Cu carbonyls enhance the performance of Ru-based SILP water–gas shift catalysts: a combined in situ DRIFTS and DFT study,Catalysis Science & Technology

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Cu carbonyls enhance the performance of Ru-based SILP water–gas shift catalysts: a combined in situ DRIFTS and DFT study
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2019-11-27 , DOI: 10.1039/c9cy01852b
Dominik Blaumeiser _{1,

2,

3,

4,

5} , Robert Stepić _{3,

4,

5,

6,

7} , Patrick Wolf _{3,

4,

5,

8} , Christian R. Wick _{3,

4,

5,

6,

7} , Marco Haumann _{3,

4,

5,

8} , Peter Wasserscheid _{3,

4,

5,

8,

9} , David M. Smith _{10,

11,

12,

13,

14} , Ana-Sunčana Smith _{3,

4,

5,

6,

7} , Tanja Bauer _{1,

2,

3,

4,

5} , Jörg Libuda _{1,

2,

3,

4,

5}

Affiliation

Ru-based supported ionic liquid phase (SILP) catalysts efficiently promote the water–gas shift reaction (WGSR). The addition of CuCl further improves the performance. This is attributed to the formation of labile Cu carbonyl species, which act as CO shuttles in the ionic liquid (IL) phase. We apply in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to monitor the formation of these Cu carbonyls in an imidazolium-based SILP system. To aid the identification of the relevant Cu carbonyls, we perform density functional theory (DFT) calculations. In the present study, we investigate [Ru(CO)₃Cl₂]₂/CuCl/[C₄C₁C₁Im]Cl/Al₂O₃ and CuCl/[C₄C₁C₁Im]Cl/Al₂O₃ with various CuCl : IL ratios. The relevant Cu carbonyls are identified as neutral CuCl monomers and dimers, as well as monoanionic monomers and dimers. Moreover, we demonstrate that the ratio of the individual Cu carbonyl species depends on the CuCl : IL ratio.

中文翻译：

铜羰基化合物增强Ru基SILP水煤气变换催化剂的性能：原位DRIFTS和DFT结合研究

钌基负载型离子液体（SILP）催化剂有效地促进了水煤气变换反应（WGSR）。CuCl的添加进一步改善了性能。这归因于不稳定的铜羰基物质的形成，其在离子液体（IL）相中充当CO穿梭。我们应用原位漫反射红外傅里叶变换光谱（DRIFTS）来监视基于咪唑鎓的SILP系统中这些铜羰基的形成。为了帮助识别相关的羰基铜，我们执行密度泛函理论（DFT）计算。在本研究中，我们研究[Ru（CO）₃ Cl ₂ ] ₂ / CuCl / [C ₄ C ₁ C ₁ Im] Cl / Al ₂O ₃和具有各种CuCl：IL比率的CuCl / [C ₄ C ₁ C ₁ Im] Cl / Al ₂ O ₃。相关的羰基铜被确定为中性CuCl单体和二聚体，以及单阴离子单体和二聚体。此外，我们证明了各个羰基铜物种的比例取决于CuCl：IL的比例。

更新日期：2019-11-27

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