{"title":"在氧化铝支撑的第 5 族过渡金属碳化物催化剂上将 CO2 选择性还原为 CO","authors":"","doi":"10.1016/j.apcata.2024.119963","DOIUrl":null,"url":null,"abstract":"<div><p>We show the applicability of a preparation method, previously reported for obtaining tailored bulk VC<sub>x</sub> catalysts, for alumina-supported G5TMCs. The characteristics of the G5TMCs/Al<sub>2</sub>O<sub>3</sub> catalysts and their behaviour in the selective reduction of CO<sub>2</sub> to CO through the RWGS reaction is reported. VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts were active, stable and highly selective; meanwhile NbC/Al<sub>2</sub>O<sub>3</sub> and TaC/Al<sub>2</sub>O<sub>3</sub> were not active. VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts exhibited selectivity to CO over 99.5 % at temperature above 773 K. The characteristics of alumina-supported vanadium carbide particles depended on the vanadium precursor and on the atmosphere used during the catalyst preparation. XPS characterization of VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts revealed the presence of carbide species on surface before and after RWGS reaction. The catalytic behaviour of VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> is analysed in the light of their characteristics and compared with bulk VC<sub>x</sub> counterparts. The most performant catalyst, VC(Pr)/Al<sub>2</sub>O<sub>3</sub><sub>,</sub> was stable over 4 days at 723 K, with ∼100 % selectivity to CO and CO<sub>2</sub> conversion of ∼11 %.</p></div>","PeriodicalId":243,"journal":{"name":"Applied Catalysis A: General","volume":null,"pages":null},"PeriodicalIF":4.7000,"publicationDate":"2024-09-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S0926860X24004083/pdfft?md5=293c77c63c14770c68e3f040e986dd12&pid=1-s2.0-S0926860X24004083-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Selective reduction of CO2 to CO over alumina-supported catalysts of group 5 transition metal carbides\",\"authors\":\"\",\"doi\":\"10.1016/j.apcata.2024.119963\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>We show the applicability of a preparation method, previously reported for obtaining tailored bulk VC<sub>x</sub> catalysts, for alumina-supported G5TMCs. The characteristics of the G5TMCs/Al<sub>2</sub>O<sub>3</sub> catalysts and their behaviour in the selective reduction of CO<sub>2</sub> to CO through the RWGS reaction is reported. VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts were active, stable and highly selective; meanwhile NbC/Al<sub>2</sub>O<sub>3</sub> and TaC/Al<sub>2</sub>O<sub>3</sub> were not active. VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts exhibited selectivity to CO over 99.5 % at temperature above 773 K. The characteristics of alumina-supported vanadium carbide particles depended on the vanadium precursor and on the atmosphere used during the catalyst preparation. XPS characterization of VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> catalysts revealed the presence of carbide species on surface before and after RWGS reaction. The catalytic behaviour of VC<sub>x</sub>/Al<sub>2</sub>O<sub>3</sub> is analysed in the light of their characteristics and compared with bulk VC<sub>x</sub> counterparts. The most performant catalyst, VC(Pr)/Al<sub>2</sub>O<sub>3</sub><sub>,</sub> was stable over 4 days at 723 K, with ∼100 % selectivity to CO and CO<sub>2</sub> conversion of ∼11 %.</p></div>\",\"PeriodicalId\":243,\"journal\":{\"name\":\"Applied Catalysis A: General\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.7000,\"publicationDate\":\"2024-09-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S0926860X24004083/pdfft?md5=293c77c63c14770c68e3f040e986dd12&pid=1-s2.0-S0926860X24004083-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Catalysis A: General\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0926860X24004083\",\"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/S0926860X24004083","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
我们展示了氧化铝支撑的 G5TMCs 的制备方法的适用性,这种方法以前曾报道过用于获得定制的块状 VCx 催化剂。报告了 G5TMCs/Al2O3 催化剂的特性及其在通过 RWGS 反应将 CO2 选择性还原为 CO 的过程中的表现。VCx/Al2O3 催化剂具有活性、稳定性和高选择性;而 NbC/Al2O3 和 TaC/Al2O3 则没有活性。在温度高于 773 K 时,VCx/Al2O3 催化剂对 CO 的选择性超过 99.5%。氧化铝支撑的碳化钒颗粒的特性取决于钒前驱体和催化剂制备过程中使用的气氛。VCx/Al2O3 催化剂的 XPS 表征显示,在 RWGS 反应前后,表面都存在碳化物。根据 VCx/Al2O3 的特性对其催化性能进行了分析,并将其与块状 VCx 催化剂进行了比较。性能最好的催化剂 VC(Pr)/Al2O3 在 723 K 下稳定运行 4 天,对 CO 的选择性为 100%,CO2 转化率为 11%。
Selective reduction of CO2 to CO over alumina-supported catalysts of group 5 transition metal carbides
We show the applicability of a preparation method, previously reported for obtaining tailored bulk VCx catalysts, for alumina-supported G5TMCs. The characteristics of the G5TMCs/Al2O3 catalysts and their behaviour in the selective reduction of CO2 to CO through the RWGS reaction is reported. VCx/Al2O3 catalysts were active, stable and highly selective; meanwhile NbC/Al2O3 and TaC/Al2O3 were not active. VCx/Al2O3 catalysts exhibited selectivity to CO over 99.5 % at temperature above 773 K. The characteristics of alumina-supported vanadium carbide particles depended on the vanadium precursor and on the atmosphere used during the catalyst preparation. XPS characterization of VCx/Al2O3 catalysts revealed the presence of carbide species on surface before and after RWGS reaction. The catalytic behaviour of VCx/Al2O3 is analysed in the light of their characteristics and compared with bulk VCx counterparts. The most performant catalyst, VC(Pr)/Al2O3, was stable over 4 days at 723 K, with ∼100 % selectivity to CO and CO2 conversion of ∼11 %.
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.