{"title":"水热老化对 CeWOx 上标准和快速 SCR 的影响:关于吸附位点和反应机理的定量研究","authors":"Yanlong Huo, Yu Sun, Kuo Liu, Yunbo Yu, Hong He","doi":"10.1021/acs.iecr.4c02509","DOIUrl":null,"url":null,"abstract":"CeWO<sub><i>x</i></sub> after hydrothermal aging at 700 °C for 10 h exhibited >90% nitrogen oxide (NO<sub><i>x</i></sub>) conversion at 200–450 °C either in the presence or absence of H<sub>2</sub>O during fast selective catalytic reduction of NO<sub><i>x</i></sub> (fast SCR), which was higher than or comparable to other oxide catalysts without hydrothermal aging reported in the literature. Even after hydrothermal aging at 800 °C for 10 h, CeWO<sub><i>x</i></sub> could achieve >80% NO<sub><i>x</i></sub> conversion at 200–400 °C, either in the presence or absence of H<sub>2</sub>O. After hydrothermal aging, the adsorption amounts of NO and NH<sub>3</sub> on aged CeWO<sub><i>x</i></sub> decreased dramatically, and NO activation, nitrate production, and the “nitrite path” (Langmuir–Hinshelwood mechanism) were inhibited, causing a drastic decline in NO<sub><i>x</i></sub> conversion during standard SCR. During fast SCR, although the adsorption amount of NO was low, the interaction between gaseous NO<sub>2</sub> and NH<sub>3</sub> to form NH<sub>4</sub>NO<sub>3</sub> increased the adsorption amounts of NO<sub>2</sub> and NH<sub>3</sub>, compensating for the loss of adsorption sites. NH<sub>4</sub>NO<sub>3</sub> took part in the “NH<sub>4</sub>NO<sub>3</sub> fast path” and “NH<sub>4</sub>NO<sub>3</sub> path” (Eley–Rideal mechanism) and was an important intermediate for obtaining a high activity. These are the reasons why fast SCR maintains an excellent activity. The presence of water inhibited the “nitrite path” and “NH<sub>4</sub>NO<sub>3</sub> path”, leading to decreased NO<sub><i>x</i></sub> conversion.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"21 1","pages":""},"PeriodicalIF":3.9000,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Effects of Hydrothermal Aging on Standard and Fast SCR over CeWOx: A Quantitative Study on Adsorption Sites and Reaction Mechanism\",\"authors\":\"Yanlong Huo, Yu Sun, Kuo Liu, Yunbo Yu, Hong He\",\"doi\":\"10.1021/acs.iecr.4c02509\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"CeWO<sub><i>x</i></sub> after hydrothermal aging at 700 °C for 10 h exhibited >90% nitrogen oxide (NO<sub><i>x</i></sub>) conversion at 200–450 °C either in the presence or absence of H<sub>2</sub>O during fast selective catalytic reduction of NO<sub><i>x</i></sub> (fast SCR), which was higher than or comparable to other oxide catalysts without hydrothermal aging reported in the literature. Even after hydrothermal aging at 800 °C for 10 h, CeWO<sub><i>x</i></sub> could achieve >80% NO<sub><i>x</i></sub> conversion at 200–400 °C, either in the presence or absence of H<sub>2</sub>O. After hydrothermal aging, the adsorption amounts of NO and NH<sub>3</sub> on aged CeWO<sub><i>x</i></sub> decreased dramatically, and NO activation, nitrate production, and the “nitrite path” (Langmuir–Hinshelwood mechanism) were inhibited, causing a drastic decline in NO<sub><i>x</i></sub> conversion during standard SCR. During fast SCR, although the adsorption amount of NO was low, the interaction between gaseous NO<sub>2</sub> and NH<sub>3</sub> to form NH<sub>4</sub>NO<sub>3</sub> increased the adsorption amounts of NO<sub>2</sub> and NH<sub>3</sub>, compensating for the loss of adsorption sites. NH<sub>4</sub>NO<sub>3</sub> took part in the “NH<sub>4</sub>NO<sub>3</sub> fast path” and “NH<sub>4</sub>NO<sub>3</sub> path” (Eley–Rideal mechanism) and was an important intermediate for obtaining a high activity. These are the reasons why fast SCR maintains an excellent activity. The presence of water inhibited the “nitrite path” and “NH<sub>4</sub>NO<sub>3</sub> path”, leading to decreased NO<sub><i>x</i></sub> conversion.\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"21 1\",\"pages\":\"\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2024-11-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial & Engineering Chemistry Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.iecr.4c02509\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial & Engineering Chemistry Research","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1021/acs.iecr.4c02509","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Effects of Hydrothermal Aging on Standard and Fast SCR over CeWOx: A Quantitative Study on Adsorption Sites and Reaction Mechanism
CeWOx after hydrothermal aging at 700 °C for 10 h exhibited >90% nitrogen oxide (NOx) conversion at 200–450 °C either in the presence or absence of H2O during fast selective catalytic reduction of NOx (fast SCR), which was higher than or comparable to other oxide catalysts without hydrothermal aging reported in the literature. Even after hydrothermal aging at 800 °C for 10 h, CeWOx could achieve >80% NOx conversion at 200–400 °C, either in the presence or absence of H2O. After hydrothermal aging, the adsorption amounts of NO and NH3 on aged CeWOx decreased dramatically, and NO activation, nitrate production, and the “nitrite path” (Langmuir–Hinshelwood mechanism) were inhibited, causing a drastic decline in NOx conversion during standard SCR. During fast SCR, although the adsorption amount of NO was low, the interaction between gaseous NO2 and NH3 to form NH4NO3 increased the adsorption amounts of NO2 and NH3, compensating for the loss of adsorption sites. NH4NO3 took part in the “NH4NO3 fast path” and “NH4NO3 path” (Eley–Rideal mechanism) and was an important intermediate for obtaining a high activity. These are the reasons why fast SCR maintains an excellent activity. The presence of water inhibited the “nitrite path” and “NH4NO3 path”, leading to decreased NOx conversion.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.