Nonoxidative coupling of ethane with gold loaded photocatalysts

Singh, Surya Pratap; Yamamoto, Akira; Yoshida, Hisao

doi:10.1039/d1cy02193a

Cited by 7 publications

(4 citation statements)

References 63 publications

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“…To further investigate the radical mechanism of the PEC process, we tested the PEC oxidation of C 2 H 6 . 34 Fig. 7 shows the time course of the C 2 H 6 activation on the WO 3 photoanode.…”

Section: Resultsmentioning

confidence: 99%

Photoelectrochemical C–H activation of methane to methyl radical at room temperature

Amano

Shintani

Sakakura

et al. 2023

Catal. Sci. Technol.

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“…To further investigate the radical mechanism of the PEC process, we tested the PEC oxidation of C 2 H 6 . 34 Fig. 7 shows the time course of the C 2 H 6 activation on the WO 3 photoanode.…”

Section: Resultsmentioning

confidence: 99%

Photoelectrochemical C–H activation of methane to methyl radical at room temperature

Amano

Shintani

Sakakura

et al. 2023

Catal. Sci. Technol.

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“…The combination of methyl radicals gives ethane molecules while the protons can be removed by superoxide radicals to form water. After the formation of ethane, these molecules can follow similar coupling mechanisms, for example, coupling methane to generate longer-chain hydrocarbons or to form olefin via the side dehydrogenation processes (detailed discussion in Supplementary Note 13) 33 .…”

Section: Articlementioning

confidence: 99%

Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts

Li,

et al. 2023

Nat Energy

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Photocatalytic oxidative coupling of methane (OCM) produces C2 molecules that can be used as building blocks for synthesis of fuels and chemicals. However, the yield rate and the selectivity of C2 products are still moderate due to the stable nature of methane molecules. Here we develop a Au nanocluster-loaded TiO2 photocatalyst by a sputtering approach, achieving a high methane conversion rate of 1.1 mmol h−1, C2 selectivity of ~90% and apparent quantum efficiency of 10.3 ± 0.6%. The high C2/C2+ yield rate is on the same order of magnitude as the benchmark thermal catalysts in OCM processes operated at high temperature (>680 °C). Au nanoparticles are shown to prolong TiO2 photoelectron lifetimes by a factor of 66 for O2 reduction, together with Au acting as a hole acceptor and catalytic centre to promote methane adsorption, C–H activation and C–C coupling. This work underscores the importance of multifunctional co-catalysts and mechanistic understanding to improve photocatalytic OCM.

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“…These requirements call for not only the development of a photocatalyst but also the design of a reactor to control the catalytic conversion process. Several excellent works have been reported using Au/TiO 2 as catalysts to explore the photocatalytic conversion of methane and other alkanes. − Notably, Tang et al recently developed a Au nanocluster-loaded TiO 2 photocatalyst by a sputtering approach, achieving a high methane conversion rate of 1.1 mmol h –1 , C 2 selectivity of ∼90%, and apparent quantum efficiency of 10.3 ± 0.6% . Nevertheless, it is still worth further modulating active oxygen species, revealing the localized surface plasmon resonance (LSPR) effect, and engineering the reactor over this material system, which are expected to open a new avenue for boosting photocatalytic OCM.…”

Section: Introductionmentioning

confidence: 99%

Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane

Chen,

Zhao,

Liu

et al. 2024

J. Am. Chem. Soc.

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Photocatalytic oxidative coupling of methane (OCM) into value-added industrial chemicals offers an appealing green technique for achieving sustainable development, whereas it encounters double bottlenecks in relatively low methane conversion rate and severe overoxidation. Herein, we engineer a continuous gas flow system to achieve efficient photocatalytic OCM while suppressing overoxidation by synergizing the moderate active oxygen species, surface plasmon-mediated polarization, and multipoint gas intake flow reactor. Particularly, a remarkable CH4 conversion rate of 218.2 μmol h–1 with an excellent selectivity of ∼90% toward C2+ hydrocarbons and a remarkable stability over 240 h is achieved over a designed Au/TiO2 photocatalyst in our continuous gas flow system with a homemade three-dimensional (3D) printed flow reactor. This work provides an informative concept to engineer a high-performance flow system for photocatalytic OCM by synergizing the design of the reactor and photocatalyst to synchronously regulate the mass transfer, activation of reactants, and inhibition of overoxidation.

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Nonoxidative coupling of ethane with gold loaded photocatalysts

Abstract: Direct and continuous conversion of ethane to yield n-butane and hydrogen at near room temperature (ca. 320 K) was examined with gold loaded gallium oxide and titanium dioxide photocatalysts without...

Cited by 7 publications

References 63 publications

Photoelectrochemical C–H activation of methane to methyl radical at room temperature

Photoelectrochemical C–H activation of methane to methyl radical at room temperature

Efficient hole abstraction for highly selective oxidative coupling of methane by Au-sputtered TiO2 photocatalysts

Continuous Flow System for Highly Efficient and Durable Photocatalytic Oxidative Coupling of Methane

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