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FeWO 在选择性催化还原 NO 与 NH 中的优异性能:Fe 和 W 之间的相互作用。

Superior Performance of FeWO for the Selective Catalytic Reduction of NO with NH: Interaction between Fe and W.

机构信息

Key Laboratory of Industrial Ecology and Environmental Engineering (MOE), School of Environmental Sciences and Technology, Dalian University of Technology , Linggong Road 2, Dalian, 116024, China.

出版信息

Environ Sci Technol. 2016 Dec 20;50(24):13511-13519. doi: 10.1021/acs.est.6b03589. Epub 2016 Dec 5.

Abstract

Novel iron-tungsten catalysts were first developed for the selective catalytic reduction of NO by NH in diesel exhaust, achieving an excellent performance with a wide operating temperature window above 90% NO conversion from 225 or 250 to 450 °C (GHSVs of 30 000 or 50 000 h). It also exhibited a pronounced stability and relatively high NO conversion in the presence of HO, SO and CO. The introduction of W resulted in the formation of α-FeO and FeWO species obtained by HRTEM directly. The synergic effect of two species contributed to the high SCR activity, because of the increased surface acidity and electronic property. The FeWO with octahedral [FeO]/[WO] structure acted as the Brønsted acid sites to form highly active NH species. Combining DFT calculations with XPS and UV-vis results, it was found that the fine electron interaction between α-FeO and FeWO made the electron more easily transfer from W sites to Fe sites, which promoted the formation of NO. Judging by the kinetics and SCR activity studies, the FeWO with an appropriate W amount showed the strongest interaction, and thereby the lowest activation energy of 39 kJ•mol and optimal catalytic activity. These findings would be conducive to the reasonable design of NH-SCR catalysts by adjusting the fabrication.

摘要

新型铁钨催化剂首次被开发用于柴油机尾气中 NH 选择性催化还原 NO,在 225 或 250 至 450°C(30000 或 50000 h-1 的 GHSV)的宽操作温度窗口内实现了优异的性能,NO 转化率超过 90%。它在存在 HO、SO 和 CO 的情况下也表现出明显的稳定性和相对较高的 NO 转化率。W 的引入导致 HRTEM 直接获得α-FeO 和 FeWO 物种的形成。两种物质的协同效应有助于提高 SCR 活性,因为表面酸度和电子特性增加。具有八面体[FeO]/[WO]结构的 FeWO 作为 Brønsted 酸位形成高活性 NH 物种。通过结合 DFT 计算和 XPS 和 UV-vis 结果发现,α-FeO 和 FeWO 之间精细的电子相互作用使得电子更容易从 W 位转移到 Fe 位,从而促进了 NO 的形成。根据动力学和 SCR 活性研究,具有适量 W 的 FeWO 表现出最强的相互作用,因此具有最低的 39 kJ·mol-1 的活化能和最佳的催化活性。这些发现将有助于通过调整制备来合理设计 NH-SCR 催化剂。

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