Jinfeng Chen, Qingze Zhang, Yuanhong Zhong, Zhaoying Wang, Yakun Guo, Ming Sun, Lin Yu
{"title":"通过添加FeNbCe提高Cu-SSZ-13的SCR性能:揭示酸性位点富集和硫酸盐抑制的协同效应","authors":"Jinfeng Chen, Qingze Zhang, Yuanhong Zhong, Zhaoying Wang, Yakun Guo, Ming Sun, Lin Yu","doi":"10.1021/acs.iecr.5c00821","DOIUrl":null,"url":null,"abstract":"To address the limitations of molecular sieves and metal oxides in the NH<sub>3</sub>-SCR of NO<sub><i>x</i></sub>, we synthesized a novel hybrid catalyst by integrating FeNbCe metal oxides with Cu-SSZ-13. The FeNbCe comodification significantly enhanced the low-temperature performance and sulfur resistance of Cu-SSZ-13 while maintaining 100% N<sub>2</sub> selectivity across a broad activity window. The incorporation of Fe, Nb, and Ce reduced weak-acid and Lewis-acid sites while increasing strong Brønsted-acid sites, crucial for catalytic activity. The FeNbCe/Cu-SSZ-13 catalyst exhibited an enhanced surface oxygen content and redox capacity, promoting the “fast SCR” pathway and improving N<sub>2</sub> selectivity at low temperatures. The FeNbCe oxides synergistically reacted with SO<sub>2</sub>, protecting Cu<sup>2+</sup> active sites from sulfur poisoning and maintaining 100% NO<sub><i>x</i></sub> conversion for 4 h after SO<sub>2</sub> introduction, maintaining 85% within 24 h. In situ DRIFTS characterization confirmed the dominance of the Langmuir-Hinshelwood (L-H) mechanism. The FeNbCe modification represents a significant advancement in the field of NH<sub>3</sub>–SCR catalysis, offering a practical and effective solution to enhance the performance of Cu-SSZ-13 while addressing key challenges such as sulfur resistance and low-temperature activity.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"1 1","pages":""},"PeriodicalIF":3.9000,"publicationDate":"2025-05-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced SCR Performance of Cu-SSZ-13 via FeNbCe Incorporation: Unveiling the Synergistic Effect on Acidic Site Enrichment and Sulfate Inhibition\",\"authors\":\"Jinfeng Chen, Qingze Zhang, Yuanhong Zhong, Zhaoying Wang, Yakun Guo, Ming Sun, Lin Yu\",\"doi\":\"10.1021/acs.iecr.5c00821\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"To address the limitations of molecular sieves and metal oxides in the NH<sub>3</sub>-SCR of NO<sub><i>x</i></sub>, we synthesized a novel hybrid catalyst by integrating FeNbCe metal oxides with Cu-SSZ-13. The FeNbCe comodification significantly enhanced the low-temperature performance and sulfur resistance of Cu-SSZ-13 while maintaining 100% N<sub>2</sub> selectivity across a broad activity window. The incorporation of Fe, Nb, and Ce reduced weak-acid and Lewis-acid sites while increasing strong Brønsted-acid sites, crucial for catalytic activity. The FeNbCe/Cu-SSZ-13 catalyst exhibited an enhanced surface oxygen content and redox capacity, promoting the “fast SCR” pathway and improving N<sub>2</sub> selectivity at low temperatures. The FeNbCe oxides synergistically reacted with SO<sub>2</sub>, protecting Cu<sup>2+</sup> active sites from sulfur poisoning and maintaining 100% NO<sub><i>x</i></sub> conversion for 4 h after SO<sub>2</sub> introduction, maintaining 85% within 24 h. In situ DRIFTS characterization confirmed the dominance of the Langmuir-Hinshelwood (L-H) mechanism. The FeNbCe modification represents a significant advancement in the field of NH<sub>3</sub>–SCR catalysis, offering a practical and effective solution to enhance the performance of Cu-SSZ-13 while addressing key challenges such as sulfur resistance and low-temperature activity.\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"1 1\",\"pages\":\"\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-05-22\",\"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.5c00821\",\"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.5c00821","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}
Enhanced SCR Performance of Cu-SSZ-13 via FeNbCe Incorporation: Unveiling the Synergistic Effect on Acidic Site Enrichment and Sulfate Inhibition
To address the limitations of molecular sieves and metal oxides in the NH3-SCR of NOx, we synthesized a novel hybrid catalyst by integrating FeNbCe metal oxides with Cu-SSZ-13. The FeNbCe comodification significantly enhanced the low-temperature performance and sulfur resistance of Cu-SSZ-13 while maintaining 100% N2 selectivity across a broad activity window. The incorporation of Fe, Nb, and Ce reduced weak-acid and Lewis-acid sites while increasing strong Brønsted-acid sites, crucial for catalytic activity. The FeNbCe/Cu-SSZ-13 catalyst exhibited an enhanced surface oxygen content and redox capacity, promoting the “fast SCR” pathway and improving N2 selectivity at low temperatures. The FeNbCe oxides synergistically reacted with SO2, protecting Cu2+ active sites from sulfur poisoning and maintaining 100% NOx conversion for 4 h after SO2 introduction, maintaining 85% within 24 h. In situ DRIFTS characterization confirmed the dominance of the Langmuir-Hinshelwood (L-H) mechanism. The FeNbCe modification represents a significant advancement in the field of NH3–SCR catalysis, offering a practical and effective solution to enhance the performance of Cu-SSZ-13 while addressing key challenges such as sulfur resistance and low-temperature activity.
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.