Jie Fan , Lutao Mao , Mingli Fu , Peng Liu , Zuliang Wu , Daiqi Ye
{"title":"通过原位 DRIFTS 探索具有稳定低温催化性能的新型八面体 Pt/Mn3O4 催化剂的甲苯氧化速率控制步骤","authors":"Jie Fan , Lutao Mao , Mingli Fu , Peng Liu , Zuliang Wu , Daiqi Ye","doi":"10.1016/j.micromeso.2024.113164","DOIUrl":null,"url":null,"abstract":"<div><p>The high efficiency and stability of catalysts are crucial for their practical application in toluene oxidation. Herein, a novel octahedral Pt/Mn<sub>3</sub>O<sub>4</sub>-110 catalyst with excellent structural stability was synthesized and 100 % toluene conversion can be achieved at low-temperature 160 °C. XRD and Raman results indicated that the structure of Pt/Mn<sub>3</sub>O<sub>4</sub>-110 can be well maintained after 120 h on-stream reaction, the resistance to H<sub>2</sub>O (3 or 5 vol%) and high concentration toluene (3000 ppm)/CO<sub>2</sub> (5 vol%) tests. In situ DRIFTS comparative studies between Pt/Mn<sub>3</sub>O<sub>4</sub>-110 and Pt/Mn<sub>3</sub>O<sub>4</sub>-100 (30 % toluene conversion at 160 °C) samples demonstrated that the rate-control steps of toluene oxidation on Pt/Mn<sub>3</sub>O<sub>4</sub>-110 and Pt/Mn<sub>3</sub>O<sub>4</sub>-100 were both the further oxidation of benzoate species in the presence of gas-phase oxygen, while the transformation of benzaldehyde to benzoate species was the rate-control step on Pt/Mn<sub>3</sub>O<sub>4</sub>-100 in the absence of gas-phase oxygen. The weaker Mn-O bonds, richer oxygen vacancies and higher mobility of oxygen species on Pt/Mn<sub>3</sub>O<sub>4</sub>-110 sample than that of Pt/Mn<sub>3</sub>O<sub>4</sub>-100 are beneficial for the easier release of lattice oxygen from the surface of catalyst and then participated in toluene oxidation via Mars-van Krevelen mechanism, contributing to easier oxidation of benzaldehyde to benzoate species and formation of formic acid and bicarbonate species.</p></div>","PeriodicalId":392,"journal":{"name":"Microporous and Mesoporous Materials","volume":null,"pages":null},"PeriodicalIF":4.8000,"publicationDate":"2024-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Exploring the rate-control step of toluene oxidation over the novel octahedral Pt/Mn3O4 catalyst with stable low-temperature catalytic performance via in situ DRIFTS\",\"authors\":\"Jie Fan , Lutao Mao , Mingli Fu , Peng Liu , Zuliang Wu , Daiqi Ye\",\"doi\":\"10.1016/j.micromeso.2024.113164\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The high efficiency and stability of catalysts are crucial for their practical application in toluene oxidation. Herein, a novel octahedral Pt/Mn<sub>3</sub>O<sub>4</sub>-110 catalyst with excellent structural stability was synthesized and 100 % toluene conversion can be achieved at low-temperature 160 °C. XRD and Raman results indicated that the structure of Pt/Mn<sub>3</sub>O<sub>4</sub>-110 can be well maintained after 120 h on-stream reaction, the resistance to H<sub>2</sub>O (3 or 5 vol%) and high concentration toluene (3000 ppm)/CO<sub>2</sub> (5 vol%) tests. In situ DRIFTS comparative studies between Pt/Mn<sub>3</sub>O<sub>4</sub>-110 and Pt/Mn<sub>3</sub>O<sub>4</sub>-100 (30 % toluene conversion at 160 °C) samples demonstrated that the rate-control steps of toluene oxidation on Pt/Mn<sub>3</sub>O<sub>4</sub>-110 and Pt/Mn<sub>3</sub>O<sub>4</sub>-100 were both the further oxidation of benzoate species in the presence of gas-phase oxygen, while the transformation of benzaldehyde to benzoate species was the rate-control step on Pt/Mn<sub>3</sub>O<sub>4</sub>-100 in the absence of gas-phase oxygen. The weaker Mn-O bonds, richer oxygen vacancies and higher mobility of oxygen species on Pt/Mn<sub>3</sub>O<sub>4</sub>-110 sample than that of Pt/Mn<sub>3</sub>O<sub>4</sub>-100 are beneficial for the easier release of lattice oxygen from the surface of catalyst and then participated in toluene oxidation via Mars-van Krevelen mechanism, contributing to easier oxidation of benzaldehyde to benzoate species and formation of formic acid and bicarbonate species.</p></div>\",\"PeriodicalId\":392,\"journal\":{\"name\":\"Microporous and Mesoporous Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2024-05-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Microporous and Mesoporous Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1387181124001860\",\"RegionNum\":3,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Microporous and Mesoporous Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1387181124001860","RegionNum":3,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
Exploring the rate-control step of toluene oxidation over the novel octahedral Pt/Mn3O4 catalyst with stable low-temperature catalytic performance via in situ DRIFTS
The high efficiency and stability of catalysts are crucial for their practical application in toluene oxidation. Herein, a novel octahedral Pt/Mn3O4-110 catalyst with excellent structural stability was synthesized and 100 % toluene conversion can be achieved at low-temperature 160 °C. XRD and Raman results indicated that the structure of Pt/Mn3O4-110 can be well maintained after 120 h on-stream reaction, the resistance to H2O (3 or 5 vol%) and high concentration toluene (3000 ppm)/CO2 (5 vol%) tests. In situ DRIFTS comparative studies between Pt/Mn3O4-110 and Pt/Mn3O4-100 (30 % toluene conversion at 160 °C) samples demonstrated that the rate-control steps of toluene oxidation on Pt/Mn3O4-110 and Pt/Mn3O4-100 were both the further oxidation of benzoate species in the presence of gas-phase oxygen, while the transformation of benzaldehyde to benzoate species was the rate-control step on Pt/Mn3O4-100 in the absence of gas-phase oxygen. The weaker Mn-O bonds, richer oxygen vacancies and higher mobility of oxygen species on Pt/Mn3O4-110 sample than that of Pt/Mn3O4-100 are beneficial for the easier release of lattice oxygen from the surface of catalyst and then participated in toluene oxidation via Mars-van Krevelen mechanism, contributing to easier oxidation of benzaldehyde to benzoate species and formation of formic acid and bicarbonate species.
期刊介绍：
Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal.
Topics which are particularly of interest include:
All aspects of natural microporous and mesoporous solids
The synthesis of crystalline or amorphous porous materials
The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic
The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions
All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials
Adsorption (and other separation techniques) using microporous or mesoporous adsorbents
Catalysis by microporous and mesoporous materials
Host/guest interactions
Theoretical chemistry and modelling of host/guest interactions
All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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