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Unraveling the Role of Zinc on Bimetallic Fe5C2–ZnO Catalysts for Highly Selective Carbon Dioxide Hydrogenation to High Carbon α-Olefins
ACS Catalysis ( IF 12.9 ) Pub Date : 2021-02-02 , DOI: 10.1021/acscatal.0c04627
Chao Zhang 1 , Chenxi Cao 1 , Yulong Zhang 1 , Xianglin Liu 1 , Jing Xu 1 , Minghui Zhu 1 , Weifeng Tu 2 , Yi-Fan Han 1, 2
Affiliation  

In this work, Fe–Zn catalysts were prepared, characterized, and examined for the synthesis of linear high carbon α-olefins (LAOs; C ≥ 4) directly from CO2 hydrogenation. The relationship of performance and structure has been established to unravel the role of ZnO in bimetallic Fe5C2–ZnO catalysts. A Fe2Zn1 catalyst showed high selectivity to C2–C7 olefins (a selectivity of 57.8% in gas phase) after 200 h of time-on-stream and total C4+ olefins selectivity in liquid products of 81.9% with 85.9% LAOs in C4+ alkenes at a CO2 conversion of 35.0%. The dominant mechanism of deactivation was ascribed to phase transformation from FeCx to FeOx in comparison with Fe2O3 and Fe5Zn1. Zn and Na were proved to migrate onto the surface during the activation process. The interaction between Zn and Na could suppress the oxidation of FeCx by H2O and CO2. This study revealed the deactivation mechanism and stabilization effects of Zn on the active phase of FeCx during CO2 hydrogenation.

中文翻译:

揭示锌在高选择性碳氢化为高碳α-烯烃的双金属Fe 5 C 2 -ZnO催化剂上的作用

在这项工作中,制备,表征和检验了直接由CO 2加氢合成线性高碳α-烯烃(LAOs; C≥4)的Fe-Zn催化剂。已经建立了性能和结构之间的关系,以阐明ZnO在双金属Fe 5 C 2 -ZnO催化剂中的作用。在运行200小时后,Fe2Zn1催化剂显示出对C 2 -C 7烯烃的高选择性(气相中的选择性为57.8%),液体产品中的总C 4+烯烃选择性为81.9%,其中LAO为85.9%。 C 4+烯烃的CO 2转化率为35.0%。失活的主要机理归因于FeC的相变与Fe 2 O 3和Fe5Zn1相比, x为FeO x。锌和钠被证明在活化过程中迁移到表面上。Zn和Na的相互作用可以抑制H 2 O和CO 2对FeC x的氧化。这项研究揭示了Zn在CO 2加氢过程中对FeC x活性相的失活机理和稳定作用。
更新日期:2021-02-19
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