2021
DOI: 10.1021/acscatal.1c02597
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Theoretical Insights into Dual-Metal-Site Catalysts for the Nonoxidative Coupling of Methane

Abstract: Direct conversion of methane to C2 hydrocarbons under nonoxidative conditions is an attractive technology but is challenging due to high reaction temperature, severe coke deposition, and low selectivity. Here, we report three dual-metal-site catalysts (DMSCs) based on nitrogen-doped graphene (FeCo–N–C, Fe2–N–C, and Co2–N–C) for nonoxidative coupling of methane to C2 hydrocarbons from a theoretical perspective. Our calculated results reveal that DMSCs present universally better performance in methane activation… Show more

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Cited by 18 publications
(20 citation statements)
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References 58 publications
(89 reference statements)
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“…It is possible to observe from Figure 2a that the adsorption of methane is an exothermic process for all the decorated EDNCs considered in this study, leading to more thermodynamically stable products when CH 3 and H are chemisorbed on different edge sites. It is noteworthy that the CH 4 adsorption was reported to be endothermic on doped metal sites on graphene 11,56 and bimetallic catalysts 55,57 in previous works. A large energetic difference was found between the two adsorption configurations of CH 3 and H on N-EDNC and B-EDNC.…”
Section: Activation Of Ch 4 On Edncsmentioning
confidence: 86%
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“…It is possible to observe from Figure 2a that the adsorption of methane is an exothermic process for all the decorated EDNCs considered in this study, leading to more thermodynamically stable products when CH 3 and H are chemisorbed on different edge sites. It is noteworthy that the CH 4 adsorption was reported to be endothermic on doped metal sites on graphene 11,56 and bimetallic catalysts 55,57 in previous works. A large energetic difference was found between the two adsorption configurations of CH 3 and H on N-EDNC and B-EDNC.…”
Section: Activation Of Ch 4 On Edncsmentioning
confidence: 86%
“…4,10 This process generally requires high temperatures to overcome the kinetic barrier for methane cracking and hydrogen desorption, which can result in the severe deactivation of the catalyst due to coking, thus being a major drawback of metal-based catalysts. 1,9,11,12 Therefore, significant effort has been made toward the design of efficient catalysts that are expected to improve the selectivity activation of C−H bonds, while being resistant to carbon poisoning. 13−16 Much attention has been directed to the improvement of the process of catalytic methane decomposition (CMD) into hydrogen H 2 production in the past decade.…”
Section: Introductionmentioning
confidence: 99%
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“…In addition, using microkinetic analysis, Huang et al have revealed that the NGr-supported Fe−Co, Fe−Fe, and Co−Co DMSCs are all good catalysts for the nonoxidative coupling of methane, and the homonuclear Co−Co DMSC exhibits better stability and superior activity than the others. 24 Mechanistic exploration using density functional theory (DFT) simulations by Wang et al determined that the Fe−Co dual-site structure can result in an energetically preferential side-on adsorption reactant configuration. 25 This special structure preactivates the bond on the bridge site, reducing the oxygen reduction barrier.…”
Section: Introductionmentioning
confidence: 99%
“…In this regard, a variety of metal combinations including Fe–Co, Fe–Cu, Ni–Cu, Co–Pt, and Co–Zn on NGr have been investigated theoretically and been identified as good candidates for heterogeneous catalysts. In addition, using microkinetic analysis, Huang et al have revealed that the NGr-supported Fe–Co, Fe–Fe, and Co–Co DMSCs are all good catalysts for the nonoxidative coupling of methane, and the homonuclear Co–Co DMSC exhibits better stability and superior activity than the others …”
Section: Introductionmentioning
confidence: 99%