{"title":"串联 Pt/TiO2 和 Fe3C 催化剂用于在高空间速度下将 CO2 直接转化为轻烃","authors":"","doi":"10.1016/j.jcis.2024.09.053","DOIUrl":null,"url":null,"abstract":"<div><p>CO<sub>2</sub> hydrogenation to hydrocarbons under high space velocity is crucial for industrial applications, but traditional Fe-based catalysts often suffer from the low activity and poor stability. Herein, we report a new tandem catalyst system combining Pt/TiO<sub>2</sub> catalysts with Fe<sub>3</sub>C catalysts for the direct conversion of CO<sub>2</sub> into <em>C</em><sub>2</sub>-C<sub>4</sub> hydrocarbons under high space velocity. The Pt/TiO<sub>2</sub> component promotes *CO intermediate production with an enhanced Reverse Water-Gas Shift (RWGS) reaction efficiency, providing a highly reactive species for the Fe<sub>3</sub>C catalyst to achieve Fischer-Tropsch synthesis (FTS). By maximizing the contact interface between the Pt/TiO<sub>2</sub> and Fe-based components through a granule mixing configuration, we achieve significant enhancements in both CO<sub>2</sub> conversion rate (24.0 %) and <em>C</em><sub>2</sub>-C<sub>4</sub> hydrocarbons selectivity (51.1 %) under the gaseous hourly space velocity (GHSV) of 100000 mL g<sub>cat</sub><sup>−1</sup>h<sup>−1</sup>. Besides, excellent stability is achieved by the tandem catalysts with continuous catalysis for up to 80 h without significant decrease in activity. Through modulation of the reduction states of iron oxide, we effectively tune the composition of Fe-based catalyst, thereby tailoring the product distribution. Through this work, we not only offer a promising avenue for reducing CO<sub>2</sub> for efficient CO<sub>2</sub> utilization but also highlight the importance of catalyst design in advancing sustainable chemical synthesis.</p></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":null,"pages":null},"PeriodicalIF":9.4000,"publicationDate":"2024-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Tandem Pt/TiO2 and Fe3C catalysts for direct transformation of CO2 to light hydrocarbons under high space velocity\",\"authors\":\"\",\"doi\":\"10.1016/j.jcis.2024.09.053\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>CO<sub>2</sub> hydrogenation to hydrocarbons under high space velocity is crucial for industrial applications, but traditional Fe-based catalysts often suffer from the low activity and poor stability. Herein, we report a new tandem catalyst system combining Pt/TiO<sub>2</sub> catalysts with Fe<sub>3</sub>C catalysts for the direct conversion of CO<sub>2</sub> into <em>C</em><sub>2</sub>-C<sub>4</sub> hydrocarbons under high space velocity. The Pt/TiO<sub>2</sub> component promotes *CO intermediate production with an enhanced Reverse Water-Gas Shift (RWGS) reaction efficiency, providing a highly reactive species for the Fe<sub>3</sub>C catalyst to achieve Fischer-Tropsch synthesis (FTS). By maximizing the contact interface between the Pt/TiO<sub>2</sub> and Fe-based components through a granule mixing configuration, we achieve significant enhancements in both CO<sub>2</sub> conversion rate (24.0 %) and <em>C</em><sub>2</sub>-C<sub>4</sub> hydrocarbons selectivity (51.1 %) under the gaseous hourly space velocity (GHSV) of 100000 mL g<sub>cat</sub><sup>−1</sup>h<sup>−1</sup>. Besides, excellent stability is achieved by the tandem catalysts with continuous catalysis for up to 80 h without significant decrease in activity. Through modulation of the reduction states of iron oxide, we effectively tune the composition of Fe-based catalyst, thereby tailoring the product distribution. Through this work, we not only offer a promising avenue for reducing CO<sub>2</sub> for efficient CO<sub>2</sub> utilization but also highlight the importance of catalyst design in advancing sustainable chemical synthesis.</p></div>\",\"PeriodicalId\":351,\"journal\":{\"name\":\"Journal of Colloid and Interface Science\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":9.4000,\"publicationDate\":\"2024-09-07\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Colloid and Interface Science\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0021979724021106\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Colloid and Interface Science","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021979724021106","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
在高空间速度下将 CO2 加氢转化为碳氢化合物对工业应用至关重要,但传统的铁基催化剂往往存在活性低和稳定性差的问题。在此,我们报告了一种结合了 Pt/TiO2 催化剂和 Fe3C 催化剂的新型串联催化剂体系,用于在高空间速度下将 CO2 直接转化为 C2-C4 碳氢化合物。Pt/TiO2 催化剂能促进 *CO 中间体的生成,提高水气反向变换 (RWGS) 反应的效率,为 Fe3C 催化剂提供高活性物质,从而实现费托合成 (FTS)。通过颗粒混合配置最大限度地提高 Pt/TiO2 和铁基组分之间的接触界面,我们在 100000 mL gcat-1h-1 气体时空速度(GHSV)条件下显著提高了 CO2 转化率(24.0%)和 C2-C4 碳氢化合物选择性(51.1%)。此外,串联催化剂具有极佳的稳定性,可连续催化长达 80 小时而活性不会显著降低。通过调节氧化铁的还原态,我们有效地调节了铁基催化剂的组成,从而调整了产物的分布。通过这项工作,我们不仅为还原二氧化碳以高效利用二氧化碳提供了一条前景广阔的途径,而且突出了催化剂设计在推进可持续化学合成中的重要性。
Tandem Pt/TiO2 and Fe3C catalysts for direct transformation of CO2 to light hydrocarbons under high space velocity
CO2 hydrogenation to hydrocarbons under high space velocity is crucial for industrial applications, but traditional Fe-based catalysts often suffer from the low activity and poor stability. Herein, we report a new tandem catalyst system combining Pt/TiO2 catalysts with Fe3C catalysts for the direct conversion of CO2 into C2-C4 hydrocarbons under high space velocity. The Pt/TiO2 component promotes *CO intermediate production with an enhanced Reverse Water-Gas Shift (RWGS) reaction efficiency, providing a highly reactive species for the Fe3C catalyst to achieve Fischer-Tropsch synthesis (FTS). By maximizing the contact interface between the Pt/TiO2 and Fe-based components through a granule mixing configuration, we achieve significant enhancements in both CO2 conversion rate (24.0 %) and C2-C4 hydrocarbons selectivity (51.1 %) under the gaseous hourly space velocity (GHSV) of 100000 mL gcat−1h−1. Besides, excellent stability is achieved by the tandem catalysts with continuous catalysis for up to 80 h without significant decrease in activity. Through modulation of the reduction states of iron oxide, we effectively tune the composition of Fe-based catalyst, thereby tailoring the product distribution. Through this work, we not only offer a promising avenue for reducing CO2 for efficient CO2 utilization but also highlight the importance of catalyst design in advancing sustainable chemical synthesis.
期刊介绍:
The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality.
Emphasis:
The journal emphasizes fundamental scientific innovation within the following categories:
A.Colloidal Materials and Nanomaterials
B.Soft Colloidal and Self-Assembly Systems
C.Adsorption, Catalysis, and Electrochemistry
D.Interfacial Processes, Capillarity, and Wetting
E.Biomaterials and Nanomedicine
F.Energy Conversion and Storage, and Environmental Technologies