{"title":"在具有孤立 VO4 位点的 V/MSN 催化剂上将甲烷选择性氧化为甲醛和一氧化碳","authors":"","doi":"10.1016/j.apcata.2024.119928","DOIUrl":null,"url":null,"abstract":"<div><p>The selective oxidation of methane to value-added C<sub>1</sub> chemicals (e.g., HCHO and CO) is a crucial process in the chemical industry. Recent studies indicate that the generation of highly dispersed isolated active sites is crucial for improving the performance in the selective oxidation of methane and studying the corresponding structure–activity relationship. Therefore, we used mesoporous silica nanoparticles (MSN) as supports and utilized grafting method to prepare catalysts with more selective oxidation active centers (isolated VO<sub>4</sub>). The study found that isolated VO<sub>4</sub> centers are the active sites for the selective oxidation of methane to formaldehyde, and CO is the product of further oxidation of formaldehyde. The total selectivity of formaldehyde and CO on all catalysts is higher than 83.6 %. Among them, the highly dispersed and isolated VO<sub>4</sub> tetrahedral active centers on the 2 V/MSN catalyst could stably convert methane to formaldehyde, achieving the highest formaldehyde yield of 3.7 % at 670 °C.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7000,"publicationDate":"2024-08-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Selective oxidation of methane to formaldehyde and carbon monoxide over V/MSN catalysts with isolated VO4 sites\",\"authors\":\"\",\"doi\":\"10.1016/j.apcata.2024.119928\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>The selective oxidation of methane to value-added C<sub>1</sub> chemicals (e.g., HCHO and CO) is a crucial process in the chemical industry. Recent studies indicate that the generation of highly dispersed isolated active sites is crucial for improving the performance in the selective oxidation of methane and studying the corresponding structure–activity relationship. Therefore, we used mesoporous silica nanoparticles (MSN) as supports and utilized grafting method to prepare catalysts with more selective oxidation active centers (isolated VO<sub>4</sub>). The study found that isolated VO<sub>4</sub> centers are the active sites for the selective oxidation of methane to formaldehyde, and CO is the product of further oxidation of formaldehyde. The total selectivity of formaldehyde and CO on all catalysts is higher than 83.6 %. Among them, the highly dispersed and isolated VO<sub>4</sub> tetrahedral active centers on the 2 V/MSN catalyst could stably convert methane to formaldehyde, achieving the highest formaldehyde yield of 3.7 % at 670 °C.</p></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-08-30\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X24003739\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Catalysis A: General","FirstCategoryId":"1","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0926860X24003739","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
将甲烷选择性氧化为高附加值的 C1 化学物质(如 HCHO 和 CO)是化学工业中的一个重要过程。最近的研究表明,生成高度分散的孤立活性位点对于提高甲烷选择性氧化的性能和研究相应的结构-活性关系至关重要。因此,我们以介孔二氧化硅纳米颗粒(MSN)为载体,利用接枝法制备了具有更多选择性氧化活性中心(孤立 VO4)的催化剂。研究发现,孤立的 VO4 中心是甲烷选择性氧化为甲醛的活性位点,而 CO 是甲醛进一步氧化的产物。所有催化剂对甲醛和 CO 的总选择性均高于 83.6%。其中,2 V/MSN 催化剂上高度分散和隔离的 VO4 四面体活性中心可将甲烷稳定地转化为甲醛,在 670 °C 时甲醛产率最高,达到 3.7%。
Selective oxidation of methane to formaldehyde and carbon monoxide over V/MSN catalysts with isolated VO4 sites
The selective oxidation of methane to value-added C1 chemicals (e.g., HCHO and CO) is a crucial process in the chemical industry. Recent studies indicate that the generation of highly dispersed isolated active sites is crucial for improving the performance in the selective oxidation of methane and studying the corresponding structure–activity relationship. Therefore, we used mesoporous silica nanoparticles (MSN) as supports and utilized grafting method to prepare catalysts with more selective oxidation active centers (isolated VO4). The study found that isolated VO4 centers are the active sites for the selective oxidation of methane to formaldehyde, and CO is the product of further oxidation of formaldehyde. The total selectivity of formaldehyde and CO on all catalysts is higher than 83.6 %. Among them, the highly dispersed and isolated VO4 tetrahedral active centers on the 2 V/MSN catalyst could stably convert methane to formaldehyde, achieving the highest formaldehyde yield of 3.7 % at 670 °C.
期刊介绍:
Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications.
Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.