Anastasia Yu. Molokova, Davide Salusso, Elisa Borfecchia, Fei Wen, Stefano Magliocco, Silvia Bordiga, Ton V. W. Janssens, Kirill A. Lomachenko, Gloria Berlier
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We demonstrate here that the reaction with NO at 200 °C is limited after exposure of the [Cu<small><sub>2</sub></small><small><sup>II</sup></small>(NH<small><sub>3</sub></small>)<small><sub>4</sub></small>O<small><sub>2</sub></small>]<small><sup>2+</sup></small> complex to SO<small><sub>2</sub></small> or SO<small><sub>2</sub></small>/O<small><sub>2</sub></small>. Heating the catalyst to 300 °C in NO restores the reaction, albeit at a significantly lower rate. The lower reactivity towards NO indicates that exposure of [Cu<small><sub>2</sub></small><small><sup>II</sup></small>(NH<small><sub>3</sub></small>)<small><sub>4</sub></small>O<small><sub>2</sub></small>]<small><sup>2+</sup></small> to SO<small><sub>2</sub></small> induces changes in the chemistry of Cu in the catalyst. This implies that poisoning of Cu-chabazite catalysts by SO<small><sub>2</sub></small> is, at least in part, of the chemical nature, and may be not limited to the physical pore blocking.","PeriodicalId":66,"journal":{"name":"Catalysis Science & Technology","volume":null,"pages":null},"PeriodicalIF":4.4000,"publicationDate":"2024-08-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The chemical nature of SO2 poisoning of Cu-CHA-based SCR catalysts for NOx removal in diesel exhausts\",\"authors\":\"Anastasia Yu. Molokova, Davide Salusso, Elisa Borfecchia, Fei Wen, Stefano Magliocco, Silvia Bordiga, Ton V. W. Janssens, Kirill A. 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We demonstrate here that the reaction with NO at 200 °C is limited after exposure of the [Cu<small><sub>2</sub></small><small><sup>II</sup></small>(NH<small><sub>3</sub></small>)<small><sub>4</sub></small>O<small><sub>2</sub></small>]<small><sup>2+</sup></small> complex to SO<small><sub>2</sub></small> or SO<small><sub>2</sub></small>/O<small><sub>2</sub></small>. Heating the catalyst to 300 °C in NO restores the reaction, albeit at a significantly lower rate. The lower reactivity towards NO indicates that exposure of [Cu<small><sub>2</sub></small><small><sup>II</sup></small>(NH<small><sub>3</sub></small>)<small><sub>4</sub></small>O<small><sub>2</sub></small>]<small><sup>2+</sup></small> to SO<small><sub>2</sub></small> induces changes in the chemistry of Cu in the catalyst. 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引用次数: 0
摘要
本研究探讨了二氧化硫暴露对基于铜-茶钒石的 SCR 催化剂催化性能的影响,该催化剂用于柴油机尾气中,通过 NH3-SCR 反应减少氮氧化物的排放。SCR 活性由 NO 与 [Cu2II(NH3)4O2]2+ 中间体的反应决定。该中间体也是对二氧化硫反应活性最高的铜种。我们在此证明,[Cu2II(NH3)4O2]2+ 复合物与 SO2 或 SO2/O2 接触后,在 200 ℃ 下与 NO 的反应受到限制。在 NO 中将催化剂加热至 300 °C,可以恢复反应,但反应速率明显降低。对 NO 较低的反应活性表明,[Cu2II(NH3)4O2]2+ 与 SO2 的接触会引起催化剂中 Cu 化学性质的变化。这意味着二氧化硫对铜-钠钙石催化剂的毒害至少部分是化学性的,可能并不局限于物理孔隙堵塞。
The chemical nature of SO2 poisoning of Cu-CHA-based SCR catalysts for NOx removal in diesel exhausts
This study addresses the impact of SO2 exposure on the catalytic performance of a Cu-chabazite-based SCR catalyst, as used in diesel exhausts, to reduce the emission of NOx through the NH3-SCR reaction. The SCR activity is determined by a reaction of NO with the [Cu2II(NH3)4O2]2+ intermediate. The same intermediate is also the most reactive Cu-species towards SO2. We demonstrate here that the reaction with NO at 200 °C is limited after exposure of the [Cu2II(NH3)4O2]2+ complex to SO2 or SO2/O2. Heating the catalyst to 300 °C in NO restores the reaction, albeit at a significantly lower rate. The lower reactivity towards NO indicates that exposure of [Cu2II(NH3)4O2]2+ to SO2 induces changes in the chemistry of Cu in the catalyst. This implies that poisoning of Cu-chabazite catalysts by SO2 is, at least in part, of the chemical nature, and may be not limited to the physical pore blocking.
期刊介绍:
A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis.
Editor-in-chief: Bert Weckhuysen
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