Lanyi Wang , Mengxia You , Xinyu Chen , Shengran Zhou , Dong Li , Di Yu , Chunlei Zhang , Siyu Gao , Xuehua Yu , Bing Liu , Xiaoqiang Fan , Chengyang Yin , Zhen Zhao
{"title":"树莓状 MnOx/Cu-SSZ-13 催化剂:同时去除烟尘和氮氧化物的简便制备、催化性能和反应机理","authors":"Lanyi Wang , Mengxia You , Xinyu Chen , Shengran Zhou , Dong Li , Di Yu , Chunlei Zhang , Siyu Gao , Xuehua Yu , Bing Liu , Xiaoqiang Fan , Chengyang Yin , Zhen Zhao","doi":"10.1016/j.fuel.2024.133862","DOIUrl":null,"url":null,"abstract":"<div><div>n%MnOx/Cu-SSZ-13 catalysts with raspberry-like shapes were synthesized using the steam-assisted method and incipient impregnation methods. The catalytic activities of as-prepared catalysts were also tested for the simultaneous removal of soot and nitrogen oxides (NOx), and the 40 %MnOx/Cu-SSZ-13 catalyst exhibited the best catalytic performance with the lowest T<sub>m</sub> temperature (455 °C) for soot combustion, the widest temperature window (144–417 °C) for NO conversion (>90 %), and the highest N<sub>2</sub> selectivity (96 %). The obtained catalyst achieves the efficient elimination of NOx and soot in the temperature range of diesel vehicle exhaust emissions because of its rich active oxygen species, sufficient acidic sites, excellent redox properties, high proportion of surface Mn<sup>4+</sup>, and unique raspberry-like structure. Moreover, the active sites involved in the removal of soot and NOx and reaction mechanism were also elucidated according to the results of density functional theory (DFT) calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs). The results shows that Mn<sub>2</sub>O<sub>3</sub> is the active phase for soot oxidation, while Cu-SSZ-13 is the best choice of active phase for NH<sub>3</sub> selective catalytic reduction (NH<sub>3</sub>-SCR). And the existence of Mn<sub>2</sub>O<sub>3</sub> promotes the reduction of NO on Cu-SSZ-13. Additionally, the 40 %MnOx/Cu-SSZ-13 catalyst followed the E-R mechanism in NH<sub>3</sub>-SCR at low temperatures as well as NO<sub>2</sub>-assisted mechanism and the active oxygen mechanism in soot combustion at high temperatures.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"382 ","pages":"Article 133862"},"PeriodicalIF":6.7000,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Raspberry-like shape MnOx/Cu-SSZ-13 catalysts: Facile preparation, catalytic performance and reaction mechanism for the simultaneous removal of soot and NOx\",\"authors\":\"Lanyi Wang , Mengxia You , Xinyu Chen , Shengran Zhou , Dong Li , Di Yu , Chunlei Zhang , Siyu Gao , Xuehua Yu , Bing Liu , Xiaoqiang Fan , Chengyang Yin , Zhen Zhao\",\"doi\":\"10.1016/j.fuel.2024.133862\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>n%MnOx/Cu-SSZ-13 catalysts with raspberry-like shapes were synthesized using the steam-assisted method and incipient impregnation methods. The catalytic activities of as-prepared catalysts were also tested for the simultaneous removal of soot and nitrogen oxides (NOx), and the 40 %MnOx/Cu-SSZ-13 catalyst exhibited the best catalytic performance with the lowest T<sub>m</sub> temperature (455 °C) for soot combustion, the widest temperature window (144–417 °C) for NO conversion (>90 %), and the highest N<sub>2</sub> selectivity (96 %). The obtained catalyst achieves the efficient elimination of NOx and soot in the temperature range of diesel vehicle exhaust emissions because of its rich active oxygen species, sufficient acidic sites, excellent redox properties, high proportion of surface Mn<sup>4+</sup>, and unique raspberry-like structure. Moreover, the active sites involved in the removal of soot and NOx and reaction mechanism were also elucidated according to the results of density functional theory (DFT) calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs). The results shows that Mn<sub>2</sub>O<sub>3</sub> is the active phase for soot oxidation, while Cu-SSZ-13 is the best choice of active phase for NH<sub>3</sub> selective catalytic reduction (NH<sub>3</sub>-SCR). And the existence of Mn<sub>2</sub>O<sub>3</sub> promotes the reduction of NO on Cu-SSZ-13. Additionally, the 40 %MnOx/Cu-SSZ-13 catalyst followed the E-R mechanism in NH<sub>3</sub>-SCR at low temperatures as well as NO<sub>2</sub>-assisted mechanism and the active oxygen mechanism in soot combustion at high temperatures.</div></div>\",\"PeriodicalId\":325,\"journal\":{\"name\":\"Fuel\",\"volume\":\"382 \",\"pages\":\"Article 133862\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2024-11-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0016236124030126\",\"RegionNum\":1,\"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":"Fuel","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0016236124030126","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Raspberry-like shape MnOx/Cu-SSZ-13 catalysts: Facile preparation, catalytic performance and reaction mechanism for the simultaneous removal of soot and NOx
n%MnOx/Cu-SSZ-13 catalysts with raspberry-like shapes were synthesized using the steam-assisted method and incipient impregnation methods. The catalytic activities of as-prepared catalysts were also tested for the simultaneous removal of soot and nitrogen oxides (NOx), and the 40 %MnOx/Cu-SSZ-13 catalyst exhibited the best catalytic performance with the lowest Tm temperature (455 °C) for soot combustion, the widest temperature window (144–417 °C) for NO conversion (>90 %), and the highest N2 selectivity (96 %). The obtained catalyst achieves the efficient elimination of NOx and soot in the temperature range of diesel vehicle exhaust emissions because of its rich active oxygen species, sufficient acidic sites, excellent redox properties, high proportion of surface Mn4+, and unique raspberry-like structure. Moreover, the active sites involved in the removal of soot and NOx and reaction mechanism were also elucidated according to the results of density functional theory (DFT) calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs). The results shows that Mn2O3 is the active phase for soot oxidation, while Cu-SSZ-13 is the best choice of active phase for NH3 selective catalytic reduction (NH3-SCR). And the existence of Mn2O3 promotes the reduction of NO on Cu-SSZ-13. Additionally, the 40 %MnOx/Cu-SSZ-13 catalyst followed the E-R mechanism in NH3-SCR at low temperatures as well as NO2-assisted mechanism and the active oxygen mechanism in soot combustion at high temperatures.
期刊介绍:
The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.