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作 者:徐托雨 蔡思翔[1,2,3] XU TuoYu;CAI SiXiang(School of Materials Science and Engineering,Hainan University,Haikou 570228,China;Special Glass Key Lab of Hainan Province,Hainan University,Haikou 570228,China;State Key Laboratory of Marine Resource Utilization in South China Sea,Hainan University,Haikou 570228,China)
机构地区:[1]海南大学材料科学与工程学院,海口570228 [2]海南大学海南省特种玻璃重点实验室,海口570228 [3]海南大学南海海洋资源利用国家重点实验室,海口570228
出 处:《北京化工大学学报(自然科学版)》2021年第1期25-33,共9页Journal of Beijing University of Chemical Technology(Natural Science Edition)
基 金:海南省青年基金项目(218MS004);中央引导地方科技发展专项资金(ZY2019HN0904);海南省重点研发计划项目(ZDYF2020015);海南大学科研平台建设(ZY2019HN09)。
摘 要:采用浸渍法对TiO_(2)负载的铈基催化剂进行了硫酸化改性,同时制备了未经硫酸化改性的催化剂与之对比,通过X射线衍射(XRD)、比表面积测试(BET)、氢气程序升温还原(H_(2)-TPR)、X射线光电子能谱(XPS)和吡啶红外光谱(Py-IR)等一系列手段对催化剂进行了表征。结果表明,硫酸化改性不仅能够增加催化剂表面的化学吸附氧的含量,提高催化剂的氧化还原性,而且还能极大地丰富催化剂表面的布朗斯特酸位点和路易斯酸位点,以此来增加催化剂的酸性,使得催化剂的低温活性有所提升并拓宽其温度窗口。此外,硫酸化改性为铈基催化剂表面增加了额外的超强酸位点,使催化剂在受到碱金属的毒害后,仍有大量的酸位能得以保留,能够维持对NH3的吸附,进行催化反应循环,极大地提升催化剂的抗碱金属性能。TiO_(2)-supported cerium-based catalysts have been modified by sulfation using the impregnation method, and their properties were compared with those of the unmodified catalysts. The catalysts were characterized by means of X-ray diffraction(XRD), specific surface area measurements(BET), hydrogen temperature-programmed reduction(H_(2)-TPR), X-ray photoelectron spectroscopy(XPS) and pyridine infrared spectroscopy(Py-IR). The results showed that sulfation not only increases the content of chemisorbed oxygen on the catalyst surface and improves the redox activity of the catalyst, but also greatly increases the number of Br?nsted acid sites and Lewis acid sites on the catalyst surface. The resulting increase in the acidity of the catalyst improves its low temperature activity and broadens its temperature window. In addition, extra super acid sites were generated on the surface of the cerium-based catalysts after sulfation. A significant proportion of these acid sites were retained after the catalyst was poisoned by alkali metals, allowing the adsorption of NH3 and the catalytic reaction to continue, thus improving the alkali metal resistance of the catalyst.
关 键 词:选择性催化还原 催化剂 氮氧化物 多相反应 活性
分 类 号:X511[环境科学与工程—环境工程]
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