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首页> 外文期刊>Catalysis science & technology >Dopant-driven tuning of toluene oxidation and sulfur resistance at the B-site of LaCo1-xMxO3 (M = Fe, Cr, Cu) perovskites
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Dopant-driven tuning of toluene oxidation and sulfur resistance at the B-site of LaCo1-xMxO3 (M = Fe, Cr, Cu) perovskites

机译:在LACO1-XMXO3(M = Fe,Cr,Cu)perovskites的B点上,甲苯氧化和硫耐药性的掺杂驱动调整

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The objective of this work was to investigate and contrast the mechanism of different B-site dopants for catalytic activity and sulfur resistance under equivalent conditions. LaCo1-xMxO3 (M = Fe, Cr, Cu) perovskite-type catalysts were synthesized by a sol-gel method, and the optimized samples were tested for toluene oxidation before and after sulfur aging. The properties of the catalysts were investigated in detail by XRD, FT-IR, N-2 adsorption-desorption, H-2-TPR, XPS and in situ DRIFTS to elucidate the inner mechanisms of the catalytic reaction and poisoning processes. The results indicated that introducing specific metal cations with a suitable ratio into the B-site of perovskite could improve the catalytic activity and weaken the negative effect of SO2 poisoning. The reasons for the improvement of catalytic activity on different doped catalysts are similar and mainly lie in the change of reduction property, oxidation state of the B-site, and content of oxygen vacancies. However, the mechanism of sulfur resistance caused by different dopants is not identical. The introduction of different metal cations will cause certain differences in some factors such as reducibility, lattice stability, sulfur adsorption and sulfate content, thus leading to the differentiation of sulfur tolerance for doped perovskite catalysts. In this study, the optimization effect of Fe dopant is better than that of Cr and Cu dopants, illustrating that the high stability of the perovskite lattice and the insensitivity to sulfur species are the key factors for its outstanding sulfur resistance. The results provide insights into guiding the practical composition and life cycle optimization of perovskite-type catalysts in the industrial application of removing sulfur-containing VOCs.
机译:这项工作的目的是调查和对比不同B位掺杂剂在等效条件下催化活性和硫的机理。 LACO1-XMXO3(M = Fe,Cr,Cu)通过SOL-GEL方法合成钙钛矿型催化剂,并在硫衰老之前和之后测试了优化的样品以进行甲苯氧化。 XRD,FT-IR,N-2吸附 - 吸附,H-2-TPR,XP和原位漂移详细研究了催化剂的性能,以阐明催化反应和中毒过程的内部机制。结果表明,将适当比率的特定金属阳离子引入钙钛矿的B位可以改善催化活性并削弱SO2中毒的负面影响。改善不同掺杂催化剂的催化活性的原因是相似的,主要在于还原性质的变化,B位点的氧化状态以及氧空位的含量。但是,由不同掺杂剂引起的硫耐性机理并不相同。引入不同的金属阳离子将在某些因素上引起一定的差异,例如降低性,晶格稳定性,硫吸附和硫酸盐含量,从而导致掺杂的钙钛矿催化剂的硫耐受性的分化。在这项研究中,Fe掺杂剂的优化效果比CR和Cu掺杂剂的优化效果更好,这表明钙钛矿晶格的高稳定性和对硫物种的不敏感性是其出色的硫耐性的关键因素。结果为指导钙钛矿型催化剂的实用组成和生命周期优化提供了见解,该催化剂在去除含硫的VOC的工业应用中。

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