Decomposition of Heavy Diesel SCR Urea Fluid Adsorbed in Cu/HZSM-5 SCR Catalysts Studied by FTIR Spectroscopy at Ambient Conditions

Reactions Pub Date : 2022-11-11 DOI:10.3390/reactions3040038
C. Tempelman, Brahim el Arkoubi, Jochem Spaan, Ronny Slevani, V. Degirmenci
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Abstract

A method is presented to study the decomposition of urea deposited on Cu/HZSM-5 SCR catalysts and therewith the ability of the Cu/HZSM-5 SCR catalyst to be regenerated when being overdosed with SCR urea fluids during operation. This straightforward laboratory method could speed up calibration of exhaust gas aftertreatment systems. As an example, the removal of adsorbed urea to the SCR substrate due to dosage malfunction is studied. To study the removal of adsorbed urea on the catalyst substrate, FTIR experiments have been conducted to investigate the state of the catalyst. Besides Cu/HZSM-5 also HZSM-5 and CuOx were studied as model compounds to provide more inside on the processes occurring at the Cu/HZSM-5 surface upon urea decomposition. To simulate exposure of the SCR catalyst to overdosing of the urea solution, samples were impregnated with a 32 wt% urea solution, which correlates to that of commercial heavy duty diesel urea solutions. After impregnation, the samples were heated at various temperatures in the 133–400 °C temperature region, typically the operation window of a SCR catalyst. After heating, the samples were cooled to room temperature and measured in FTIR. The obtained spectra were compared with various literature reports to correlate the observed absorption bands to urea, urea related compounds and decomposition compounds. The concentration of these adsorbed species decreases at increased thermolysis temperature and is no longer visible at temperatures >250 °C. Extended heat treatment at 200 °C revealed only minor loss of adsorbents after 6 h and were still observable in the FTIR spectra after 24 h. Urea derived adsorbents were completely removed when simulating catalyst regeneration under SCR operation conditions under continuous air flow with a humidity of 10% and at elevated temperatures (400 °C).
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常压条件下Cu/HZSM-5 SCR催化剂吸附重柴油SCR尿素液分解研究
提出了一种方法,研究了Cu/HZSM-5 SCR催化剂上沉积尿素的分解,以及Cu/HZSM-5 SCR催化剂在运行过程中过量添加SCR尿素液时的再生能力。这种简单的实验室方法可以加快废气后处理系统的校准速度。作为一个例子,研究了由于投加故障导致的SCR基板上吸附尿素的去除。为了研究吸附在催化剂底物上的尿素的去除,进行了FTIR实验来研究催化剂的状态。除Cu/HZSM-5外,还研究了HZSM-5和CuOx作为模型化合物,以提供Cu/HZSM-5表面尿素分解过程的更多内幕。为了模拟SCR催化剂暴露在过量尿素溶液中的情况,将样品浸渍在32%的尿素溶液中,这与商业重型柴油尿素溶液的浸渍量有关。浸渍后,样品在133-400°C的温度范围内加热,通常是SCR催化剂的操作窗口。加热后,将样品冷却至室温,用FTIR进行测量。将所得光谱与各种文献报道进行比较,将所观察到的吸收带与尿素、尿素相关化合物和分解化合物联系起来。这些吸附物质的浓度随着热解温度的升高而降低,并且在温度>250℃时不再可见。在200°C下延长热处理时间,6 h后吸附剂只有少量损失,24 h后在FTIR光谱中仍然可以观察到。在SCR操作条件下,在连续空气流动(湿度为10%)和高温(400°C)下模拟催化剂再生时,尿素衍生吸附剂被完全去除。
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