H2S selective catalytic oxidation over Ce substituted La1−xCexFeO3 perovskite oxides catalyst
H2S selective catalytic oxidation over Ce substituted La1−xCexFeO3 perovskite oxides catalyst
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Ce取代的La1-xCexFeO3钙钛矿氧化物催化剂上的H2S选择性催化氧化
DOI：
10.1016/j.cej.2018.05.050
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发表时间：
2018-09
影响因子：
15.1
通讯作者：
Siqiu Qu
中科院分区：
文献类型：
--
作者：
Fenglian Zhang;Xin Zhang;Guoxia Jiang;Na Li;Zhengping Hao;Siqiu Qu
采用柠檬酸盐溶胶-凝胶法合成了一系列La 1 − xCexFeO 3钙钛矿型催化剂，并考察了其对H2S选择性催化氧化反应的催化性能.结果表明，该催化剂具有较高的催化活性和硫选择性（接近100%），且具有较低的表观活化能。值得注意的是，它可以连续进行70小时，而没有显着的失活。Ce和Fe主要以LaCeFeO 3钙钛矿型氧化物和Ce-Fe固溶体的形式存在。由于Ce-Fe的协同作用，催化剂的还原性能得到了显著提高。更重要的是，Ce的适当取代可以增强催化剂表面的碱性，促进氧空位的形成，从而分别提高H2S吸附性能和晶格氧迁移率。它与改进的还原剂协同作用，共同贡献了优异的催化性能。此外，该反应遵循氧化还原机理，催化剂失活主要是由于硫酸盐物种的形成。此外，加入的水会导致逆克劳斯反应的建立，导致催化剂性能下降。
A series of La1−xCexFeO3perovskite catalysts were synthesized using a citrate sol-gel method and examined for H2S selective catalytic oxidation reaction. It was demonstrated that the catalysts exhibited prominent catalytic activity, outstanding sulfur selectivity (nearly 100%) and particularly low apparent activation energy. Remarkably, it can proceed consecutively for 70 h without notable deactivation. Moreover, Ce and Fe were mainly existed in the form of LaCeFeO3perovskite-type oxides as well as Ce-Fe solid solution. Significantly, catalysts reducibility was improved greatly due to the strongly Ce-Fe synergetic effect. More importantly, a proper substitution of Ce can enhance surface basic properties and facilitate the formation of oxygen vacancies on the catalyst surface, and hence improve H2S adsorbability and lattice oxygen mobility, respectively. It cooperating with the improved reducibility jointly contributed to the excellent catalytic performance. Furthermore, the reaction obeyed a redox mechanism and the catalyst deactivation was due mainly to the formation of sulfate species. Additionally, the added water can lead to the establishment of the reverse Claus reaction, causing the decrease of catalytic performance.
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