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机构地区:[1]新疆大学石油天然气精细化工教育部重点实验室,新疆乌鲁木齐830046 [2]中国石油新疆培训中心,新疆乌鲁木齐830000
出 处:《新疆大学学报(自然科学版)》2010年第3期343-348,共6页Journal of Xinjiang University(Natural Science Edition)
基 金:新疆大学博士科研启动基金(BS060101)资助
摘 要:在3%VOx/SiO2催化剂对正丁烷氧化脱氢(ODH)效果良好的基础上,采用共同浸渍的方法,添加金属Li、K、Ca、Sr、Al、Ni、Zn、Fe的金属氧化物为改进剂.实验结果表明:加入Li、Ca、Sr、Zn等金属虽然降低了催化剂的活性,但可以大大改善对正丁烷深度氧化的程度;Al、Fe不但降低了催化剂的活性,同时也使正丁烷深度氧化程度大增;K有利于正丁烷发生裂解反应,而不利于脱氢产物的生成;Ni可以显著改善C4烯烃的选择性,有利于1,3-丁二烯生成不利于正丁烯的生成,同时也降低了催化剂的活性.通过H2-TPR研究表明:NiO和VOx相结合形成了新物种,其还原温度介于两者之间;FeOx和VOx结合生成了更强氧化性物种;Li、K、Ca、Sr、Al、Zn改性后均未出现新的氢消耗峰,并且其氢消耗峰均向高温移动,说明金属改进剂的加入使钒活性组分更难被还原.Owing to good effect on the catalyze n-butane oxidation dehydrogen(ODH) over 3%VOx/SiO2, adding elements Li. K、 Ca、 Sr、 Al、 Ni、Zn 、Fe are co-impregnated as the improver. The experiment results shows that despite the activity of the catalyst falling with adding Li、Ca 、Sr、Zn, this can remedy profundity oxidation degree of the n-butane evidently, adding Al、 Fe not only reduces the catalyst activity but also makes the n-butane oxidation degree increasing evidently, adding K is propitious to n-butane cracking and against the dehydrogenation, adding Ni can improve the selectivity of Ca olefins notably (be propitious to 1, 3-butadiene and against n-butene), and also reduce the catalytic activity. H2-TPR shows that NiO incorporation with VOx forms new species, and whose deoxidization temperature is between the both; FeO2 incorporation with VOx creates more strong oxidation species; by Li、 K、 Ca、Sr、 Al、 Zn improving, the new hydrogen depleted peak appears, and the original hydrogen depleted peak moves to the high temperature, which shows that the metal added makes the vanadium active component more difficultly deoxidized.
关 键 词:MO-VOx/SiO2催化剂 正丁烷 氧化脱氢 金属改性
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