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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
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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
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)(3)Cl-2](2)/CuCl/[C(4)C(1)C(1)Im]Cl/Al2O3 and CuCl/[C(4)C(1)C(1)Im]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.
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机译:Ru-based支持离子液体阶段(单列直插式组件)催化剂有效促进水煤气转移反应(WGSR)。提高了性能。不稳定的形成羰基铜物种,在离子液体中充当公司航天飞机(IL)阶段。红外傅里叶变换光谱学(飘)监控这些铜金属羰基合物的形成一个imidazolium-based单列直插式组件系统。识别相关的铜金属羰基合物,我们执行密度泛函理论(DFT)计算。调查[俄文(有限公司)(3)Cl-2] (2) / CuCl / (C (4) C (1) C (1) Im] Cl /氧化铝和CuCl / (C (4) C (1) C (1) Im] Cl /氧化铝与不同CuCl: IL比率。确认为中性CuCl单体和二聚体,以及monoanionic单体和二聚体。此外,我们证明的比值取决于个人铜羰基物种CuCl:的手段。
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