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...
Main Authors: | , , , , , |
---|---|
Format: | Article |
Language: | English |
Published: |
MDPI AG
2022-11-01
|
Series: | Catalysts |
Subjects: | |
Online Access: | https://www.mdpi.com/2073-4344/12/11/1342 |
_version_ | 1797468790585294848 |
---|---|
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. |
first_indexed | 2024-03-09T19:12:23Z |
format | Article |
id | doaj.art-9286bcfa46bf41acb3c626057f533842 |
institution | Directory Open Access Journal |
issn | 2073-4344 |
language | English |
last_indexed | 2024-03-09T19:12:23Z |
publishDate | 2022-11-01 |
publisher | MDPI AG |
record_format | Article |
series | Catalysts |
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 |
work_keys_str_mv | AT jianwenlai thesynergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT yunfengma thesynergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT jiayaowu thesynergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT hongyu thesynergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT xiaodongli thesynergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT xiaoqinglin thesynergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT jianwenlai synergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT yunfengma synergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT jiayaowu synergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT hongyu synergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT xiaodongli synergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature AT xiaoqinglin synergisticcatalysisofchloroaromaticorganicsandnoxovermonolithicvanadiumbasedcatalystsatlowtemperature |