基于酸位点增强的CeO2掺杂WO3复合催化剂用于柴油机尾气脱硝

CeO2-doped WO3 composite catalyst based on acid site enhancement for diesel exhaust gas denitration

  • 摘要: 采用先电沉积后水热的方法将WO3负载于钛网上,后续采用电沉积负载CeO2制备CeO2-WO3/Ti催化剂用于柴油车尾气选择性催化还原(NH3-SCR)脱硝。通过固定床反应装置检测催化剂脱硝性能,考察了电沉积CeO2时间对催化剂脱硝性能的影响,结合SEM、XRD、XPS、H2-TPR、NH3-TPD和原位红外光谱等表征手段分析反应机制。结果表明,在WO3表面进行20 min电沉积CeO2的双组分催化剂NOx转化率提升最明显,在200 ℃时已达到91.89%,250−350 ℃均为100%。双组分催化剂表面负载了WO3纳米棒以及高度分散的CeO2,CeO2的负载引入Ce3+并提高了催化剂化学吸附氧所占比例,但样品对应氧化还原能力没有明显提升。中温段(250−350 ℃)脱硝性能提高的主要原因是复合后CeO2的引入有效增加了弱酸以及中强酸位点数量。

     

    Abstract: Based on the complicated preparation of current diesel vehicle exhaust gas denitration catalysts, an in-situ deposited composite oxide catalyst, CeO2-WO3 mixed oxide catalyst, was prepared by electrodeposition and hydrothermal methods, which was loaded on the titanium mesh and applied to the selective catalytic reduction denitration of diesel vehicle exhaust. Denitration performance of the catalysts was tested by a fixed bed reactor, and the influence of different electrodeposition time of CeO2 was investigated. The results demonstrate that 20 min is the best electrodeposition time of CeO2 (100% NOx conversion at 250−350 ℃). The high dispersion of active CeO2 on WO3 promotes the synergistic effects among different components. The as-prepared catalysts were characterized by SEM, XRD, XPS, H2-TPR, NH3-TPD and in-situ DRIFTS. It is evident that Ce3+ is successfully introduced by loading CeO2, which enhances the chemisorption of oxygen. Meanwhile, the increased acidity including both weak acid and medium-strong acid sites of CeO2-WO3 composite catalyst is observed, which improves the co-adsorption of NH3 on Lewis acid and Brønsted acid simultaneously and facilitates the denitration process. Through the characterization by in-situ DRIFTS, it is elucidated that the NH3-SCR reactions are mainly carried out following the Eley-Rideal (E-R) pathway in a medium-temperature range (250−350 ℃).

     

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