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作 者:尉继英[1] 张振中[1] 张兰[1] 孟弼芳[1] 江锋[1]
机构地区:[1]清华大学核能与新能源技术研究院北京精细陶瓷重点实验室,北京100084
出 处:《稀有金属材料与工程》2012年第3期377-382,共6页Rare Metal Materials and Engineering
基 金:National Natural Science Foundation of China(20777046,21077064);Specialized Research Fund for the Doctoral Program of Higher Education of China(20070003027)
摘 要:采用沉积沉淀法制备了CO低温氧化 Au/α-Fe2O3催化剂,利用 X 射线衍射(XRD)、X 射线光电子能谱(XPS)、BET 比表面测定、程序升温还原(H2-TPR)等表征技术,对比了制备过程 pH 值的微小变化、焙烧及光线照射对催化剂结构及催化性能的影响,探明了 Au/α-Fe2O3催化剂的活性物种。结果表明,110 ℃处理的 Au/α-Fe2O3催化剂表面同时存在 Au3+、Au0以及过渡态 Auδ+(0<δ<1),它们对 CO 氧化的活性顺序为 Au3+>Auδ+>Au0;pH 值为 8 条件下制备的催化剂 Au3+含量高、比表面积大,催化性能最好;高温焙烧使氧化态金还原的同时也使载体比表面积严重缩小,催化活性显著下降;紫外线照射可以引起 Au3+的逐渐还原以及 Au0 颗粒的生长,其催化失活作用弱于高温焙烧。Au/α-Fe2O3 catalysts for CO oxidation were prepared by chemical coprecipitation at different pH values, and the as-prepared samples were calcined or UV (2=254 nm) irradiated, respectively. The structure was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N2 adsorption and desorption analysis (BET) and temperature programmed reduction (H2-TPR), and the active Au species on the catalysts was investigated. The results show that Au^3+, Au^δ+ (0〈δ〈1) and Au^0 coexist on the surface of Au/α-Fe2O3 catalysts treated at 110 ℃, and their activity order is Au3+〉 Aua+〉 Au~. The sample prepared at pH=8 shows the best catalytic performance since it has more Au^3+ species and high specific surface area. High temperature calcination can cause serious deactivation due to the reduction of Au^3+ and Au^δ+ species, together with the decrease of the specific surface area of α-Fe2O3. UV irradiation can also cause the reduction of oxidative Au species and the growth of Au particle.
关 键 词:Au/α-Fe2O3 一氧化碳低温氧化 活性金物种 失活
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