Regulating the location of metal promoters in CuFe-based catalysts for enhanced CO2 hydrogenation to higher alcohols

IF 13.1 1区 化学 Q1 Energy
Qixin Fan , Na Liu , Jingming Zhao , Yang Yu , Yannan Sun , Yu Han , Jixin Zhang , Aimin Wang , Qingjie Ge , Jian Wei , Jian Sun
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Abstract

Regulating the location of the metal promoters plays a vital role in catalyst structure and its catalytic behavior during CO2 hydrogenation to higher alcohols. Herein, we selected the metal promoters with a precipitation pH similar to that of Cu2+ or Fe3+ to prepare a series of CuFe-based catalysts. Characterization results show that doping Al or Cr promoter, located with the Fe phase, suppressed the excessive carburization of the Fe phase and maintained an optimal proportion between Fe3O4 and amorphous iron carbide (FeCx), thus exhibiting superior catalytic activity and stability. In contrast, doping Zn or In promoter, located with the Cu phase, underwent a deeper carburization and formed more crystalline FeCx, showing an inferior performance. The CuFeCr catalyst achieved the highest space-time yield of 330 mg gcat-1 h−1 for higher alcohols among these catalysts. This study provides a novel strategy for optimizing the structure of the active phases for CO2 hydrogenation.

Abstract Image

调节cufe基催化剂中金属促进剂的位置以促进CO2加氢生成高级醇
在CO2加氢制高级醇过程中,金属促进剂位置的调节对催化剂结构及其催化行为起着至关重要的作用。本文选择沉淀pH值与Cu2+或Fe3+相近的金属促进剂制备了一系列cufe基催化剂。表征结果表明,在Fe相中掺杂Al或Cr促进剂,抑制了Fe相的过度渗碳,保持了Fe3O4与非晶态碳化铁(FeCx)的最佳比例,表现出优异的催化活性和稳定性。相比之下,掺杂Zn或In的促进剂位于Cu相中,其渗碳更深,形成的FeCx晶体更多,性能较差。CuFeCr催化剂对高阶醇的空时产率最高,为330 mg gcat-1 h -1。该研究为优化CO2加氢活性相的结构提供了一种新的策略。
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来源期刊
Journal of Energy Chemistry
Journal of Energy Chemistry CHEMISTRY, APPLIED-CHEMISTRY, PHYSICAL
CiteScore
19.10
自引率
8.40%
发文量
3631
审稿时长
15 days
期刊介绍: The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies. This journal focuses on original research papers covering various topics within energy chemistry worldwide, including: Optimized utilization of fossil energy Hydrogen energy Conversion and storage of electrochemical energy Capture, storage, and chemical conversion of carbon dioxide Materials and nanotechnologies for energy conversion and storage Chemistry in biomass conversion Chemistry in the utilization of solar energy
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