{"title":"Ti3SiC2 支持物上 CuOx 和 VOx 直接氧化甲烷的催化行为","authors":"","doi":"10.1016/j.cattod.2024.114959","DOIUrl":null,"url":null,"abstract":"<div><p>Herein we show that the Ti<sub>3</sub>SiC<sub>2</sub> MAX phase can be used as a support for deposition of different amounts of metal oxides (MO<sub>x</sub>, M = Cu or V) (5, 10 and 20 wt%) for the direct oxidation of methane to formaldehyde using molecular oxygen, at relatively low temperatures and atmospheric pressure. The oxides were deposited using a hydrothermal method at 180 °C without affecting the bulk MAX phase structure. However, during the hydrothermal treatment (HT) a thin oxide layer - found to play an important role in the reaction's selectivity– was evidenced by X-ray photoelectron spectroscopy. We thus conclude that the MO<sub>x</sub> species are responsible for the CH<sub>4</sub> activation, while the Ti<sub>3</sub>SiC<sub>2</sub> surface is responsible for the high selectivity to formaldehyde indicating that, Ti<sub>3</sub>SiC<sub>2</sub> has great potential for designing innovative catalysts for direct oxidation of methane using molecular oxygen and at atmospheric pressure.</p></div>","PeriodicalId":264,"journal":{"name":"Catalysis Today","volume":null,"pages":null},"PeriodicalIF":5.2000,"publicationDate":"2024-08-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S092058612400453X/pdfft?md5=ce68fd5d31c0d97f8c41faba5a28cc2b&pid=1-s2.0-S092058612400453X-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Catalytic behaviour of CuOx and VOx on Ti3SiC2 support for direct oxidation of methane\",\"authors\":\"\",\"doi\":\"10.1016/j.cattod.2024.114959\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Herein we show that the Ti<sub>3</sub>SiC<sub>2</sub> MAX phase can be used as a support for deposition of different amounts of metal oxides (MO<sub>x</sub>, M = Cu or V) (5, 10 and 20 wt%) for the direct oxidation of methane to formaldehyde using molecular oxygen, at relatively low temperatures and atmospheric pressure. The oxides were deposited using a hydrothermal method at 180 °C without affecting the bulk MAX phase structure. However, during the hydrothermal treatment (HT) a thin oxide layer - found to play an important role in the reaction's selectivity– was evidenced by X-ray photoelectron spectroscopy. We thus conclude that the MO<sub>x</sub> species are responsible for the CH<sub>4</sub> activation, while the Ti<sub>3</sub>SiC<sub>2</sub> surface is responsible for the high selectivity to formaldehyde indicating that, Ti<sub>3</sub>SiC<sub>2</sub> has great potential for designing innovative catalysts for direct oxidation of methane using molecular oxygen and at atmospheric pressure.</p></div>\",\"PeriodicalId\":264,\"journal\":{\"name\":\"Catalysis Today\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.2000,\"publicationDate\":\"2024-08-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S092058612400453X/pdfft?md5=ce68fd5d31c0d97f8c41faba5a28cc2b&pid=1-s2.0-S092058612400453X-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Today\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S092058612400453X\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, APPLIED\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Today","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S092058612400453X","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, APPLIED","Score":null,"Total":0}
引用次数: 0
摘要
在此,我们展示了 Ti3SiC2 MAX 相可用作沉积不同数量金属氧化物(MOx,M = Cu 或 V)(5、10 和 20 wt%)的支撑物,以便在相对较低的温度和大气压力下利用分子氧将甲烷直接氧化为甲醛。这些氧化物是在 180 °C 的水热法条件下沉积的,不会影响块状 MAX 相结构。然而,在水热处理(HT)过程中,X 射线光电子能谱显示出了一层薄薄的氧化物层,这层氧化物层对反应的选择性起着重要作用。因此,我们得出结论:MOx 物种对 CH4 活化起作用,而 Ti3SiC2 表面对甲醛的高选择性起作用,这表明 Ti3SiC2 具有设计创新催化剂的巨大潜力,可用于在常压下使用分子氧直接氧化甲烷。
Catalytic behaviour of CuOx and VOx on Ti3SiC2 support for direct oxidation of methane
Herein we show that the Ti3SiC2 MAX phase can be used as a support for deposition of different amounts of metal oxides (MOx, M = Cu or V) (5, 10 and 20 wt%) for the direct oxidation of methane to formaldehyde using molecular oxygen, at relatively low temperatures and atmospheric pressure. The oxides were deposited using a hydrothermal method at 180 °C without affecting the bulk MAX phase structure. However, during the hydrothermal treatment (HT) a thin oxide layer - found to play an important role in the reaction's selectivity– was evidenced by X-ray photoelectron spectroscopy. We thus conclude that the MOx species are responsible for the CH4 activation, while the Ti3SiC2 surface is responsible for the high selectivity to formaldehyde indicating that, Ti3SiC2 has great potential for designing innovative catalysts for direct oxidation of methane using molecular oxygen and at atmospheric pressure.
期刊介绍:
Catalysis Today focuses on the rapid publication of original invited papers devoted to currently important topics in catalysis and related subjects. The journal only publishes special issues (Proposing a Catalysis Today Special Issue), each of which is supervised by Guest Editors who recruit individual papers and oversee the peer review process. Catalysis Today offers researchers in the field of catalysis in-depth overviews of topical issues.
Both fundamental and applied aspects of catalysis are covered. Subjects such as catalysis of immobilized organometallic and biocatalytic systems are welcome. Subjects related to catalysis such as experimental techniques, adsorption, process technology, synthesis, in situ characterization, computational, theoretical modeling, imaging and others are included if there is a clear relationship to catalysis.