Argam Akopyan*, Artur Aghoyan, Ekaterina A. Eseva, Maxim O. Lukashov, Mikhail M. Belov and Davit Davtyan,
{"title":"用于加速燃料好氧氧化脱硫的增效混合碳化物催化剂","authors":"Argam Akopyan*, Artur Aghoyan, Ekaterina A. Eseva, Maxim O. Lukashov, Mikhail M. Belov and Davit Davtyan, ","doi":"10.1021/acs.energyfuels.4c0638010.1021/acs.energyfuels.4c06380","DOIUrl":null,"url":null,"abstract":"<p >Aerobic oxidative desulfurization (AODS) is a promising technique for clean fuels production. Herein we present synergistic mixed carbide catalysts (FeMoWC) synthesized rapidly by microwave irradiation for AODS process. The combination of a ternary mixture of carbides for AODS leads to a significant increase in catalytic activity compared to single-phase, dicarbides or simply oxides of transition metals. The synthesized materials were characterized in detail by a complex of methods: XRD, HRTEM, EDX, SEM, XPS, low-temperature nitrogen adsorption/desorption, H<sub>2</sub>-temperature-programmed reduction (TPR), Raman spectroscopy. Under selected conditions (150 °C, 6 atm, 0.5 wt % catalyst dosage) complete oxidation of dibenzothiophene (DBT) was achieved in just 20 min. Under optimal conditions, the specific catalytic activity was 12.73 and 293.43 mmol g<sup>–1</sup> h<sup>–1</sup> for the model and real fuel, respectively. A possible mechanism for the reaction is discussed, including the activation of atmospheric oxygen with the formation of a superoxide radical, the formation of alkyl peroxides and peroxo complexes. The proposed approaches open up wide possibilities for the future development of highly efficient AODS catalysts for practical application and production of clean motor fuels.</p>","PeriodicalId":35,"journal":{"name":"Energy & Fuels","volume":"39 13","pages":"6487–6504 6487–6504"},"PeriodicalIF":5.2000,"publicationDate":"2025-03-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Synergistic Mixed Carbide Catalysts for Accelerated Aerobic Oxidative Desulfurization of Fuels\",\"authors\":\"Argam Akopyan*, Artur Aghoyan, Ekaterina A. Eseva, Maxim O. Lukashov, Mikhail M. Belov and Davit Davtyan, \",\"doi\":\"10.1021/acs.energyfuels.4c0638010.1021/acs.energyfuels.4c06380\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Aerobic oxidative desulfurization (AODS) is a promising technique for clean fuels production. Herein we present synergistic mixed carbide catalysts (FeMoWC) synthesized rapidly by microwave irradiation for AODS process. The combination of a ternary mixture of carbides for AODS leads to a significant increase in catalytic activity compared to single-phase, dicarbides or simply oxides of transition metals. The synthesized materials were characterized in detail by a complex of methods: XRD, HRTEM, EDX, SEM, XPS, low-temperature nitrogen adsorption/desorption, H<sub>2</sub>-temperature-programmed reduction (TPR), Raman spectroscopy. Under selected conditions (150 °C, 6 atm, 0.5 wt % catalyst dosage) complete oxidation of dibenzothiophene (DBT) was achieved in just 20 min. Under optimal conditions, the specific catalytic activity was 12.73 and 293.43 mmol g<sup>–1</sup> h<sup>–1</sup> for the model and real fuel, respectively. A possible mechanism for the reaction is discussed, including the activation of atmospheric oxygen with the formation of a superoxide radical, the formation of alkyl peroxides and peroxo complexes. The proposed approaches open up wide possibilities for the future development of highly efficient AODS catalysts for practical application and production of clean motor fuels.</p>\",\"PeriodicalId\":35,\"journal\":{\"name\":\"Energy & Fuels\",\"volume\":\"39 13\",\"pages\":\"6487–6504 6487–6504\"},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2025-03-25\",\"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.4c06380\",\"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.4c06380","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}
Synergistic Mixed Carbide Catalysts for Accelerated Aerobic Oxidative Desulfurization of Fuels
Aerobic oxidative desulfurization (AODS) is a promising technique for clean fuels production. Herein we present synergistic mixed carbide catalysts (FeMoWC) synthesized rapidly by microwave irradiation for AODS process. The combination of a ternary mixture of carbides for AODS leads to a significant increase in catalytic activity compared to single-phase, dicarbides or simply oxides of transition metals. The synthesized materials were characterized in detail by a complex of methods: XRD, HRTEM, EDX, SEM, XPS, low-temperature nitrogen adsorption/desorption, H2-temperature-programmed reduction (TPR), Raman spectroscopy. Under selected conditions (150 °C, 6 atm, 0.5 wt % catalyst dosage) complete oxidation of dibenzothiophene (DBT) was achieved in just 20 min. Under optimal conditions, the specific catalytic activity was 12.73 and 293.43 mmol g–1 h–1 for the model and real fuel, respectively. A possible mechanism for the reaction is discussed, including the activation of atmospheric oxygen with the formation of a superoxide radical, the formation of alkyl peroxides and peroxo complexes. The proposed approaches open up wide possibilities for the future development of highly efficient AODS catalysts for practical application and production of clean motor fuels.
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.