Dezhou Luo , Na Zhang , Chunying Chen , Zhi Chen , Sisi Qin , Qin He , Zhengzheng Yang
{"title":"利用铈-氧化锆-镨固溶体的结构缺陷来催化消除柴油机烟尘","authors":"Dezhou Luo , Na Zhang , Chunying Chen , Zhi Chen , Sisi Qin , Qin He , Zhengzheng Yang","doi":"10.1016/j.mcat.2024.114623","DOIUrl":null,"url":null,"abstract":"<div><div>Creating structure defects in ceria-based solid solution catalysts is a crucial yet challenging task. Herein, urea-assisted synthesis strategy was designed for ceria-zirconia-praseodymia catalyst (CeZrPrO<sub>x</sub>) to create lattice defects; its effects on catalyst structure, physical-chemical properties and catalytic diesel soot purification activity were systematically investigated. Raman and X-ray photoelectron spectroscopy (XPS) findings indicate that the urea-assisted synthesized catalyst (CeZrPrO<sub>x</sub>-U) has remarkably more Ce<sup>3+</sup> proportion (structure defects), oxygen vacancies and surface reactive oxygen species (O<sub>2</sub><sup>2-</sup> and O<sup>2-</sup>). Temperature-programmed reduction by hydrogen (H<sub>2</sub>-TPR) and temperature-programmed desorption by oxygen (O<sub>2</sub>-TPD) results further prove that the oxygen migration of the CeZrPrO<sub>x</sub>-U is definitely enhanced. Compared to the conventional CeZrPrO<sub>x</sub> catalyst, the bulk lattice oxygen of the CeZrPrO<sub>x</sub>-U can be migrated to the surface to generate surface reactive oxygen species more easily. As a consequence, the prepared CeZrPrO<sub>x</sub>-U catalyst exhibits obviously better catalytic diesel soot purification activity. Therefore, this study suggests that engineering the structure defects in CeZrPrO<sub>x</sub> catalyst is an effective approach to improve physical-chemical properties and enhance the soot catalytic elimination activity of the catalyst.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"569 ","pages":""},"PeriodicalIF":3.9000,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Engineering the structure defects of ceria-zirconia-praseodymia solid solutions for diesel soot catalytic elimination\",\"authors\":\"Dezhou Luo , Na Zhang , Chunying Chen , Zhi Chen , Sisi Qin , Qin He , Zhengzheng Yang\",\"doi\":\"10.1016/j.mcat.2024.114623\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Creating structure defects in ceria-based solid solution catalysts is a crucial yet challenging task. Herein, urea-assisted synthesis strategy was designed for ceria-zirconia-praseodymia catalyst (CeZrPrO<sub>x</sub>) to create lattice defects; its effects on catalyst structure, physical-chemical properties and catalytic diesel soot purification activity were systematically investigated. Raman and X-ray photoelectron spectroscopy (XPS) findings indicate that the urea-assisted synthesized catalyst (CeZrPrO<sub>x</sub>-U) has remarkably more Ce<sup>3+</sup> proportion (structure defects), oxygen vacancies and surface reactive oxygen species (O<sub>2</sub><sup>2-</sup> and O<sup>2-</sup>). Temperature-programmed reduction by hydrogen (H<sub>2</sub>-TPR) and temperature-programmed desorption by oxygen (O<sub>2</sub>-TPD) results further prove that the oxygen migration of the CeZrPrO<sub>x</sub>-U is definitely enhanced. Compared to the conventional CeZrPrO<sub>x</sub> catalyst, the bulk lattice oxygen of the CeZrPrO<sub>x</sub>-U can be migrated to the surface to generate surface reactive oxygen species more easily. As a consequence, the prepared CeZrPrO<sub>x</sub>-U catalyst exhibits obviously better catalytic diesel soot purification activity. Therefore, this study suggests that engineering the structure defects in CeZrPrO<sub>x</sub> catalyst is an effective approach to improve physical-chemical properties and enhance the soot catalytic elimination activity of the catalyst.</div></div>\",\"PeriodicalId\":393,\"journal\":{\"name\":\"Molecular Catalysis\",\"volume\":\"569 \",\"pages\":\"\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2024-10-16\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Molecular Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468823124008058\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823124008058","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Engineering the structure defects of ceria-zirconia-praseodymia solid solutions for diesel soot catalytic elimination
Creating structure defects in ceria-based solid solution catalysts is a crucial yet challenging task. Herein, urea-assisted synthesis strategy was designed for ceria-zirconia-praseodymia catalyst (CeZrPrOx) to create lattice defects; its effects on catalyst structure, physical-chemical properties and catalytic diesel soot purification activity were systematically investigated. Raman and X-ray photoelectron spectroscopy (XPS) findings indicate that the urea-assisted synthesized catalyst (CeZrPrOx-U) has remarkably more Ce3+ proportion (structure defects), oxygen vacancies and surface reactive oxygen species (O22- and O2-). Temperature-programmed reduction by hydrogen (H2-TPR) and temperature-programmed desorption by oxygen (O2-TPD) results further prove that the oxygen migration of the CeZrPrOx-U is definitely enhanced. Compared to the conventional CeZrPrOx catalyst, the bulk lattice oxygen of the CeZrPrOx-U can be migrated to the surface to generate surface reactive oxygen species more easily. As a consequence, the prepared CeZrPrOx-U catalyst exhibits obviously better catalytic diesel soot purification activity. Therefore, this study suggests that engineering the structure defects in CeZrPrOx catalyst is an effective approach to improve physical-chemical properties and enhance the soot catalytic elimination activity of the catalyst.
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods