Tuning the hydrogenation of CO2 to lower olefins: Impact of Pt in K–doped Fe–Mn catalysts

IF 7.2 2区 工程技术 Q1 CHEMISTRY, MULTIDISCIPLINARY
Tomohiro Hojo , Tomohiro Yabe , Kazuya Yamaguchi
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引用次数: 0

Abstract

Fe-based catalysts are promising for the hydrogenation of CO2 to olefins, contributing to the mitigation of CO2 emissions. Low-pressure conditions (∼1 MPa) are preferred for the selective synthesis of lower olefin because these conditions suppress carbon chain growth and olefin re-absorption which leads to hydrogenation of olefins to paraffins. In this study, K-doped Fe–Mn–Pt/Al2O3 catalysts that could react at 1 MPa were prepared, with a focus on the role and position of Pt active sites. K–Fe17Mn2/Pt1/Al2O3 was prepared by first supporting Pt on Al2O3 followed by Fe–Mn oxide; it exhibited the highest C2–5 olefin selectivity of 28 %. Pt promoted the reverse water-gas shift reaction, and in combination with Mn, facilitated iron oxide reduction and Fe5C2 formation, enhancing the C2–5 olefin selectivity. Compared with the Pt active sites in K–Pt1/Fe17Mn2/Al2O3, which was prepared by first supporting Fe–Mn oxide on Al2O3 followed by Pt, those in K–Fe17Mn2/Pt1/Al2O3 existed around the Fe–Mn active sites. Pt continued to contribute to the Fe species reduction and the stable supply of CO, leading to improved C2–5 olefin selectivity.
调整CO2加氢以降低烯烃:Pt在k掺杂Fe-Mn催化剂中的影响
铁基催化剂有望将二氧化碳氢化为烯烃,有助于减少二氧化碳排放。低压条件(~ 1 MPa)是选择性合成低烯烃的首选条件,因为低压条件抑制碳链生长和烯烃再吸收,从而导致烯烃加氢生成石蜡。本研究制备了能在1 MPa下反应的k掺杂Fe-Mn-Pt /Al2O3催化剂,重点研究了Pt活性位点的作用和位置。先在Al2O3上负载Pt,再在Fe-Mn氧化物上负载制备K-Fe17Mn2 /Pt1/Al2O3;对C2-5烯烃的选择性最高,为28% %。Pt促进了逆水气转换反应,与Mn结合促进了氧化铁的还原和Fe5C2的生成,提高了C2-5烯烃的选择性。与先在Al2O3上负载Fe-Mn氧化物后再在Pt上负载K-Pt1 /Fe17Mn2/Al2O3中制备的Pt活性位点相比,K-Fe17Mn2 /Pt1/Al2O3中的Pt活性位点存在于Fe-Mn活性位点周围。Pt继续有助于Fe的减少和CO的稳定供应,从而提高了C2-5烯烃的选择性。
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来源期刊
Journal of CO2 Utilization
Journal of CO2 Utilization CHEMISTRY, MULTIDISCIPLINARY-ENGINEERING, CHEMICAL
CiteScore
13.90
自引率
10.40%
发文量
406
审稿时长
2.8 months
期刊介绍: The Journal of CO2 Utilization offers a single, multi-disciplinary, scholarly platform for the exchange of novel research in the field of CO2 re-use for scientists and engineers in chemicals, fuels and materials. The emphasis is on the dissemination of leading-edge research from basic science to the development of new processes, technologies and applications. The Journal of CO2 Utilization publishes original peer-reviewed research papers, reviews, and short communications, including experimental and theoretical work, and analytical models and simulations.
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