CH 4 conversion to value added products: Potential, limitations and extensions of a single step heterogeneous catalysis

Taifan, William; Baltrušaitis, Jonas

doi:10.1016/j.apcatb.2016.05.081

Cited by 207 publications

(111 citation statements)

References 206 publications

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“…It is important to understand the mechanism of the catalytic partial oxidation reaction to improve the yield of synthesis gas [44,45]. However, the pathways for the reaction are still debated, and the prospect for industrial applications is not yet clear.…”

Section: Introductionmentioning

confidence: 99%

RETRACTED: Computational Fluid Dynamics Modeling of the Catalytic Partial Oxidation of Methane in Microchannel Reactors for Synthesis Gas Production

Chen

Song

2018

Processes

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This paper addresses the issues related to the favorable operating conditions for the small-scale production of synthesis gas from the catalytic partial oxidation of methane over rhodium. Numerical simulations were performed by means of computational fluid dynamics to explore the key factors influencing the yield of synthesis gas. The effect of mixture composition, pressure, preheating temperature, and reactor dimension was evaluated to identify conditions that favor a high yield of synthesis gas. The relative importance of heterogeneous and homogenous reaction pathways in determining the distribution of reaction products was investigated. The results indicated that there is competition between the partial and total oxidation reactions occurring in the system, which is responsible for the distribution of reaction products. The contribution of heterogeneous and homogeneous reaction pathways depends upon process conditions. The temperature and pressure play an important role in determining the fuel conversion and the synthesis gas yield. Undesired homogeneous reactions are favored in large reactors, and at high temperatures and pressures, whereas desired heterogeneous reactions are favored in small reactors, and at low temperatures and pressures. At atmospheric pressure, the selectivity to synthesis gas is higher than 98% at preheating temperatures above 900 K when oxygen is used as the oxidant. At pressures below 1.0 MPa, alteration of the dimension in the range of 0.3 and 1.5 mm does not result in significant difference in reactor performance, if made at constant inlet flow velocities. Air shows great promise as the oxidant, especially at industrially relevant pressure 3.0 MPa, thereby effectively inhibiting the initiation of undesired homogeneous reactions.

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Section: Introductionmentioning

confidence: 99%

RETRACTED: Computational Fluid Dynamics Modeling of the Catalytic Partial Oxidation of Methane in Microchannel Reactors for Synthesis Gas Production

Chen

Song

2018

Processes

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“…1 Accordingly, it is desirable to develop technologies to remove residual CH 4 present from the exhaust of increasingly popular natural gas engines. 2−6 The challenge is to develop highly active catalysts that can operate at the relatively low temperatures of the exhaust gas. The high Pd loading in the current generation of preferred Pd/CeO 2 catalysts poses a cost challenge, requiring a deeper understanding of the nature of the active sites.…”

Section: Introductionmentioning

confidence: 99%

Highly Active and Stable CH₄ Oxidation by Substitution of Ce⁴⁺ by Two Pd²⁺ Ions in CeO₂(111)

et al. 2018

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Methane (CH4) combustion is an increasingly important reaction for environmental protection, for which Pd/CeO2 has emerged as the preferred catalyst. There is a lack of understanding of the nature of the active site in these catalysts. Here, we use density functional theory to understand the role of doping of Pd in the ceria surface for generating sites highly active toward the C–H bonds in CH4. Specifically, we demonstrate that two Pd2+ ions can substitute one Ce4+ ion, resulting in a very stable structure containing a highly coordinated unsaturated Pd cation that can strongly adsorb CH4 and dissociate the first C–H bond with a low energy barrier. An important aspect of the high activity of the stabilized isolated Pd cation is its ability to form a strong σ-complex with CH4, which leads to effective activation of CH4. We show that also other transition metals like Pt, Rh, and Ni can give rise to similar structures with high activity toward C–H bond dissociation. These insights provide us with a novel structural view of solid solutions of transition metals such as Pt, Pd, Ni, and Rh in CeO2, known to exhibit high activity in CH4 combustion.

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“…At present, most methane (>90 %) is directly combusted as fuel, and this utilization of methane, a compound with a higher economic value is a concern . Moreover, the impact of methane, as a greenhouse gas, on global climate change is approximately 21 times greater than that of carbon dioxide . Therefore, the necessity and significance of converting methane into other value‐added chemicals is growing and is increasingly capturing the attention of the academic community …”

Section: Methodsmentioning

confidence: 99%

Efficient and Selective Methane Borylation Through Pore Size Tuning of Hybrid Porous Organic‐Polymer‐Based Iridium Catalysts

et al. 2019

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As an ew energy source that could replace petroleum, the global reserves of methane hydrate (combustible ice) are estimated to be approximately 20 000 trillion cubic meters. Alarge amount of methane hydrate has been found under the seabed, but the transportation and storage of methane gas far from coastlines are technically unfeasible and expensive.T he direct conversion of methane into value-added chemicals and liquid fuels is highly desirable but remains challenging.Herein, we prepare as eries of iridium complexes based on porous polycarbazoles with high specific areas and good thermochemical stabilities.T hrough structure tuning we optimized their catalytic activities for the selective monoborylation of methane.O ne of these catalysts (CAL-3-Ir) can produce methyl boronic acid pinacol ester (CH 3 Bpin) in 29 %y ield in 9hwith aturnover frequency (TOF) of approximately 14 h À1 . Because its pore sizes favor monoborylated products,i th as ah igh chemoselectivity for monoborylation (CH 3 Bpin:CH 2 -(Bpin) 2 = 16:1).

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CH 4 conversion to value added products: Potential, limitations and extensions of a single step heterogeneous catalysis

Cited by 207 publications

References 206 publications

RETRACTED: Computational Fluid Dynamics Modeling of the Catalytic Partial Oxidation of Methane in Microchannel Reactors for Synthesis Gas Production

RETRACTED: Computational Fluid Dynamics Modeling of the Catalytic Partial Oxidation of Methane in Microchannel Reactors for Synthesis Gas Production

Highly Active and Stable CH₄ Oxidation by Substitution of Ce⁴⁺ by Two Pd²⁺ Ions in CeO₂(111)

Efficient and Selective Methane Borylation Through Pore Size Tuning of Hybrid Porous Organic‐Polymer‐Based Iridium Catalysts

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CH 4 conversion to value added products: Potential, limitations and extensions of a single step heterogeneous catalysis

Cited by 207 publications

References 206 publications

RETRACTED: Computational Fluid Dynamics Modeling of the Catalytic Partial Oxidation of Methane in Microchannel Reactors for Synthesis Gas Production

RETRACTED: Computational Fluid Dynamics Modeling of the Catalytic Partial Oxidation of Methane in Microchannel Reactors for Synthesis Gas Production

Highly Active and Stable CH4 Oxidation by Substitution of Ce4+ by Two Pd2+ Ions in CeO2(111)

Efficient and Selective Methane Borylation Through Pore Size Tuning of Hybrid Porous Organic‐Polymer‐Based Iridium Catalysts

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Highly Active and Stable CH₄ Oxidation by Substitution of Ce⁴⁺ by Two Pd²⁺ Ions in CeO₂(111)