Kexin Xu, Li Wang, Xinghua Zhang, Xuehai Wang, Yimin Zhu
{"title":"fau型和lta型沸石上歧化和配位对NO的高效吸附","authors":"Kexin Xu, Li Wang, Xinghua Zhang, Xuehai Wang, Yimin Zhu","doi":"10.1016/j.cej.2025.160305","DOIUrl":null,"url":null,"abstract":"High efficient NO adsorption on zeolites not only accelerates catalytic NO to N<sub>2</sub> by concentrating, but also figures out the difficulty of removing NO with low temperature and low concentration. This study evaluates the dynamic NO adsorption–desorption behaviors on 12 commercial zeolites, demonstrating 13X and 5A zeolites as excellent adsorbents with high NO adsorption capacity and low regeneration temperature. Based on extensive characterizations including N<sub>2</sub>-physisorption, NH<sub>3</sub>-TPD, CO<sub>2</sub>-TPD, <em>on-line</em> MS and <em>in-situ</em> DRIFTS, the pore structure-performance relationship, acidity-performance relationship and basicity-performance relationship have been thoroughly investigated and discussed upon NO adsorption–desorption behaviors, together with the gaseous and surface species. NO directly coordinates to the strong Lewis acid sites and strong base sites (i.e., strong Lewis acid-base pairs), leading to coordinately bonded NO<sup>δ+</sup> and NO<sup>δ-</sup> species, respectively. Besides, NO also directly disproportionates to N<sub>2</sub>O and NO<sub>2</sub>, followed by in-situ conversion of NO<sub>2</sub> into nitrate species. Thus, the coordination and disproportionation mechanisms have been identified for high-efficient NO adsorption on 13X and 5A zeolites, which supplements the current understandings of NO adsorption on zeolites and provides a new strategy to strengthen NO adsorption on zeolites with strong Lewis acid-base pairs.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"11 1","pages":""},"PeriodicalIF":13.2000,"publicationDate":"2025-02-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Disproportionation and coordination driven high-efficient NO adsorption on FAU-and LTA-type zeolites\",\"authors\":\"Kexin Xu, Li Wang, Xinghua Zhang, Xuehai Wang, Yimin Zhu\",\"doi\":\"10.1016/j.cej.2025.160305\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"High efficient NO adsorption on zeolites not only accelerates catalytic NO to N<sub>2</sub> by concentrating, but also figures out the difficulty of removing NO with low temperature and low concentration. This study evaluates the dynamic NO adsorption–desorption behaviors on 12 commercial zeolites, demonstrating 13X and 5A zeolites as excellent adsorbents with high NO adsorption capacity and low regeneration temperature. Based on extensive characterizations including N<sub>2</sub>-physisorption, NH<sub>3</sub>-TPD, CO<sub>2</sub>-TPD, <em>on-line</em> MS and <em>in-situ</em> DRIFTS, the pore structure-performance relationship, acidity-performance relationship and basicity-performance relationship have been thoroughly investigated and discussed upon NO adsorption–desorption behaviors, together with the gaseous and surface species. NO directly coordinates to the strong Lewis acid sites and strong base sites (i.e., strong Lewis acid-base pairs), leading to coordinately bonded NO<sup>δ+</sup> and NO<sup>δ-</sup> species, respectively. Besides, NO also directly disproportionates to N<sub>2</sub>O and NO<sub>2</sub>, followed by in-situ conversion of NO<sub>2</sub> into nitrate species. Thus, the coordination and disproportionation mechanisms have been identified for high-efficient NO adsorption on 13X and 5A zeolites, which supplements the current understandings of NO adsorption on zeolites and provides a new strategy to strengthen NO adsorption on zeolites with strong Lewis acid-base pairs.\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"11 1\",\"pages\":\"\"},\"PeriodicalIF\":13.2000,\"publicationDate\":\"2025-02-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.cej.2025.160305\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2025.160305","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Disproportionation and coordination driven high-efficient NO adsorption on FAU-and LTA-type zeolites
High efficient NO adsorption on zeolites not only accelerates catalytic NO to N2 by concentrating, but also figures out the difficulty of removing NO with low temperature and low concentration. This study evaluates the dynamic NO adsorption–desorption behaviors on 12 commercial zeolites, demonstrating 13X and 5A zeolites as excellent adsorbents with high NO adsorption capacity and low regeneration temperature. Based on extensive characterizations including N2-physisorption, NH3-TPD, CO2-TPD, on-line MS and in-situ DRIFTS, the pore structure-performance relationship, acidity-performance relationship and basicity-performance relationship have been thoroughly investigated and discussed upon NO adsorption–desorption behaviors, together with the gaseous and surface species. NO directly coordinates to the strong Lewis acid sites and strong base sites (i.e., strong Lewis acid-base pairs), leading to coordinately bonded NOδ+ and NOδ- species, respectively. Besides, NO also directly disproportionates to N2O and NO2, followed by in-situ conversion of NO2 into nitrate species. Thus, the coordination and disproportionation mechanisms have been identified for high-efficient NO adsorption on 13X and 5A zeolites, which supplements the current understandings of NO adsorption on zeolites and provides a new strategy to strengthen NO adsorption on zeolites with strong Lewis acid-base pairs.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.