Xueyu Du , Caiting Li , Jie Zhang , Kuang Yang , Xuan Liu , Le Huang , Ziang Zhang , Pengfei Wang
{"title":"Mn-Co氧化物与活性炭载体协同作用促进甲苯在MnCo/AC上的催化氧化","authors":"Xueyu Du , Caiting Li , Jie Zhang , Kuang Yang , Xuan Liu , Le Huang , Ziang Zhang , Pengfei Wang","doi":"10.1016/j.fuel.2025.136002","DOIUrl":null,"url":null,"abstract":"<div><div>Activated coke (AC), with well-developed porous structure, has been extensively applied as adsorbents and support of catalysts for air pollutants control. In this work, Mn-Co oxides supported on AC were synthesized for toluene removal. The optimal Mn<sub>1</sub>Co<sub>9</sub>/AC exhibited remarkable toluene removal efficiency above 90 % at 238 ℃, comparable to some pure metal-oxides catalysts but with a lower cost. Besides, Mn<sub>1</sub>Co<sub>9</sub>/AC sustained toluene removal efficiency above 80 % even with 500 ppm SO<sub>2</sub> or 10 vol% H<sub>2</sub>O at 240 ℃, implying its potential of industrial application. Characterizations revealed that the strong metal oxides-support interaction endowed Mn<sub>1</sub>Co<sub>9</sub>/AC with enhanced adsorption of reactants, highly-dispersed active components and accelerated electron transport. Additionally, the synergy between MnO<sub>x</sub> and CoO<sub>x</sub> facilitated the formation of active oxygen species, including abundant surface adsorbed oxygen, oxygen vacancies and lattice oxygen with high mobility, metal ions with higher valence, and thus superior reducibility. Combined with FTIR, the initial oxidation of toluene → benzyl alcohol → benzaldehyde → benzoic acid proceeded at lower temperature, while the further oxidation of benzoic acid → maleic anhydride → carbonates → CO<sub>2</sub> + H<sub>2</sub>O occurred with elevated temperature. And O<sub>2</sub> facilitated both toluene adsorption and subsequent oxidation of intermediates, especially for benzyl alcohol oxidation, via continuous replenishment of consumed active oxygen species.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"402 ","pages":"Article 136002"},"PeriodicalIF":7.5000,"publicationDate":"2025-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Boosting catalytic oxidation of toluene on MnCo/AC by synergistic effect of Mn-Co oxides and AC support\",\"authors\":\"Xueyu Du , Caiting Li , Jie Zhang , Kuang Yang , Xuan Liu , Le Huang , Ziang Zhang , Pengfei Wang\",\"doi\":\"10.1016/j.fuel.2025.136002\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Activated coke (AC), with well-developed porous structure, has been extensively applied as adsorbents and support of catalysts for air pollutants control. In this work, Mn-Co oxides supported on AC were synthesized for toluene removal. The optimal Mn<sub>1</sub>Co<sub>9</sub>/AC exhibited remarkable toluene removal efficiency above 90 % at 238 ℃, comparable to some pure metal-oxides catalysts but with a lower cost. Besides, Mn<sub>1</sub>Co<sub>9</sub>/AC sustained toluene removal efficiency above 80 % even with 500 ppm SO<sub>2</sub> or 10 vol% H<sub>2</sub>O at 240 ℃, implying its potential of industrial application. Characterizations revealed that the strong metal oxides-support interaction endowed Mn<sub>1</sub>Co<sub>9</sub>/AC with enhanced adsorption of reactants, highly-dispersed active components and accelerated electron transport. Additionally, the synergy between MnO<sub>x</sub> and CoO<sub>x</sub> facilitated the formation of active oxygen species, including abundant surface adsorbed oxygen, oxygen vacancies and lattice oxygen with high mobility, metal ions with higher valence, and thus superior reducibility. Combined with FTIR, the initial oxidation of toluene → benzyl alcohol → benzaldehyde → benzoic acid proceeded at lower temperature, while the further oxidation of benzoic acid → maleic anhydride → carbonates → CO<sub>2</sub> + H<sub>2</sub>O occurred with elevated temperature. And O<sub>2</sub> facilitated both toluene adsorption and subsequent oxidation of intermediates, especially for benzyl alcohol oxidation, via continuous replenishment of consumed active oxygen species.</div></div>\",\"PeriodicalId\":325,\"journal\":{\"name\":\"Fuel\",\"volume\":\"402 \",\"pages\":\"Article 136002\"},\"PeriodicalIF\":7.5000,\"publicationDate\":\"2025-06-21\",\"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/S0016236125017272\",\"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/S0016236125017272","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}
Boosting catalytic oxidation of toluene on MnCo/AC by synergistic effect of Mn-Co oxides and AC support
Activated coke (AC), with well-developed porous structure, has been extensively applied as adsorbents and support of catalysts for air pollutants control. In this work, Mn-Co oxides supported on AC were synthesized for toluene removal. The optimal Mn1Co9/AC exhibited remarkable toluene removal efficiency above 90 % at 238 ℃, comparable to some pure metal-oxides catalysts but with a lower cost. Besides, Mn1Co9/AC sustained toluene removal efficiency above 80 % even with 500 ppm SO2 or 10 vol% H2O at 240 ℃, implying its potential of industrial application. Characterizations revealed that the strong metal oxides-support interaction endowed Mn1Co9/AC with enhanced adsorption of reactants, highly-dispersed active components and accelerated electron transport. Additionally, the synergy between MnOx and CoOx facilitated the formation of active oxygen species, including abundant surface adsorbed oxygen, oxygen vacancies and lattice oxygen with high mobility, metal ions with higher valence, and thus superior reducibility. Combined with FTIR, the initial oxidation of toluene → benzyl alcohol → benzaldehyde → benzoic acid proceeded at lower temperature, while the further oxidation of benzoic acid → maleic anhydride → carbonates → CO2 + H2O occurred with elevated temperature. And O2 facilitated both toluene adsorption and subsequent oxidation of intermediates, especially for benzyl alcohol oxidation, via continuous replenishment of consumed active oxygen species.
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.