Potassium‐Promoted Molybdenum Carbide as a Highly Active and Selective Catalyst for CO<sub>2</sub> Conversion to CO

Porosoff, Marc D.; Baldwin, Jeffrey W.; Peng, Xi; Mpourmpakis, Giannis; Willauer, Heather D.

doi:10.1002/cssc.201700412

Cited by 78 publications

(68 citation statements)

References 50 publications

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“…[4a, 6] Moreover,t he La-promoted Fe 0.975 Ir 0.025 O 3 can facilitatet he generation of CO from CO 2 decomposition( CO 2 conversion of less than 2%)w ithout the addition of H 2 gas at 1,273 K. [7] Therefore, it is necessary to search non-noble metal catalysta lternatives to reduce the high cost for this important process. [4a,c, 6a, 7] Recent successful investigation of cobalt-modified molybdenumc arbide( Co-Mo 2 C) wasr eportedt od ecompose CO 2 gas with ac onversion of 9.5 %a nd CO selectivity of 98.1 %a t5 73 K. [4b] Furthermore, K-promoted Mo 2 C( K-Mo 2 C/g-Al 2 O 3 )a sa na ctive and selective catalystachieved high efficiency for CO 2 conversion of 40 %a tr elatively high temperature of 723 K. [8] Polycrystalline hexagonal a-Mo 2 Cw ith ac onversion of 16 %a nd CO selectivity of > 99 %a t6 73 Kw as also realized. [9] However,t he development of ac ost-effective catalytic system to enable the cleana nd efficient decomposition of CO 2 to CO at low temperatures is still required.…”

Section: Introductionmentioning

confidence: 99%

Efficient Reduction of CO₂ to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

Yin

Yuan

et al. 2018

Chemistry A European J

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The route of converting CO to CO by reverse water-gas shift (RWGS) reaction is of particular interest due to the direct use of CO as feedstock in many significant industrial processes. Here, an engineered cobalt-cobalt oxide core-shell catalyst (Co@CoO) with nanochains structure has been made for the efficient reduction of CO to useful CO. Owing to the excellent performance for H activation of metal nanoparticles and the enhanced absorption and activation for CO molecule of defective metal oxides, the unique synergistic effect of metallic Co and encapsulating coordinatively unsaturated CoO species shows high performance for clean generation of CO under moderate and practical conditions. Furthermore, with N-dopant into the defective CoO shell, the Co@CoO-N achieves the highest conversion of 19.2 % and an exceptional CO evolution rate of 96 mL min g at 523 K with a gas hourly space velocity (GHSV) of 42,000 mL g h , which is comparable with the previously reported materials under identical conditions.

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Section: Introductionmentioning

confidence: 99%

Efficient Reduction of CO₂ to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

Yin

Yuan

et al. 2018

Chemistry A European J

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“…As a competing reaction in the synthesis of methanol, CO 2 hydrogenation to CO is also an efficient path for the conversion and storage of energy. CO is a basic chemical product that can be converted to a variety of hydrocarbons and energy‐rich chemicals using some mature technologies . Therefore, the technological breakthrough of CO 2 hydrogenation to produce methanol or CO will bring huge environmental and economic benefits .…”

Section: Introductionmentioning

confidence: 99%

The Synergistic Effect of CuZnCeO_x in Controlling the Formation of Methanol and CO from CO₂ Hydrogenation

Qin

Guan

et al. 2018

ChemCatChem

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CO 2 hydrogenation will be essential for a sustainable society if methanol and CO can be efficiently obtained using appropriate catalysts. In this paper, a highly efficient CuZnCeO x catalyst was synthesized using a parallel flow coprecipitation method, and was evaluated in CO 2 hydrogenation to produce methanol and CO. Interestingly, the catalyst shows excellent activity and stability, and the selectivity of the products can be controlled by the amount of CeO x . Characterization results show that a significant synergistic effect between Cu and metal oxides (ZnO and/or CeO x ) was observed at the composite catalysts. Cu plays a critical role in the activation of H 2 , and CeO x strongly adsorbs CO 2 . CeO x improved the dispersion of Cu nanoparticles and promoted the spillover of atomic hydrogen, which was beneficial to the generation of methanol. Meanwhile, ZnO exhibited weak adsorption ability for CO 2 , which was beneficial for the generation of CO. In addition, ZnO can significantly improve the dispersion of the CeO x nanoparticles. Both the dispersion of active sites and the activation abilities of CO 2 are critical for catalyst activity and product selectivity. Thus, the ternary catalyst CuZnCeO x shows higher performance than the binary catalysts (CuZnO x and CuCeO x ) in the CO 2 hydrogenation reaction. This paper provides a viable way to produce selectively methanol or CO from CO 2 hydrogenation.[a] Dr.

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“…This option is particularly attractive, as CO 2 provides an essentially untapped source of carbon as aC 1 feedstock. CO 2 can be converted catalytically to other chemicals,s uch as CO, [8] methanol, [9] methane, [10] and dimethyl carbonate. [11] However, forC O 2 to be utilized, in most cases it must initially be activated through electron transfer,w hichr esults in ab ent CO 2 À anion.…”

Section: Introductionmentioning

confidence: 99%

Design of Copper‐Based Bimetallic Nanoparticles for Carbon Dioxide Adsorption and Activation

et al. 2018

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Cu-based nanoparticles (NPs) are promising candidates for the catalytic hydrogenation of CO to useful chemicals because of their low cost. However, CO adsorption and activation on Cu is not feasible. In this work we demonstrate a computational framework that identifies Cu-based bimetallic NPs able to adsorb and activate CO based on DFT calculations. We screen a series of heteroatoms on Cu-based NPs based on their preference to occupy a surface site on the NP and to adsorb and activate CO . We revealed two descriptors for CO adsorption on the bimetallic NPs, the heteroatom (i) local d-band center and (ii) electropositivity, which both drive an effective charge transfer from the NP to CO . We identified the CuZr bimetallic NP as a candidate nanostructure for CO adsorption and showed that although the Zr sites can be oxidized because of their high oxophilicity, they are still able to adsorb and activate CO strongly. Importantly, our computational results are verified by targeted synthesis, characterization, and CO adsorption experiments that demonstrate that i) Zr segregates on the surface of Cu, ii) Zr is oxidized to form a bimetallic mixed CuZr oxide catalyst, which iii) can strongly adsorb CO , whereas Cu NPs cannot. Overall our work highlights the importance of the generation of binding sites on a NP surface based on (catalyst) stability and electronic structure properties, which can lead to the design of more effective CO reduction catalysts.

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Potassium‐Promoted Molybdenum Carbide as a Highly Active and Selective Catalyst for CO₂ Conversion to CO

Cited by 78 publications

References 50 publications

Efficient Reduction of CO₂ to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

Efficient Reduction of CO₂ to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

The Synergistic Effect of CuZnCeO_x in Controlling the Formation of Methanol and CO from CO₂ Hydrogenation

Design of Copper‐Based Bimetallic Nanoparticles for Carbon Dioxide Adsorption and Activation

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Potassium‐Promoted Molybdenum Carbide as a Highly Active and Selective Catalyst for CO2 Conversion to CO

Cited by 78 publications

References 50 publications

Efficient Reduction of CO2 to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

Efficient Reduction of CO2 to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

The Synergistic Effect of CuZnCeOx in Controlling the Formation of Methanol and CO from CO2 Hydrogenation

Design of Copper‐Based Bimetallic Nanoparticles for Carbon Dioxide Adsorption and Activation

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Potassium‐Promoted Molybdenum Carbide as a Highly Active and Selective Catalyst for CO₂ Conversion to CO

Efficient Reduction of CO₂ to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

Efficient Reduction of CO₂ to CO Using Cobalt–Cobalt Oxide Core–Shell Catalysts

The Synergistic Effect of CuZnCeO_x in Controlling the Formation of Methanol and CO from CO₂ Hydrogenation