Hongzhe Zhao, Zhitao Han*, Shaosi Cheng, You Tian, Qingliang Zeng, Yeshan Li and Dong Ma,
{"title":"用于氨的选择性催化氧化的 Ru 改性 Ce0.7Zr0.3Ox 催化剂的催化活性和反应机理","authors":"Hongzhe Zhao, Zhitao Han*, Shaosi Cheng, You Tian, Qingliang Zeng, Yeshan Li and Dong Ma, ","doi":"10.1021/acs.energyfuels.4c0373910.1021/acs.energyfuels.4c03739","DOIUrl":null,"url":null,"abstract":"<p >To solve the problem of the poor low-temperature NH<sub>3</sub> selective catalytic oxidation (NH<sub>3</sub>–SCO) performance of CeZrO<sub><i>x</i></sub> catalysts, a series of Ru/CeZrO<sub><i>x</i></sub> catalysts with various Ru mass ratios were prepared via the impregnation–precipitation method. The introduction of Ru could significantly improve the low-temperature catalytic performance of CeZrO<sub><i>x</i></sub> catalysts from activity test results. Among prepared catalysts, the catalyst with a Ru mass ratio of 0.5 wt % and a Ce/Zr molar ratio of 7:3 (denoted as Ru<sub>0.5</sub>/CZO) was considered to have an excellent NH<sub>3</sub>–SCO performance; NH<sub>3</sub> conversion reached 100 and 91.2% N<sub>2</sub> selectivity at 237 °C. Physicochemical properties of Ru<sub>0.5</sub>/CZO and CZO catalysts were compared through a series of characterization tests to investigate the relationship between the introduction of Ru and the NH<sub>3</sub>–SCO performance. H<sub>2</sub>-TPR results revealed an interaction between the Ru and Ce species. The introduction of Ru significantly shifted the reduction peak toward the lower-temperature direction, enhancing the low-temperature redox performance of the CZO catalyst. NH<sub>3</sub>-TPD results indicated that Ru<sub>0.5</sub>/CZO catalysts had abundant acid sites on its surface, facilitating NH<sub>3</sub> adsorption and oxidation. In situ DRIFTS characterization results indicated that the reaction mechanism of the Ru<sub>0.5</sub>/CZO catalyst might be both internal-selective catalytic reduction (i-SCR) and imine (−NH) mechanisms.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"38 22","pages":"22440–22449 22440–22449"},"PeriodicalIF":5.2000,"publicationDate":"2024-11-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Catalytic Activity and Reaction Mechanism of Ru-Modified Ce0.7Zr0.3Ox Catalysts for Selective Catalytic Oxidation of Ammonia\",\"authors\":\"Hongzhe Zhao, Zhitao Han*, Shaosi Cheng, You Tian, Qingliang Zeng, Yeshan Li and Dong Ma, \",\"doi\":\"10.1021/acs.energyfuels.4c0373910.1021/acs.energyfuels.4c03739\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >To solve the problem of the poor low-temperature NH<sub>3</sub> selective catalytic oxidation (NH<sub>3</sub>–SCO) performance of CeZrO<sub><i>x</i></sub> catalysts, a series of Ru/CeZrO<sub><i>x</i></sub> catalysts with various Ru mass ratios were prepared via the impregnation–precipitation method. The introduction of Ru could significantly improve the low-temperature catalytic performance of CeZrO<sub><i>x</i></sub> catalysts from activity test results. Among prepared catalysts, the catalyst with a Ru mass ratio of 0.5 wt % and a Ce/Zr molar ratio of 7:3 (denoted as Ru<sub>0.5</sub>/CZO) was considered to have an excellent NH<sub>3</sub>–SCO performance; NH<sub>3</sub> conversion reached 100 and 91.2% N<sub>2</sub> selectivity at 237 °C. Physicochemical properties of Ru<sub>0.5</sub>/CZO and CZO catalysts were compared through a series of characterization tests to investigate the relationship between the introduction of Ru and the NH<sub>3</sub>–SCO performance. H<sub>2</sub>-TPR results revealed an interaction between the Ru and Ce species. The introduction of Ru significantly shifted the reduction peak toward the lower-temperature direction, enhancing the low-temperature redox performance of the CZO catalyst. NH<sub>3</sub>-TPD results indicated that Ru<sub>0.5</sub>/CZO catalysts had abundant acid sites on its surface, facilitating NH<sub>3</sub> adsorption and oxidation. In situ DRIFTS characterization results indicated that the reaction mechanism of the Ru<sub>0.5</sub>/CZO catalyst might be both internal-selective catalytic reduction (i-SCR) and imine (−NH) mechanisms.</p>\",\"PeriodicalId\":35,\"journal\":{\"name\":\"Energy & Fuels\",\"volume\":\"38 22\",\"pages\":\"22440–22449 22440–22449\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2024-11-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy & Fuels\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c03739\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy & Fuels","FirstCategoryId":"5","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.energyfuels.4c03739","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Catalytic Activity and Reaction Mechanism of Ru-Modified Ce0.7Zr0.3Ox Catalysts for Selective Catalytic Oxidation of Ammonia
To solve the problem of the poor low-temperature NH3 selective catalytic oxidation (NH3–SCO) performance of CeZrOx catalysts, a series of Ru/CeZrOx catalysts with various Ru mass ratios were prepared via the impregnation–precipitation method. The introduction of Ru could significantly improve the low-temperature catalytic performance of CeZrOx catalysts from activity test results. Among prepared catalysts, the catalyst with a Ru mass ratio of 0.5 wt % and a Ce/Zr molar ratio of 7:3 (denoted as Ru0.5/CZO) was considered to have an excellent NH3–SCO performance; NH3 conversion reached 100 and 91.2% N2 selectivity at 237 °C. Physicochemical properties of Ru0.5/CZO and CZO catalysts were compared through a series of characterization tests to investigate the relationship between the introduction of Ru and the NH3–SCO performance. H2-TPR results revealed an interaction between the Ru and Ce species. The introduction of Ru significantly shifted the reduction peak toward the lower-temperature direction, enhancing the low-temperature redox performance of the CZO catalyst. NH3-TPD results indicated that Ru0.5/CZO catalysts had abundant acid sites on its surface, facilitating NH3 adsorption and oxidation. In situ DRIFTS characterization results indicated that the reaction mechanism of the Ru0.5/CZO catalyst might be both internal-selective catalytic reduction (i-SCR) and imine (−NH) mechanisms.
期刊介绍:
Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.