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深入了解 MgAlCe 层状双氢氧化物衍生的 Ce 含量均匀的稀土催化剂上的 HS 选择性催化氧化性能。

Insight into the HS selective catalytic oxidation performance on well-mixed Ce-containing rare earth catalysts derived from MgAlCe layered double hydroxides.

机构信息

Department of Environmental Nano-Materials, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, PR China; National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 101408, PR China.

Department of Environmental Nano-Materials, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, PR China; National Engineering Laboratory for VOCs Pollution Control Material & Technology, University of Chinese Academy of Sciences, Beijing 101408, PR China.

出版信息

J Hazard Mater. 2018 Jan 15;342:749-757. doi: 10.1016/j.jhazmat.2017.09.014. Epub 2017 Sep 9.

Abstract

A series of well-mixed Ce-containing MgAlCe rare earth catalysts derived from layered double hydroxides were synthesized and tested for HS 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 Ce to Ce by O as compared to the reduction rate of Ce to Ce by HS. Particularly, the added water, a Lewis base, can compete with inefficient S 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 S catalyst to inactive S. Thus, lead to a decrease of deposited inefficient S catalyst content. Consequently, decrease the catalytic activity.

摘要

一系列经过充分混合的 Ce 负载的 MgAlCe 稀土催化剂是由层状双氢氧化物合成并用于 HS 选择性催化氧化的。特别的是,催化剂表面存在的是本征缺陷位,而不是化学吸附的 O 空位。显著的是,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,该催化剂遵循逐步反应机制,催化剂失活主要是由于 Ce 被 O 氧化为 Ce 的速率比 HS 还原 Ce 为 Ce 的速率慢。特别的是,添加的水作为路易斯碱,可以与低效 S 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,导致硫的存在形式从低效 S 催化剂转化为不活跃的 S,从而导致沉积的低效 S 催化剂含量减少。结果,降低了催化活性。

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