Photothermal steam reforming of methane over silica-supported nickel catalysts with temperature gradients

Sarwana, Wirya; Takami, Daichi; Yamamoto, Akira; Yoshida, Hisao

doi:10.1039/d2cy01721k

Cited by 4 publications

(2 citation statements)

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“…CO 2 conversion to CO (Eq. 1 ) is an endothermic reaction with an Δ Η o = 41 kJ/mol 47 (equivalent to a temperature of 4930 K or 0.425 eV). The temperature is significantly higher than one can generate at the plasmon surface 48 .…”

Section: Resultsmentioning

confidence: 99%

Exploiting hot electrons from a plasmon nanohybrid system for the photoelectroreduction of CO2

Dey,

Silveira,

Vadell

et al. 2024

Commun Chem

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Plasmonic materials convert light into hot carriers and heat to mediate catalytic transformation. The participation of hot carriers (photocatalysis) remains a subject of vigorous debate, often argued on the basis that carriers have ultrashort lifetime incompatible with drive photochemical processes. This study utilises plasmon hot electrons directly in the photoelectrocatalytic reduction of CO2 to CO via a Ppasmonic nanohybrid. Through the deliberate construction of a plasmonic nanohybrid system comprising NiO/Au/ReI(phen-NH2)(CO)3Cl (phen-NH2 = 1,10-Phenanthrolin-5-amine) that is unstable above 580 K; it was possible to demonstrate hot electrons are the main culprit in CO2 reduction. The engagement of hot electrons in the catalytic process is derived from many approaches that cover the processes in real-time, from ultrafast charge generation and separation to catalysis occurring on the minute scale. Unbiased in situ FTIR spectroscopy confirmed the stepwise reduction of the catalytic system. This, coupled with the low thermal stability of the ReI(phen-NH2)(CO)3Cl complex, explicitly establishes plasmonic hot carriers as the primary contributors to the process. Therefore, mediating catalytic reactions by plasmon hot carriers is feasible and holds promise for further exploration. Plasmonic nanohybrid systems can leverage plasmon’s unique photophysics and capabilities because they expedite the carrier’s lifetime.

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Section: Resultsmentioning

confidence: 99%

Exploiting hot electrons from a plasmon nanohybrid system for the photoelectroreduction of CO2

Dey,

Silveira,

Vadell

et al. 2024

Commun Chem

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“…Moreover, the formation rates of CO and H 2 linearly increased with the weight hourly space velocity increasing (Figure S9). These results imply that the catalytic activity depends on the thermodynamic equilibrium, although it is difficult to evaluate the thermodynamic equilibrium due to the temperature gradient in the catalysts under light irradiation. − Photothermal catalytic activity is believed to depend on both the number of active sites in the catalyst and the resulting temperature under reaction conditions. However, the latter contribution is expected to be larger under the experimental conditions in this study.…”

Section: Resultsmentioning

confidence: 99%

Photothermal Dry Reforming of Methane over Phyllosilicate-Derived Silica-Supported Nickel Catalysts

Takami,

Tsubakimoto,

Sarwana

et al. 2023

ACS Appl. Energy Mater.

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The development of catalytic technology for CO 2 recycling attracts much international attention for producing valuable chemicals and reducing CO 2 emissions. Photothermal dry reforming of methane (PT-DRM) is a promising technology to convert CO 2 into syngas (a mixture of CO and H 2 ) using solar energy. In this study, we found that silica-supported nickel catalysts (Ni/SiO 2 ) prepared via Ni phyllosilicate by the ammonia evaporation methods exhibited improved catalytic activity and enhanced resistance to sintering and carbon deposition in PT-DRM under visible and near-infrared light compared to that prepared by the conventional wetness impregnation method due to the highly dispersed Ni nanoparticles coated with thin SiO 2 layers. The catalytic activity and surface temperature reached maximums at the Ni loading of around 25 wt %. Furthermore, the light absorption and thermal diffusivity of the catalyst material increased with the increase in Ni loading, where the former contributes to the increase of the surface temperature and the latter to the decrease due to the higher heat dissipation. Hence, the Ni loading had positive and negative effects on the irradiated surface temperature of the catalytic part, and these thermal properties affected the photothermal catalytic activity for PT-DRM. These findings indicate the significance of suppressing heat dissipation in the design of photothermal catalysts for effective light energy utilization.

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Photothermal Dry Reforming of Methane on Yolk‐Shell Co–Ni Alloy@SiO₂ Catalyst

El‐Naggar,

Takami,

Asanuma

et al. 2024

ChemCatChem

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Photothermal dry reforming of methane (PT‐DRM) is an appealing pathway to convert carbon dioxide and methane into synthesis gas, a mixture of carbon monoxide and hydrogen, via photothermal heating induced by concentrated sunlight. Coke formation and sintering of active metal nanoparticles, however, are a key issue for catalyst stability. In the present study, we demonstrated Co–Ni alloy nanoparticles encapsulated with a porous SiO2 shell exhibited improved catalytic activity and stability for PT‐DRM using visible/near‐IR light irradiation without any other external heating. The addition of a trace amount of Co (1–5 mol% relative to total metal) and SiO2 encapsulation enhanced the stability by simultaneously suppressing coke formation and sintering of the metal nanoparticles. Furthermore, we revealed that the position of the light irradiation spot has a crucial role in the conversions of methane and carbon dioxide and product selectivity, presumably due to large temperature gradient under the light irradiation. These findings would contribute to designing for effective PT‐DRM catalysts with improved activity and enhanced resistance for both coke formation and sintering and emphasize the significant contribution of the temperature gradients to the performance in PT‐DRM.

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Photothermal steam reforming of methane over silica-supported nickel catalysts with temperature gradients

Abstract: Photothermal steam reforming of methane (PTSRM) is a promising catalytic technology for converting stable methane and water into hydrogen utilizing solar energy. In the present study, the photothermal catalytic activity...

Cited by 4 publications

References 61 publications

Exploiting hot electrons from a plasmon nanohybrid system for the photoelectroreduction of CO2

Exploiting hot electrons from a plasmon nanohybrid system for the photoelectroreduction of CO2

Photothermal Dry Reforming of Methane over Phyllosilicate-Derived Silica-Supported Nickel Catalysts

Photothermal Dry Reforming of Methane on Yolk‐Shell Co–Ni Alloy@SiO₂ Catalyst

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Photothermal steam reforming of methane over silica-supported nickel catalysts with temperature gradients

Abstract: Photothermal steam reforming of methane (PTSRM) is a promising catalytic technology for converting stable methane and water into hydrogen utilizing solar energy. In the present study, the photothermal catalytic activity...

Cited by 4 publications

References 61 publications

Exploiting hot electrons from a plasmon nanohybrid system for the photoelectroreduction of CO2

Exploiting hot electrons from a plasmon nanohybrid system for the photoelectroreduction of CO2

Photothermal Dry Reforming of Methane over Phyllosilicate-Derived Silica-Supported Nickel Catalysts

Photothermal Dry Reforming of Methane on Yolk‐Shell Co–Ni Alloy@SiO2 Catalyst

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Photothermal Dry Reforming of Methane on Yolk‐Shell Co–Ni Alloy@SiO₂ Catalyst