to 10% copper content were prepared by the impregnation method. The catalytic performance for partial oxidation of methane was investigated in a continuous flow microreactor under atmospheric pressure. The textural and chemical properties of the catalysts were characterized by XRD, TEM, BET and Hz-TPR techniques. The results indicated that the catalysts modified with Cu promoter showed better performance than those without modification. For the 12.5%Ni/2.5%/Cu/SBA-15 catalyst, at 850 ℃ the conversion of CH4 reached 97.9% and the selectivity of CO and H2 reached 98.0% and 96.0%, respectively. In XRD patterns of the Ni/Cu/SBA-15 catalyst with 7.5 to 10% Cu contents there were CuO characteristic peaks beside NiO characteristic peaks. The mesoporous structure of SBA-15 was retained in all of the catalysts. TPR analysis of the catalysts revealed that a strong interaction between Ni, Cu promoter and SBA-15 support may be existed. This interaction enhanced significantly the redox properties of the catalysts resulting in the higher catalytic activity.
文摘合成了以N-甲基咪唑为配体,Cu为活性中心的络合金属多相催化剂Cu(I)-NHC-SBA-15。通过1H-NMR、13CNMR、有机元素分析和FTIR对各步合成反应产物结构经行了鉴定;用SEM、N2吸附脱附等方法对催化剂进行了表征;用ICP测定了催化剂Cu含量。对催化剂催化2,4-二甲氧基溴苯还原脱溴活性进行了测试。在反应时间为24 h,通过正交实验和单因素实验,考察了催化剂用量、反应温度、还原剂用量等因素对脱溴率的影响,并确定了最佳反应条件:催化剂用量为0.05 g、水合肼用量为2 m L、反应温度为80℃,脱溴效果较好,脱溴率达到98.5%。对催化剂重复使用进行了初步研究。对催化反应动力学进行了初步研究,结果表明,该多相催化反应是由表面反应速度控制,并符合一级动力学反应。对反应机理进行了初步探讨。
