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The dual effects of ammonium bisulfate on the selective catalytic reduction of NO with NH3 over Fe2O3-WO3 catalyst confined in MCM-41

[Display omitted] •The dual effects of ABS on NH3-SCR performance of Fe2O3-WO3/MCM-41 is observed and illustrated for the first time.•The formation of surface metal sulfates sustainably promotes the catalytic performance.•Nearly 90% of sulfates in ABS are immobilized after NH4+ consumption.•Both the...

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Published in:Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2020-06, Vol.389, p.124271, Article 124271
Main Authors: Guo, Kai, Zhu, Yuxiang, Yan, Zhen, Liu, Annai, Du, Xiangze, Wang, Xin, Tan, Wei, Li, Lulu, Sun, Jingfang, Tong, Qing, Tang, Changjin, Dong, Lin
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cited_by cdi_FETCH-LOGICAL-c297t-7e120e4b3371274d0664499094584eca1242df4c3232204834f67fb35b1ba6fa3
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container_title Chemical engineering journal (Lausanne, Switzerland : 1996)
container_volume 389
creator Guo, Kai
Zhu, Yuxiang
Yan, Zhen
Liu, Annai
Du, Xiangze
Wang, Xin
Tan, Wei
Li, Lulu
Sun, Jingfang
Tong, Qing
Tang, Changjin
Dong, Lin
description [Display omitted] •The dual effects of ABS on NH3-SCR performance of Fe2O3-WO3/MCM-41 is observed and illustrated for the first time.•The formation of surface metal sulfates sustainably promotes the catalytic performance.•Nearly 90% of sulfates in ABS are immobilized after NH4+ consumption.•Both the acidity and redox properties of catalyst are greatly improved after metal sulfates formation. Ammonium bisulfate (ABS) has long been considered as a main poisoning material in the selective catalytic reduction by NH3 (NH3-SCR) due to the inevitable coverage of sticky ABS on catalytic active sites in sulfur-containing atmospheres, which severely hinders the achievement of stable and highly active NH3-SCR catalysts. In the present study, we report a novel observation of the dual effects of ABS on the NH3-SCR reaction. That is, ABS inhibits the NH3-SCR performance of Fe2O3-WO3/MCM-41 catalyst at low temperatures (50–200 °C) but shows apparent and sustainable reaction promotion when the temperature surpasses 250 °C. X-ray photoelectron spectroscopy (XPS) and NO probing adsorption confirmed that when ABS is deposited on the catalyst surface, a partial interaction between ABS and the Fe2O3-WO3 component occurs, resulting in blocking of the active sites and an obvious loss of catalytic activity. With increasing reaction temperature, the ammonium in ABS can be facilely consumed by NO/O2, thus inducing the disintegration of poisoning species. The sulfate group transforms into metal sulfate and survives at high temperatures. Importantly, owing to the strong inductive effect of sulfate species, both the acidity and redox properties of the catalyst are greatly improved, which contributes to the enhanced activity. The results of the present study expand our knowledge of the role of ABS in the NH3-SCR reaction and will be useful for designing high-performing NH3-SCR catalysts.
doi_str_mv 10.1016/j.cej.2020.124271
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Ammonium bisulfate (ABS) has long been considered as a main poisoning material in the selective catalytic reduction by NH3 (NH3-SCR) due to the inevitable coverage of sticky ABS on catalytic active sites in sulfur-containing atmospheres, which severely hinders the achievement of stable and highly active NH3-SCR catalysts. In the present study, we report a novel observation of the dual effects of ABS on the NH3-SCR reaction. That is, ABS inhibits the NH3-SCR performance of Fe2O3-WO3/MCM-41 catalyst at low temperatures (50–200 °C) but shows apparent and sustainable reaction promotion when the temperature surpasses 250 °C. X-ray photoelectron spectroscopy (XPS) and NO probing adsorption confirmed that when ABS is deposited on the catalyst surface, a partial interaction between ABS and the Fe2O3-WO3 component occurs, resulting in blocking of the active sites and an obvious loss of catalytic activity. With increasing reaction temperature, the ammonium in ABS can be facilely consumed by NO/O2, thus inducing the disintegration of poisoning species. The sulfate group transforms into metal sulfate and survives at high temperatures. Importantly, owing to the strong inductive effect of sulfate species, both the acidity and redox properties of the catalyst are greatly improved, which contributes to the enhanced activity. 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Ammonium bisulfate (ABS) has long been considered as a main poisoning material in the selective catalytic reduction by NH3 (NH3-SCR) due to the inevitable coverage of sticky ABS on catalytic active sites in sulfur-containing atmospheres, which severely hinders the achievement of stable and highly active NH3-SCR catalysts. In the present study, we report a novel observation of the dual effects of ABS on the NH3-SCR reaction. That is, ABS inhibits the NH3-SCR performance of Fe2O3-WO3/MCM-41 catalyst at low temperatures (50–200 °C) but shows apparent and sustainable reaction promotion when the temperature surpasses 250 °C. X-ray photoelectron spectroscopy (XPS) and NO probing adsorption confirmed that when ABS is deposited on the catalyst surface, a partial interaction between ABS and the Fe2O3-WO3 component occurs, resulting in blocking of the active sites and an obvious loss of catalytic activity. With increasing reaction temperature, the ammonium in ABS can be facilely consumed by NO/O2, thus inducing the disintegration of poisoning species. The sulfate group transforms into metal sulfate and survives at high temperatures. Importantly, owing to the strong inductive effect of sulfate species, both the acidity and redox properties of the catalyst are greatly improved, which contributes to the enhanced activity. 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Ammonium bisulfate (ABS) has long been considered as a main poisoning material in the selective catalytic reduction by NH3 (NH3-SCR) due to the inevitable coverage of sticky ABS on catalytic active sites in sulfur-containing atmospheres, which severely hinders the achievement of stable and highly active NH3-SCR catalysts. In the present study, we report a novel observation of the dual effects of ABS on the NH3-SCR reaction. That is, ABS inhibits the NH3-SCR performance of Fe2O3-WO3/MCM-41 catalyst at low temperatures (50–200 °C) but shows apparent and sustainable reaction promotion when the temperature surpasses 250 °C. X-ray photoelectron spectroscopy (XPS) and NO probing adsorption confirmed that when ABS is deposited on the catalyst surface, a partial interaction between ABS and the Fe2O3-WO3 component occurs, resulting in blocking of the active sites and an obvious loss of catalytic activity. With increasing reaction temperature, the ammonium in ABS can be facilely consumed by NO/O2, thus inducing the disintegration of poisoning species. The sulfate group transforms into metal sulfate and survives at high temperatures. Importantly, owing to the strong inductive effect of sulfate species, both the acidity and redox properties of the catalyst are greatly improved, which contributes to the enhanced activity. The results of the present study expand our knowledge of the role of ABS in the NH3-SCR reaction and will be useful for designing high-performing NH3-SCR catalysts.</abstract><pub>Elsevier B.V</pub><doi>10.1016/j.cej.2020.124271</doi><orcidid>https://orcid.org/0000-0001-8626-5509</orcidid></addata></record>
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subjects Ammonium bisulfate
Fe2O3-WO3 catalyst
Metal sulfate
NH3-SCR
Sulfur-resistant
title The dual effects of ammonium bisulfate on the selective catalytic reduction of NO with NH3 over Fe2O3-WO3 catalyst confined in MCM-41
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