Mechanistic study of methanol synthesis from CO2 hydrogenation on Rh-doped Cu(111) surfaces

Liu, Lingna; Fan, Fei; Bai, Min; Xue, Fan; Ma, Xiangrong; Jiang, Zhao; Fang, Tao

doi:10.1016/j.mcat.2019.01.009

Cited by 70 publications

(35 citation statements)

References 63 publications

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“…In methanol synthesis: Rh metal surfaces are poorly examined by computational studies and there is no DFT study on pure Rh surfaces. Recently, Liu et al [208] explored the effect of Rh doped Cu(111) surfaces (Cu(111), Rh 3 Cu 6 (111), Rh 6 Cu 3 (111) and Rh ML surfaces) on CO 2 hydrogenation via RWGS pathway using GGA with PW91 functional together with DNP function. The calculated results shown both kinetic and thermodynamic facilitation of methanol synthesis, especially on Rh 3 Cu 6 (111) surface.…”

Section: Rh Catalytic Surfacesmentioning

confidence: 99%

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

et al. 2020

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Density functional theory (DFT) of the CO2 behavior on the catalyst surface provides valuable insights about the C=O bond activation, information about adsorption and dissociation of CO2, understanding the elementary steps involved in the mechanism of the CO2 hydrogenation reaction. Nowadays, DFT computational studies for the catalytic hydrogenation of CO2 are becoming very popular. Therefore, this article is focused on a comprehensive review of the DFT studies in thermocatalytic hydrogenation of CO2 at the gas‐surface interface and discusses three aspects: 1) processes taking place on the surfaces and facets of transition metal heterogeneous catalysts, 2) adsorption of CO2 on surfaces of different transition metals; 3) current understanding of reaction mechanisms taking place on the catalytic surface for the production of different compounds. A detailed schematic overview of the possible CO2 hydrogenation mechanisms and DFT simulations presented here will enhance the current understanding of the CO2 catalytic hydrogenation.

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Section: Rh Catalytic Surfacesmentioning

confidence: 99%

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

et al. 2020

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“…However, there is still debate regarding the reaction mechanism and catalyst requirements [4,10,11]. As far as catalysts are concerned, efforts have been made to improve the performance of CZA by either replacing/doping Cu with noble metals (e.g., Pt, Pd) [12][13][14][15] or by adding oxides in order to enhance the adsorption properties of the support and to increase the dispersion of the Cu phases [16][17][18][19][20][21]. This is the reason why the majority of studies pinpoint some sort of coupling in the mechanism between the copper phase and the support oxide, with the latter being the anchor point for one of the oxygen atoms of CO 2 [22,23].…”

Section: Introductionmentioning

confidence: 99%

CO2 Hydrogenation to Methanol over La2O3-Promoted CuO/ZnO/Al2O3 Catalysts: A Kinetic and Mechanistic Study

2020

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The hydrogenation of CO2 to methanol has been investigated over CuO/ZnO/Al2O3 (CZA) catalysts, where a part of the Al2O3 (0, 25, 50, 75, or 100%) was substituted by La2O3. Results of catalytic performance tests obtained at atmospheric pressure showed that the addition of La2O3 generally resulted in a decrease of CO2 conversion and in an increase of methanol selectivity. Optimal results were obtained for the CZA-La50 catalyst, which exhibited a 30% higher yield of methanol, compared to the un-promoted sample. This was attributed to the relatively high specific surface area and porosity of this material, the creation of basic sites of moderate strength, which enhance adsorption of CO2 and intermediates that favor hydrogenation steps, and the ability of the catalyst to maintain a large part of the copper in its metallic form under reaction conditions. The reaction mechanism was studied with the use of in situ infrared spectroscopy (DRIFTS). It was found that the reaction proceeded with the intermediate formation of surface formate and methoxy species and that both methanol and CO were mainly produced via a common formate intermediate species. The kinetic behavior of the best performing CZA-La50 catalyst was investigated in the temperature range 190–230 °C as a function of the partial pressures of H2 (0.3–0.9 atm) and CO2 (0.05–0.20 atm), and a kinetic model was developed, which described the measured reaction rates satisfactorily.

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“…RWGSR activities are also significantly depending on the shape and exposed crystal face of catalysts because they can determine the virtual adsorption energy and desorption energy of intermediates in the reaction process (Liu et al, 2019 ).…”

Section: Catalytic Systemmentioning

confidence: 99%

Recent Advances in Supported Metal Catalysts and Oxide Catalysts for the Reverse Water-Gas Shift Reaction

Chen

Song

et al. 2020

Front. Chem.

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The reverse water-gas shift reaction (RWGSR), a crucial stage in the conversion of abundant CO 2 into chemicals or hydrocarbon fuels, has attracted extensive attention as a renewable system to synthesize fuels by non-traditional routes. There have been persistent efforts to synthesize catalysts for industrial applications, with attention given to the catalytic activity, CO selectivity, and thermal stability. In this review, we describe the thermodynamics, kinetics, and atomic-level mechanisms of the RWGSR in relation to efficient RWGSR catalysts consisting of supported catalysts and oxide catalysts. In addition, we rationally classify, summarize, and analyze the effects of physicochemical properties, such as the morphologies, compositions, promoting abilities, and presence of strong metal-support interactions (SMSI), on the catalytic performance and CO selectivity in the RWGSR over supported catalysts. Regarding oxide catalysts (i.e., pure oxides, spinel, solid solution, and perovskite-type oxides), we emphasize the relationships among their surface structure, oxygen storage capacity (OSC), and catalytic performance in the RWGSR. Furthermore, the abilities of perovskite-type oxides to enhance the RWGSR with chemical looping cycles (RWGSR-CL) are systematically illustrated. These systematic introductions shed light on development of catalysts with high performance in RWGSR.

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Mechanistic study of methanol synthesis from CO2 hydrogenation on Rh-doped Cu(111) surfaces

Cited by 70 publications

References 63 publications

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

CO2 Hydrogenation to Methanol over La2O3-Promoted CuO/ZnO/Al2O3 Catalysts: A Kinetic and Mechanistic Study

Recent Advances in Supported Metal Catalysts and Oxide Catalysts for the Reverse Water-Gas Shift Reaction

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Mechanistic study of methanol synthesis from CO2 hydrogenation on Rh-doped Cu(111) surfaces

Cited by 70 publications

References 63 publications

Recent Developments in the Modelling of Heterogeneous Catalysts for CO2 Conversion to Chemicals

Recent Developments in the Modelling of Heterogeneous Catalysts for CO2 Conversion to Chemicals

CO2 Hydrogenation to Methanol over La2O3-Promoted CuO/ZnO/Al2O3 Catalysts: A Kinetic and Mechanistic Study

Recent Advances in Supported Metal Catalysts and Oxide Catalysts for the Reverse Water-Gas Shift Reaction

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Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals

Recent Developments in the Modelling of Heterogeneous Catalysts for CO₂ Conversion to Chemicals