The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low Temperature

In this study, four monolithic, vanadium-based catalysts in granular (Vox/TiO<sub>2</sub>), honeycomb-type (Vox-Wox/TiO<sub>2</sub> and Vox-MoOx/TiO<sub>2</sub>), and corrugated forms (Vox-Wox/TiO<sub>2</sub>) were investigated by multiple characteriza...

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Main Authors: Jianwen Lai, Yunfeng Ma, Jiayao Wu, Hong Yu, Xiaodong Li, Xiaoqing Lin
Format: Article
Language:English
Published: MDPI AG 2022-11-01
Series:Catalysts
Subjects:
Online Access:https://www.mdpi.com/2073-4344/12/11/1342
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author Jianwen Lai
Yunfeng Ma
Jiayao Wu
Hong Yu
Xiaodong Li
Xiaoqing Lin
author_facet Jianwen Lai
Yunfeng Ma
Jiayao Wu
Hong Yu
Xiaodong Li
Xiaoqing Lin
author_sort Jianwen Lai
collection DOAJ
description In this study, four monolithic, vanadium-based catalysts in granular (Vox/TiO<sub>2</sub>), honeycomb-type (Vox-Wox/TiO<sub>2</sub> and Vox-MoOx/TiO<sub>2</sub>), and corrugated forms (Vox-Wox/TiO<sub>2</sub>) were investigated by multiple characterization methods (BET, XRF, XPS, XRD, H<sub>2</sub>-TPR, and NH<sub>3</sub>-TPD). Their catalytic performances were evaluated by the oxidation-reduction performance of ortho-dichlorobenzene (o-DCB) and NO/NH<sub>3</sub>. The modification of Wox and MoOx could promote catalytic activity by accelerating the transformation of V<sup>5+</sup>/V<sup>4+</sup> and enriching the strong acid sites. The introduction of NO/NH<sub>3</sub> significantly impaired the o-DCB oxidation, ascribed to the competitive adsorption of reactants on acid sites. The performance of Vox/TiO<sub>2</sub> and Vox-MoOx/TiO<sub>2</sub> catalysts indicated that strong acidity could enhance catalytic abilities over o-DCB and Nox. Nevertheless, the CE (conversion efficiency) of o-DCB was more related to a large BET surface area and a high amount of V<sup>5+</sup> species, while the CE of Nox was more associated with redox ability and Vox surface density. The V<sup>4+</sup>/V<sup>5+</sup> and O<sub>S-A</sub>/O<sub>S-L</sub> ratio increased prominently after the oxidation of o-DCB, indicating that it was the reoxidation of V<sup>4+</sup> species, rather than the supplement of oxygen, that limited the reaction rate. This work revealed catalytic activity was positively affiliated with the surface area, amount of V<sup>5+</sup> species, transformation rate of V<sup>4+</sup>/V<sup>5+</sup>, redox ability, and abundance of strong acid sites. Additionally, the results could guide the selectivity and improvement of industrial low-temperature catalysts for synergistic elimination of chloroaromatic organics and Nox.
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spelling doaj.art-9286bcfa46bf41acb3c626057f5338422023-11-24T04:05:51ZengMDPI AGCatalysts2073-43442022-11-011211134210.3390/catal12111342The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low TemperatureJianwen Lai0Yunfeng Ma1Jiayao Wu2Hong Yu3Xiaodong Li4Xiaoqing Lin5State Key Laboratory for Clean Energy Utilization, Institute for Thermal Power Engineering, Zhejiang University, Hangzhou 310027, ChinaState Key Laboratory for Clean Energy Utilization, Institute for Thermal Power Engineering, Zhejiang University, Hangzhou 310027, ChinaState Key Laboratory for Clean Energy Utilization, Institute for Thermal Power Engineering, Zhejiang University, Hangzhou 310027, ChinaState Key Laboratory for Clean Energy Utilization, Institute for Thermal Power Engineering, Zhejiang University, Hangzhou 310027, ChinaState Key Laboratory for Clean Energy Utilization, Institute for Thermal Power Engineering, Zhejiang University, Hangzhou 310027, ChinaState Key Laboratory for Clean Energy Utilization, Institute for Thermal Power Engineering, Zhejiang University, Hangzhou 310027, ChinaIn this study, four monolithic, vanadium-based catalysts in granular (Vox/TiO<sub>2</sub>), honeycomb-type (Vox-Wox/TiO<sub>2</sub> and Vox-MoOx/TiO<sub>2</sub>), and corrugated forms (Vox-Wox/TiO<sub>2</sub>) were investigated by multiple characterization methods (BET, XRF, XPS, XRD, H<sub>2</sub>-TPR, and NH<sub>3</sub>-TPD). Their catalytic performances were evaluated by the oxidation-reduction performance of ortho-dichlorobenzene (o-DCB) and NO/NH<sub>3</sub>. The modification of Wox and MoOx could promote catalytic activity by accelerating the transformation of V<sup>5+</sup>/V<sup>4+</sup> and enriching the strong acid sites. The introduction of NO/NH<sub>3</sub> significantly impaired the o-DCB oxidation, ascribed to the competitive adsorption of reactants on acid sites. The performance of Vox/TiO<sub>2</sub> and Vox-MoOx/TiO<sub>2</sub> catalysts indicated that strong acidity could enhance catalytic abilities over o-DCB and Nox. Nevertheless, the CE (conversion efficiency) of o-DCB was more related to a large BET surface area and a high amount of V<sup>5+</sup> species, while the CE of Nox was more associated with redox ability and Vox surface density. The V<sup>4+</sup>/V<sup>5+</sup> and O<sub>S-A</sub>/O<sub>S-L</sub> ratio increased prominently after the oxidation of o-DCB, indicating that it was the reoxidation of V<sup>4+</sup> species, rather than the supplement of oxygen, that limited the reaction rate. This work revealed catalytic activity was positively affiliated with the surface area, amount of V<sup>5+</sup> species, transformation rate of V<sup>4+</sup>/V<sup>5+</sup>, redox ability, and abundance of strong acid sites. Additionally, the results could guide the selectivity and improvement of industrial low-temperature catalysts for synergistic elimination of chloroaromatic organics and Nox.https://www.mdpi.com/2073-4344/12/11/13421,2-dichlorobenzeneNH<sub>3</sub>-SCRmodification of Wox and MoOxmonolithic typecommercial catalysts
spellingShingle Jianwen Lai
Yunfeng Ma
Jiayao Wu
Hong Yu
Xiaodong Li
Xiaoqing Lin
The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low Temperature
Catalysts
1,2-dichlorobenzene
NH<sub>3</sub>-SCR
modification of Wox and MoOx
monolithic type
commercial catalysts
title The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low Temperature
title_full The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low Temperature
title_fullStr The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low Temperature
title_full_unstemmed The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low Temperature
title_short The Synergistic Catalysis of Chloroaromatic Organics and NOx over Monolithic Vanadium-Based Catalysts at Low Temperature
title_sort synergistic catalysis of chloroaromatic organics and nox over monolithic vanadium based catalysts at low temperature
topic 1,2-dichlorobenzene
NH<sub>3</sub>-SCR
modification of Wox and MoOx
monolithic type
commercial catalysts
url https://www.mdpi.com/2073-4344/12/11/1342
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