Sui Wan , Thomas Häber , Patrick Lott , Rainer Suntz , Olaf Deutschmann
{"title":"平面激光诱导荧光法研究H2在Pd上还原NO的实验研究","authors":"Sui Wan , Thomas Häber , Patrick Lott , Rainer Suntz , Olaf Deutschmann","doi":"10.1016/j.jaecs.2023.100229","DOIUrl":null,"url":null,"abstract":"<div><p>This study investigates the NO reduction by H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> on a Pd/Al<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span> catalyst in a temperature range of 100–300 °C and NO/H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> ratios from 0.5–2, aiming to gain a deeper understanding of the reaction kinetics and its interaction with mass transfer. Planar laser-induced fluorescence (PLIF) is used to visualize the NO distributions over the catalyst, supplemented by end-of-pipe gas analysis of other components. The reduced Pd-based catalyst undergoes a slow deactivation after exposure to the reactive flow, leading to reduced overall NO conversion and decreased selectivity towards N<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>. The NO-PLIF measurements are only conducted on the reduced catalyst without considering the temporal evolutions. Despite the overall NO conversion varying only around 50%–65% across all the investigated conditions, the spatially resolved NO distributions reveal three distinct regimes that limit the overall NO conversion: the regime governed by intrinsic reaction rates, the regime constrained by H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> availability, and the regime restricted by NO diffusion. These findings, demonstrating the interaction between reaction kinetics and mass transfer over a heterogeneous catalyst, highlight the significance of analyzing spatially resolved concentration distributions obtained through PLIF measurements. This approach complements the conventional end-of-pipe analysis, offering a more comprehensive understanding of the underlying processes.</p></div>","PeriodicalId":100104,"journal":{"name":"Applications in Energy and Combustion Science","volume":"16 ","pages":"Article 100229"},"PeriodicalIF":5.0000,"publicationDate":"2023-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2666352X23001188/pdfft?md5=f350afcb0ae319ac856fda6548ec8631&pid=1-s2.0-S2666352X23001188-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Experimental investigation of NO reduction by H2 on Pd using planar laser-induced fluorescence\",\"authors\":\"Sui Wan , Thomas Häber , Patrick Lott , Rainer Suntz , Olaf Deutschmann\",\"doi\":\"10.1016/j.jaecs.2023.100229\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>This study investigates the NO reduction by H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> on a Pd/Al<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>O<span><math><msub><mrow></mrow><mrow><mn>3</mn></mrow></msub></math></span> catalyst in a temperature range of 100–300 °C and NO/H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> ratios from 0.5–2, aiming to gain a deeper understanding of the reaction kinetics and its interaction with mass transfer. Planar laser-induced fluorescence (PLIF) is used to visualize the NO distributions over the catalyst, supplemented by end-of-pipe gas analysis of other components. The reduced Pd-based catalyst undergoes a slow deactivation after exposure to the reactive flow, leading to reduced overall NO conversion and decreased selectivity towards N<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span>. The NO-PLIF measurements are only conducted on the reduced catalyst without considering the temporal evolutions. Despite the overall NO conversion varying only around 50%–65% across all the investigated conditions, the spatially resolved NO distributions reveal three distinct regimes that limit the overall NO conversion: the regime governed by intrinsic reaction rates, the regime constrained by H<span><math><msub><mrow></mrow><mrow><mn>2</mn></mrow></msub></math></span> availability, and the regime restricted by NO diffusion. These findings, demonstrating the interaction between reaction kinetics and mass transfer over a heterogeneous catalyst, highlight the significance of analyzing spatially resolved concentration distributions obtained through PLIF measurements. This approach complements the conventional end-of-pipe analysis, offering a more comprehensive understanding of the underlying processes.</p></div>\",\"PeriodicalId\":100104,\"journal\":{\"name\":\"Applications in Energy and Combustion Science\",\"volume\":\"16 \",\"pages\":\"Article 100229\"},\"PeriodicalIF\":5.0000,\"publicationDate\":\"2023-12-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2666352X23001188/pdfft?md5=f350afcb0ae319ac856fda6548ec8631&pid=1-s2.0-S2666352X23001188-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applications in Energy and Combustion Science\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2666352X23001188\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applications in Energy and Combustion Science","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2666352X23001188","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Experimental investigation of NO reduction by H2 on Pd using planar laser-induced fluorescence
This study investigates the NO reduction by H on a Pd/AlO catalyst in a temperature range of 100–300 °C and NO/H ratios from 0.5–2, aiming to gain a deeper understanding of the reaction kinetics and its interaction with mass transfer. Planar laser-induced fluorescence (PLIF) is used to visualize the NO distributions over the catalyst, supplemented by end-of-pipe gas analysis of other components. The reduced Pd-based catalyst undergoes a slow deactivation after exposure to the reactive flow, leading to reduced overall NO conversion and decreased selectivity towards N. The NO-PLIF measurements are only conducted on the reduced catalyst without considering the temporal evolutions. Despite the overall NO conversion varying only around 50%–65% across all the investigated conditions, the spatially resolved NO distributions reveal three distinct regimes that limit the overall NO conversion: the regime governed by intrinsic reaction rates, the regime constrained by H availability, and the regime restricted by NO diffusion. These findings, demonstrating the interaction between reaction kinetics and mass transfer over a heterogeneous catalyst, highlight the significance of analyzing spatially resolved concentration distributions obtained through PLIF measurements. This approach complements the conventional end-of-pipe analysis, offering a more comprehensive understanding of the underlying processes.