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揭示氧化铝促进铈钨催化剂用于 NH-SCR 的非凡砷抗性起源。

Unveiling the Remarkable Arsenic Resistance Origin of Alumina Promoted Cerium-Tungsten Catalysts for NH-SCR.

机构信息

School of Space and Environment, Beihang University, Beijing 100191, P. R. China.

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China.

出版信息

Environ Sci Technol. 2020 Nov 17;54(22):14740-14749. doi: 10.1021/acs.est.0c05152. Epub 2020 Nov 5.

Abstract

The deactivation of selective catalytic reduction (SCR) catalysts by arsenic is a serious problem for NH-SCR. However, it is tough to design catalysts with good resistance to arsenic compared to other poisons such as alkali metal, SO, etc., because As not only deteriorates surface acidity but also redox property, causing excessive NO generation. A novel CeO-WO-AlO catalyst is developed with excellent arsenic resistance in this study, which presents only less than 10% activity loss compared to nearly 40% loss for CeO-WO with same arsenic loading (As: 2.1 wt %). Moreover, a significant negative impact on the NO generation for poisoning catalysts from 26.7 to 7.5 ppm has also been found. The characterization results demonstrated that the interaction between cerium and arsenic lead to Lewis acid sites and oxygen vacancies loss as well as unexpected oxidation sites formation. However, the introduction of Al weakens the deactivation effect by replacing cerium to interact with arsenic. Three aspects are proposed for obtaining excellent arsenic-resistant performance: (1) the protection of Lewis acid sites, (2) release of oxygen vacancies from As restriction, and (3) confinement of As oxidizing capacity. This study may provide an effective strategy to design and develop novel virtuous antipoisoning catalysts.

摘要

砷对选择性催化还原(SCR)催化剂的失活是 NH-SCR 的一个严重问题。然而,与其他毒物(如碱金属、SO 等)相比,设计具有良好抗砷能力的催化剂是很困难的,因为砷不仅会降低表面酸度,还会降低氧化还原性能,导致过多的 NO 生成。在本研究中开发了一种新型的 CeO-WO-AlO 催化剂,具有出色的抗砷能力,与相同砷负载量(As:2.1wt%)的 CeO-WO 相比,其活性损失不到 10%(仅损失不到 40%)。此外,还发现对中毒催化剂的 NO 生成有显著的负面影响,从 26.7ppm 降至 7.5ppm。表征结果表明,铈与砷的相互作用导致了路易斯酸位和氧空位的损失以及意想不到的氧化位的形成。然而,引入 Al 会通过取代铈与砷相互作用来削弱失活效应。提出了三个方面来获得优异的抗砷性能:(1)保护路易斯酸位,(2)释放 As 限制的氧空位,(3)限制 As 的氧化能力。本研究可能为设计和开发新型良性抗毒催化剂提供了有效的策略。

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