Unravelling the nature, evolution and spatial gradients of active species and active sites in the catalyst bed of unpromoted and K/Ba-promoted Cu/Al2O3 during CO2 capture-reduction

Hyakutake, Tsuyoshi; Beek, Wouter van; Urakawa, Atsushi

doi:10.1039/c5ta09461e

Cited by 45 publications

(86 citation statements)

References 19 publications

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“…CO 2 hydrogenation to CO (RWGS), which has attracted wide attention because this process occupies the pivotal stage in the transitioning of CO 2 . Due to excellent selectivity to CO over the Cu‐base catalysts, they have been widely used for RWGS reaction . Besides, the supported Cr 2 O 3 ‐based materials have been documented as the most promising ones due to their high catalytic activity for CO 2 oxidative dehydrogenation of alkanes .…”

Section: Figurementioning

confidence: 99%

“…[28,29] Due to excellent selectivity to CO over the Cu-base catalysts, they have been widely used for RWGS reaction. [30,31] Besides, the supported Cr 2 O 3 -based materials have been documented as the most promising ones due to their high catalytic activity for CO 2 oxidative dehydrogenation of alkanes. [32] While the RWGS reaction is a key step in whole dehydrogenation process.…”

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confidence: 99%

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Facile Preparation of Inverse Nanoporous Cr₂O₃/Cu Catalysts for Reverse Water‐Gas Shift Reaction

et al. 2019

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The inverse oxide/metal structures represent a new class of heterogeneous catalysts with great research interests due to their diverse interfacial structures between oxides and metal supports, which often lead to unique catalytic properties. Herein, we report a facile and general strategy to prepare inverse catalysts with nanoporous structures by dealloying. As an example, inverse nanoporous Cr2O3/Cu (NP−Cr2O3/Cu) catalysts with a bi‐continuous nanoporous structure are fabricated by room temperature chemical dealloying of CrCuAl alloy in alkaline solution, which exhibit excellent performance in CO2 reduction to CO (reverse water‐gas shift, RWGS), significantly higher performance than the traditional Cu/Cr2O3 catalyst and inverse catalysts obtained by other traditional preparation methods. Density functional theory (DFT) calculation results show that CO2 reduction is evidently promoted by the synergistic effects of Cr2O3 cluster and nanoporous Cu. These results suggest a promising route for the preparation of various heterogeneous catalysts with tailored functionalities.

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confidence: 99%

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Facile Preparation of Inverse Nanoporous Cr₂O₃/Cu Catalysts for Reverse Water‐Gas Shift Reaction

et al. 2019

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“…In fact, studies on CO 2 hydrogenation catalysts based on alumina-supported Cu nanoparticles are rare,a nd the influence of CH 3 OH or the effect of the Lewis acidic support on activity/product selectivity are often overlooked. [15,[49][50][51][52][53][54][55] To understand the role of alumina, we reasoned that studying alumina-supported Cu nanoparticles in the absence of zinc oxide would be ideal. We thus prepared small and narrowly dispersed Cu nanoparticles on Al 2 O 3 via SOMC.…”

Section: Introductionmentioning

confidence: 99%

CO₂ Hydrogenation on Cu/Al₂O₃: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst

et al. 2019

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Selective hydrogenation of CO2 into methanol is a key sustainable technology, where Cu/Al2O3 prepared by surface organometallic chemistry displays high activity towards CO2 hydrogenation compared to Cu/SiO2, yielding CH3OH, dimethyl ether (DME), and CO. CH3OH formation rate increases due to the metal–oxide interface and involves formate intermediates according to advanced spectroscopy and DFT calculations. Al2O3 promotes the subsequent conversion of CH3OH to DME, showing bifunctional catalysis, but also increases the rate of CO formation. The latter takes place 1) directly by activation of CO2 at the metal–oxide interface, and 2) indirectly by the conversion of formate surface species and CH3OH to methyl formate, which is further decomposed into CH3OH and CO. This study shows how Al2O3, a Lewis acidic and non‐reducible support, can promote CO2 hydrogenation by enabling multiple competitive reaction pathways on the oxide and metal–oxide interface.

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“…However, considering the high reactivity of alumina toward many small molecules, including CH 3 OH (see below), for example, the dehydration of CH 3 OH to dimethyl ether (DME), the involvement of alumina during the hydrogenation of CO 2 should be considered. In fact, studies on CO 2 hydrogenation catalysts based on alumina‐supported Cu nanoparticles are rare, and the influence of CH 3 OH or the effect of the Lewis acidic support on activity/product selectivity are often overlooked …”

Section: Introductionmentioning

confidence: 99%

CO₂ Hydrogenation on Cu/Al₂O₃: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst

et al. 2019

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Selective hydrogenation of CO 2 into methanol is ak ey sustainable technology,w here Cu/Al 2 O 3 prepared by surface organometallic chemistry displays high activity to-wardsC O 2 hydrogenation compared to Cu/SiO 2 ,y ielding CH 3 OH, dimethyl ether (DME), and CO.C H 3 OH formation rate increases due to the metal-oxide interface and involves formate intermediates according to advanced spectroscopyand DFT calculations.A l 2 O 3 promotes the subsequent conversion of CH 3 OH to DME, showing bifunctional catalysis,b ut also increases the rate of CO formation. The latter takes place 1) directly by activation of CO 2 at the metal-oxide interface, and 2) indirectly by the conversion of formate surface species and CH 3 OH to methyl formate,w hich is further decomposed into CH 3 OH and CO.T his study shows howA l 2 O 3 ,aLewis acidic and non-reducible support, can promote CO 2 hydrogenation by enabling multiple competitive reaction pathways on the oxide and metal-oxide interface.Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi.

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Unravelling the nature, evolution and spatial gradients of active species and active sites in the catalyst bed of unpromoted and K/Ba-promoted Cu/Al₂O₃ during CO₂ capture-reduction

Abstract: Space- and time-resolved operando DRIFTS, XAFS, and XRD uncovered the involved surface chemical species and active sites, especially the unique functions of K and Cu, during the CO2 capture-reduction process.

Cited by 45 publications

References 19 publications

Facile Preparation of Inverse Nanoporous Cr₂O₃/Cu Catalysts for Reverse Water‐Gas Shift Reaction

Facile Preparation of Inverse Nanoporous Cr₂O₃/Cu Catalysts for Reverse Water‐Gas Shift Reaction

CO₂ Hydrogenation on Cu/Al₂O₃: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst

CO₂ Hydrogenation on Cu/Al₂O₃: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst

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Unravelling the nature, evolution and spatial gradients of active species and active sites in the catalyst bed of unpromoted and K/Ba-promoted Cu/Al2O3 during CO2 capture-reduction

Abstract: Space- and time-resolved operando DRIFTS, XAFS, and XRD uncovered the involved surface chemical species and active sites, especially the unique functions of K and Cu, during the CO2 capture-reduction process.

Cited by 45 publications

References 19 publications

Facile Preparation of Inverse Nanoporous Cr2O3/Cu Catalysts for Reverse Water‐Gas Shift Reaction

Facile Preparation of Inverse Nanoporous Cr2O3/Cu Catalysts for Reverse Water‐Gas Shift Reaction

CO2 Hydrogenation on Cu/Al2O3: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst

CO2 Hydrogenation on Cu/Al2O3: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst

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Unravelling the nature, evolution and spatial gradients of active species and active sites in the catalyst bed of unpromoted and K/Ba-promoted Cu/Al₂O₃ during CO₂ capture-reduction

Facile Preparation of Inverse Nanoporous Cr₂O₃/Cu Catalysts for Reverse Water‐Gas Shift Reaction

Facile Preparation of Inverse Nanoporous Cr₂O₃/Cu Catalysts for Reverse Water‐Gas Shift Reaction

CO₂ Hydrogenation on Cu/Al₂O₃: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst

CO₂ Hydrogenation on Cu/Al₂O₃: Role of the Metal/Support Interface in Driving Activity and Selectivity of a Bifunctional Catalyst