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介孔沸石中 Mn-Ce 氧化物的低温选择性催化还原 NO 的新型屏蔽和协同效应,具有增强的 SO/HO 耐受性。

Novel shielding and synergy effects of Mn-Ce oxides confined in mesoporous zeolite for low temperature selective catalytic reduction of NO with enhanced SO/HO tolerance.

机构信息

Key Laboratory of Jiangxi Province for Environment and Energy Catalysis, College of Chemistry, Nanchang University, 999 Xuefu Road, Nanchang, Jiangxi 330031, China.

School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China.

出版信息

J Hazard Mater. 2020 Sep 5;396:122592. doi: 10.1016/j.jhazmat.2020.122592. Epub 2020 Apr 14.

DOI:10.1016/j.jhazmat.2020.122592
PMID:32298863
Abstract

Nitrogen oxides (NO) are a primary source of air pollutants from combustion of fossil fuels. Though Mn-Ce based catalysts exhibit superior low temperature activities, their water and SO tolerance is inferior to other metal oxide catalysts, due to their strong water adsorption and sulfate species formation tendency at low reaction temperatures. Herein, a confinement strategy was adopted to design and synthesize a novel Mn-Ce based catalyst for selective catalytic reduction of NO with NH. The confined MnCeO catalyst was assembled with a simple one pot method, using a mesoporous zeolite (ZSM-5) as the shell and Mn-Ce oxides as the active core (MnCeO@Z5). Owing to the zeolite shell's shielding effect and the synergy between the alumina-silica zeolite shell's acidic properties and the mixed oxide cores' redox properties, the novel MnCeO@Z5 catalyst displayed enhanced water and SO resistance as compared to the MnCeO supported on ZSM-5 (MnCeO/Z5) and its precursor (MnCeO@Al-SiO). Evidently, the zeolite sheath hinders sulfate species formation, and this phenomenon was further investigated by in situ diffuse reflectance infrared Fourier transform spectroscopy (In situ DRIFTS). The novel shielding and acid-redox synergy effect/strategy adopted in this work can be applied to design other high performance deNO catalysts for air pollution control.

摘要

氮氧化物 (NO) 是化石燃料燃烧产生的主要空气污染物之一。尽管 Mn-Ce 基催化剂在低温下表现出优异的活性,但由于其在低温下具有较强的水吸附性和硫酸盐物种形成倾向,其水和 SO 耐受性不如其他金属氧化物催化剂。本文采用限域策略设计并合成了一种新型 Mn-Ce 基催化剂,用于 NH 选择性催化还原 NO。限域 MnCeO 催化剂采用简单的一锅法组装,以介孔沸石 (ZSM-5) 作为壳层,Mn-Ce 氧化物作为活性核 (MnCeO@Z5)。由于沸石壳的屏蔽作用以及沸石壳的酸性和混合氧化物核的氧化还原性能之间的协同作用,新型 MnCeO@Z5 催化剂表现出比负载在 ZSM-5 上的 MnCeO (MnCeO/Z5) 和其前体 (MnCeO@Al-SiO) 更高的水和 SO 耐受性。显然,沸石护套阻碍了硫酸盐物种的形成,这一现象通过原位漫反射红外傅里叶变换光谱 (In situ DRIFTS) 进一步进行了研究。本工作中采用的新型屏蔽和酸-氧化还原协同效应/策略可应用于设计其他用于空气污染控制的高性能脱硝催化剂。

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