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Insight into the H2S Selective Catalytic Oxidation Performances on Well-Mixed Ce-Containing Rare Earth Catalyst Derived from MgAlCe Layered Double Hydroxides
Journal of Hazardous Materials ( IF 13.6 ) Pub Date : 2017-09-09 , DOI: 10.1016/j.jhazmat.2017.09.014
Fenglian Zhang , Xin Zhang , Zhengping Hao , Guoxia Jiang , Hongling Yang , Siqiu Qu

A series of well-mixed Ce-containing MgAlCe rare earth catalysts derived from layered double hydroxides were synthesized and tested for H2S selective catalytic oxidation. Particularly, no chemisorption O-vacancies but intrinsic defect sites were present on catalyst surface. Significantly, the catalysts exhibited excellent catalytic activity, reasonable durability, and outstanding sulfur selectivity (100%) at relatively low temperatures. Furthermore, the catalyst followed a step-wise mechanism, and the catalyst deactivation was due mainly to the slower oxidation rate of Ce3+ to Ce4+ by O2 as compared to the reduction rate of Ce4+ to Ce3+ by H2S. Particularly, the added water, a Lewis base, can compete with inefficient S8 catalyst for the occupation of Lewis acid sites and active sites. Meanwhile, it can change the characteristics of catalyst surface, resulting in sulfur existing form transforming from inefficient S8 catalyst to inactive S3. Thus, lead to a decrease of deposited inefficient S8 catalyst content. Consequently, decrease the catalytic activity.

中文翻译:

MgAlCe层状双金属氢氧化物在混合良好的含Ce稀土催化剂上H 2 S选择性催化氧化性能的见解

合成了一系列得自层状双氢氧化物的充分混合的含Ce的MgAlCe稀土催化剂,并进行了H 2 S选择性催化氧化的测试。特别地,在催化剂表面上不存在化学吸附的O空位,而是固有的缺陷位点。值得注意的是,该催化剂在相对较低的温度下表现出优异的催化活性,合理的耐久性和出色的硫选择性(100%)。此外,催化剂遵循逐步机理,并且催化剂失活主要是由于与H将Ce 4+还原为Ce 3+的速率相比,O 2将Ce 3+氧化为Ce 4+的速率较慢。2个特别是,添加的水,路易斯碱,可以与效率低下的S 8催化剂竞争,占据路易斯酸位和活性位。同时,它可以改变催化剂表面的特性,导致存在的硫形式从无效的S 8催化剂转变为惰性S 3。因此,导致沉积的无效S 8催化剂含量的降低。因此,降低了催化活性。
更新日期:2017-09-10
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