Nonoxidative Coupling of Methane over Ceria-Supported Single-Atom Pt Catalysts in DBD Plasma

Liu, Lina; Das, Sonali; Zhang, Zhikun; Kawi, Sibudjing

doi:10.1021/acsami.1c21550

Cited by 42 publications

(23 citation statements)

References 69 publications

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“…In addition, hydrogen is coproduced as a valuable byproduct. 24 The above points provide support for NOCM being more attractive than OCM in many cases. because no oxidant is used, the activation energy for methane conversion becomes high compared to that in OCM, and the reaction is thermodynamically unfavorable.…”

Section: Introductionmentioning

confidence: 74%

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Oxidative Addition of Methane and Reductive Elimination of Ethane and Hydrogen on Surfaces: From Pure Metals to Single Atom Alloys

et al. 2022

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Oxidative addition of CH4 to the catalyst surface produces CH3 and H. If the CH3 species generated on the surface couple with each other, reductive elimination of C2H6 may be achieved. Similarly, H’s could couple to form H2. This is the outline of nonoxidative coupling of methane (NOCM). It is difficult to achieve this reaction on a typical Pt catalyst surface. This is because methane is overoxidized and coking occurs. In this study, the authors approach this problem from a molecular aspect, relying on organometallic or complex chemistry concepts. Diagrams obtained by extending the concepts of the Walsh diagram to surface reactions are used extensively. C–H bond activation, i.e., oxidative addition, and C–C and H–H bond formation, i.e., reductive elimination, on metal catalyst surfaces are thoroughly discussed from the point of view of orbital theory. The density functional theory method for structural optimization and accurate energy calculations and the extended Hückel method for detailed analysis of crystal orbital changes and interactions play complementary roles. Limitations of monometallic catalysts are noted. Therefore, a rational design of single atom alloy (SAA) catalysts is attempted. As a result, the effectiveness of the Pt1/Au(111) SAA catalyst for NOCM is theoretically proposed. On such an SAA surface, one would expect to find a single Pt monatomic site in a sea of inert Au atoms. This is desirable for both inhibiting overoxidation and promoting reductive elimination.

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Section: Introductionmentioning

confidence: 74%

“…NOCM was first reported in 1991, and since then its study has been active worldwide. ,, In NOCM, no oxidants are used, and production of undesirable CO x species does not occur. In addition, hydrogen is coproduced as a valuable byproduct . The above points provide support for NOCM being more attractive than OCM in many cases.…”

Section: Introductionmentioning

confidence: 76%

Oxidative Addition of Methane and Reductive Elimination of Ethane and Hydrogen on Surfaces: From Pure Metals to Single Atom Alloys

et al. 2022

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“…Pt-based catalysts also exhibit excellent catalytic activity and coking resistance in PAMD systems. For example, Liu et al [236] reported the plasma-catalytic direct nonoxidative coupling of CH 4 into C 2 hydrocarbons over ceria-supported atomically dispersed Pt (Pt/CeO 2 -SAC) catalysts in DBD plasma. The Pt/CeO 2 -SAC coupled DBD plasma can achieve CH 4 conversion of 39% and C 2 selectivity of 54%, and the outstanding activity is attributed to abundant coordinatively unsaturated Pt sites in catalyst, which were more active for C-H bond cleavage.…”

Section: Hydrocarbon Products Production Via Pamd Systemmentioning

confidence: 99%

Plasma‐Assisted Reforming of Methane

Feng

Sun

et al. 2022

Advanced Science

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Methane (CH4) is inexpensive, high in heating value, relatively low in carbon footprint compared to coal, and thus a promising energy resource. However, the locations of natural gas production sites are typically far from industrial areas. Therefore, transportation is needed, which could considerably increase the sale price of natural gas. Thus, the development of distributed, clean, affordable processes for the efficient conversion of CH4 has increasingly attracted people's attention. Among them are plasma technology with the advantages of mild operating conditions, low space need, and quick generation of energetic and chemically active species, which allows the reaction to occur far from the thermodynamic equilibrium and at a reasonable cost. Significant progress in plasma‐assisted reforming of methane (PARM) is achieved and reviewed in this paper from the perspectives of reactor development, thermal and nonthermal PARM routes, and catalysis. The factors affecting the conversion of reactants and the selectivity of products are studied. The findings from the past works and the insight into the existing challenges in this work should benefit the further development of reactors, high‐performance catalysts, and PARM routes.

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“…Furthermore, we also found that the metal size and dispersion of catalysts played a high priority role in accelerating the conversion of CH 4 and CO 2 in DBD plasma. 9 , 15 , 16 Therefore, more attention should be paid to the low-temperature characteristics of catalysts in plasma reactions. Layered double hydroxides (LDHs), also known as hydrotalcites, with a general formula of [M 1– x 2+ M x 3+ (OH) 2 ] x + [A x / n ] n − · m H 2 O, are a family of two-dimensional nanostructured anionic clays comprising of brucite-like layers.…”

Section: Introductionmentioning

confidence: 99%

Plasma-Catalytic CO₂ Reforming of Toluene over Hydrotalcite-Derived NiFe/(Mg, Al)O_x Catalysts

Liu

Dai

Das

et al. 2023

JACS Au

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The removal of tar and CO2 in syngas from biomass gasification is crucial for the upgrading and utilization of syngas. CO2 reforming of tar (CRT) is a potential solution which simultaneously converts the undesirable tar and CO2 to syngas. In this study, a hybrid dielectric barrier discharge (DBD) plasma-catalytic system was developed for the CO2 reforming of toluene, a model tar compound, at a low temperature (∼200 °C) and ambient pressure. Periclase-phase (Mg, Al)O x nanosheet-supported NiFe alloy catalysts with various Ni/Fe ratios were synthesized from ultrathin Ni–Fe–Mg–Al hydrotalcite precursors and employed in the plasma-catalytic CRT reaction. The result demonstrated that the plasma-catalytic system is promising in promoting the low-temperature CRT reaction by generating synergy between DBD plasma and the catalyst. Among the various catalysts, Ni4Fe1-R exhibited superior activity and stability because of its highest specific surface area, which not only provided sufficient active sites for the adsorption of reactants and intermediates but also enhanced the electric field in the plasma. Furthermore, the stronger lattice distortion of Ni4Fe1-R provided more isolated O2– for CO2 adsorption, and having the most intensive interaction between Ni and Fe in Ni4Fe1-R restrained the catalyst deactivation induced by the segregation of Fe from the alloy to form FeO x . Finally, in situ Fourier transform infrared spectroscopy combined with comprehensive catalyst characterization was used to elucidate the reaction mechanism of the plasma-catalytic CRT reaction and gain new insights into the plasma-catalyst interfacial effect.

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Nonoxidative Coupling of Methane over Ceria-Supported Single-Atom Pt Catalysts in DBD Plasma

Cited by 42 publications

References 69 publications

Oxidative Addition of Methane and Reductive Elimination of Ethane and Hydrogen on Surfaces: From Pure Metals to Single Atom Alloys

Oxidative Addition of Methane and Reductive Elimination of Ethane and Hydrogen on Surfaces: From Pure Metals to Single Atom Alloys

Plasma‐Assisted Reforming of Methane

Plasma-Catalytic CO₂ Reforming of Toluene over Hydrotalcite-Derived NiFe/(Mg, Al)O_x Catalysts

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Nonoxidative Coupling of Methane over Ceria-Supported Single-Atom Pt Catalysts in DBD Plasma

Cited by 42 publications

References 69 publications

Oxidative Addition of Methane and Reductive Elimination of Ethane and Hydrogen on Surfaces: From Pure Metals to Single Atom Alloys

Oxidative Addition of Methane and Reductive Elimination of Ethane and Hydrogen on Surfaces: From Pure Metals to Single Atom Alloys

Plasma‐Assisted Reforming of Methane

Plasma-Catalytic CO2 Reforming of Toluene over Hydrotalcite-Derived NiFe/(Mg, Al)Ox Catalysts

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Resources

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Plasma-Catalytic CO₂ Reforming of Toluene over Hydrotalcite-Derived NiFe/(Mg, Al)O_x Catalysts