Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts

Razdan, Neil K.; Kumar, Anurag; Bhan, Aditya

doi:10.1016/j.jcat.2019.03.016

Cited by 24 publications

(20 citation statements)

References 33 publications

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“…The incorporation of ZnO into ZrO 2 to form solid solution enhanced the signal at g value of 2.003 and thus the generation of oxygen vacancies over both ZnO-ZrO 2 and K + -ZnO-ZrO 2 samples. We believe that the increased density of oxygen vacancy sites favours the activation of CO as well as H 2 30,45,47 .…”

Section: Resultsmentioning

confidence: 91%

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

et al. 2020

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Synthesis of ethanol from non-petroleum carbon resources via syngas (a mixture of H 2 and CO) is an important but challenging research target. The current conversion of syngas to ethanol suffers from low selectivity or multiple processes with high energy consumption. Here, we report a high-selective conversion of syngas into ethanol by a triple tandem catalysis. An efficient trifunctional tandem system composed of potassium-modified ZnO-ZrO 2 , modified zeolite mordenite and Pt-Sn/SiC working compatibly in syngas stream in one reactor can afford ethanol with a selectivity of 90%. We demonstrate that the K + -ZnO-ZrO 2 catalyses syngas conversion to methanol and the mordenite with eight-membered ring channels functions for methanol carbonylation to acetic acid, which is then hydrogenated to ethanol over the Pt-Sn/SiC catalyst. The present work offers an effective methodology leading to high selective conversion by decoupling a single-catalyst-based complicated and uncontrollable reaction into well-controlled multi-steps in tandem in one reactor.

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Section: Resultsmentioning

confidence: 91%

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

et al. 2020

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“…Indeed, one can envision that nanoparticles of the MoC 1.1 type could be responsible for the activity seen over MoC x /ZSM-5 catalysts when transforming methane into larger hydrocarbons. [16][17][18]21 Computational study. To disclose the chemistry behind the described experiments for the MoC x /Au(111) systems, methane adsorption and first C-H bond scission have been studied on eight different supported MoC y nanoparticles with C/Mo ratios ranging from 0.67 to 1.50, as in the experiments.…”

Section: Resultsmentioning

confidence: 99%

“…Such a type of dissociative interaction probably occurs when nanoparticles of MoC y are dispersed in the cages of zeolites and methane is transformed into ethane, benzene and other hydrocarbons. [16][17][18]21…”

Section: Unravelling Trends For C-h Bond Activation On Bulk Surfaces and Nanostructures Of Molybdenum Carbides To Further Investigate Keymentioning

confidence: 99%

“…12,13 On these systems, cooperative interactions between cation and oxide sites are behind the dissociation of the first C-H bond in methane with energy barriers below 0.5 eV. 12,13,14 Transition metal carbides (TMCs) have also been tested as possible catalysts for methane conversion, 7,[15][16][17][18] although the most stable extended surfaces of typical TMCs such as MoC and TiC exhibit a very low reactivity towards methane with no evidence of dissociation. 7,19 Theoretical calculations suggested that metal-terminated metastable surfaces of carbides could be active for the dissociation of methane.…”

Section: Introductionmentioning

confidence: 99%

“…In fact, it is known that TMC nanoparticles supported inside zeolites can catalyse the conversion of methane into ethane, benzene and other hydrocarbons. [16][17][18]21 In principle, both the structure of the nanoparticle and its carbon/metal ratio could affect its ability to bind and dissociate methane.…”

Section: Introductionmentioning

confidence: 99%

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Boosting the activity of transition metal carbides towards methane activation by nanostructuring

Figueras

Gutiérrez

Prats

et al. 2020

Phys. Chem. Chem. Phys.

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Multilayered Two‐Dimensional V₂CT_x MXene for Methane Dehydroaromatization

et al. 2020

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We report a thermally stable multilayered two‐dimensional vanadium carbide (V2CTx) MXenes catalyst for the direct conversion of methane (CH4) into benzene (C6H6). The multilayered carbide structure shows state‐of‐the‐art CH4 conversion 11.8 % with a C6H6 formation rate of 1.9 mmol gcat−1h−1 (4.84 % C6H6 yield) at 700 °C, which is comparable to the benchmark Mo/ZSM‐5 catalyst. The structure‐activity relationship was explored by numerous characterization techniques including in‐situ/operando Raman‐MS, ex‐situ X‐ray diffraction (XRD), scanning electron microscopy (SEM), X‐ray photoelectron spectroscopy (XPS), and ammonia temperature programmed desorption (NH3‐TPD). This work provides a new platform to design and explore multilayered two‐dimensional catalysts demonstrating confinement effect to convert CH4 into *C2H3 intermediates which further oligomerize inside multilayered structures producing C6H6 as the final product.

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Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts

Cited by 24 publications

References 33 publications

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

Boosting the activity of transition metal carbides towards methane activation by nanostructuring

Multilayered Two‐Dimensional V₂CT_x MXene for Methane Dehydroaromatization

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Controlling kinetic and diffusive length-scales during absorptive hydrogen removal in methane dehydroaromatization on MoCx/H-ZSM-5 catalysts

Cited by 24 publications

References 33 publications

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

Single-pass transformation of syngas into ethanol with high selectivity by triple tandem catalysis

Boosting the activity of transition metal carbides towards methane activation by nanostructuring

Multilayered Two‐Dimensional V2CTx MXene for Methane Dehydroaromatization

Contact Info

Product

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Multilayered Two‐Dimensional V₂CT_x MXene for Methane Dehydroaromatization