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Design of efficient ZnO/ZrO2 modified CuCoAl catalysts for boosting higher alcohol synthesis in syngas conversion
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2021-09-21 , DOI: 10.1016/j.apcatb.2021.120739
Chao Huang 1, 2 , Can Zhu 1, 2 , Mingwei Zhang 1 , Jiangang Chen 1 , Kegong Fang 1
Affiliation  

Selective synthesis of higher alcohols from syngas conversion is highly desirable, but still very challenging. Here, focusing on the commonly used CuCoAl (CCA) catalyst, we attempted to reconcile the capability of the non-dissociation of CO species and the activation of H2 through adding ZnO modified ZrO2 composite into the catalyst for the promotion of higher alcohols synthesis. Under the guidance of such concept, a series of CCA|ZnO/ZrO2 (m: n) modified catalysts (m: n, represent the mass ratio of ZnO to ZrO2) were prepared by mortar-mixing CuCoAl and ZnO/ZrO2 components (2/1 wt ratio). It was found that the CCA|ZnO/ZrO2 (4:1) catalyst showed a highest total alcohols (ROH) selectivity of 42.6 wt% with excellent C2+OH/ROH fraction of 83.7% among the investigated catalysts. The surface [H*]/[C*] ratio of CCA|ZnO/ZrO2 catalysts, as revealed by (CO + H2)-TPD-MS results, increased with the rise of ZnO/ZrO2 ratio. Moreover, the CCA|ZnO/ZrO2 (4:1) catalyst with moderate [H*]/[C*] ratio could acquire the highest ROH selectivity and best space time yield of total alcohols (STYROH) due to that the balance of relative amount of CO*, CHx* and H* species provided the more probability of CnHx*-CO* coupling reaction for higher alcohols synthesis, rather than the hydrogenation reaction of CHx* or CnHx* species and water gas shift reaction.



中文翻译:

用于促进合成气转化中高级醇合成的高效 ZnO/ZrO2 改性 CuCoAl 催化剂的设计

从合成气转化中选择性合成高级醇是非常理想的,但仍然非常具有挑战性。在此,针对常用的CuCoAl(CCA)催化剂,我们尝试通过在催化剂中加入ZnO改性ZrO 2复合物来促进CO物种的不解离和H 2的活化,以促进高级醇的合成. 在此理念的指导下,通过砂浆混合CuCoAl和ZnO/ZrO 2制备了一系列CCA|ZnO/ZrO 2 (m:n)改性催化剂(m:n,代表ZnO与ZrO 2的质量比)组分(2/1 重量比)。发现CCA|ZnO/ZrO 2(4:1) 催化剂显示最高的总醇 (ROH) 选择性为 42.6 wt%,在所研究的催化剂中具有 83.7% 的优异 C 2+ OH/ROH 分数。(CO + H 2 )-TPD-MS 结果表明,CCA|ZnO/ZrO 2催化剂的表面 [H*]/[C*] 比值随着 ZnO/ZrO 2比值的增加而增加。此外,具有中等 [H*]/[C*] 比的 CCA|ZnO/ZrO 2 (4:1) 催化剂可以获得最高的 ROH 选择性和最佳的总醇 (STY ROH )时空产率,这是由于平衡相对数量的 CO*、CH x * 和 H* 物种提供了更多的 C n H x概率  *-CO*偶联反应用于高级醇的合成,而不是CH x * 或C n H x * 物种的加氢反应和水煤气变换反应。

更新日期:2021-09-29
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