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The construction of iron-based catalysts encapsulated by graphite for CO2 hydrogenation to light olefins
Chemical Engineering Journal ( IF 15.1 ) Pub Date : 2024-04-26 , DOI: 10.1016/j.cej.2024.151674
Zhongyue Luo , Fei Han , Pengze Zhang , Yali Zhao , Sibo Huang , Qingxin Guan , Wei Li

Developing efficient catalytic materials and unveiling the active factors are significant for selective hydrogenation of CO to light olefins (C). Herein, FeO-FeC nanoparticles coated by graphite without other doped elements were synthesized successfully. The optimal catalyst exhibited CO conversion of 48.0%, C space–time yield of 29.0 mmol·g·h, and a stability of 100 h (3.0 MPa, 320 °C, and GHSV = 12000 mL·g·h). The core–shell structure derived from the strong interaction between the phenolic hydroxyl group of resin and iron ions, as well as the encapsulation of the copolymer P123. The characterization results revealed that the size of core–shell particles and thickness of graphite layers could be regulated by P123, which affected the conversion of CO and products distribution significantly. Moreover, the combined results of diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) and Raman spectra suggested small particle size and thin graphite shell strengthen the adsorption and conversion of CO, playing an important role in the formation of light olefins. This work proposes a simple and feasible synthesis strategy to construct FeO-FeC particles encapsulated by graphite shell, which provides insights into catalysts design and the reaction mechanism of CO conversion to light olefins.

中文翻译:

石墨封装铁基催化剂的构建用于CO2加氢制轻质烯烃

开发高效催化材料并揭示活性因子对于CO选择性加氢制低碳烯烃(C)具有重要意义。在此,成功合成了石墨包覆的 FeO-FeC 纳米颗粒,不含其他掺杂元素。最佳催化剂的CO转化率为48.0%,C时空产率为29.0 mmol·g·h,稳定性为100 h(3.0 MPa,320 ℃,GHSV = 12000 mL·g·h)。核壳结构源自树脂的酚羟基与铁离子之间的强相互作用,以及共聚物P123的封装。表征结果表明,P123可以调节核壳颗粒的尺寸和石墨层的厚度,从而显着影响CO的转化和产物分布。此外,漫反射红外傅里叶变换光谱(DRIFT)和拉曼光谱的综合结果表明,小粒径和薄石墨壳增强了CO的吸附和转化,在轻质烯烃的形成中发挥了重要作用。这项工作提出了一种简单可行的合成策略来构建石墨壳封装的 FeO-FeC 颗粒,为催化剂设计和 CO 转化为轻质烯烃的反应机理提供了见解。
更新日期:2024-04-26
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