Solar‐Light‐Driven CO₂ Reduction by CH₄ on Silica‐Cluster‐Modified Ni Nanocrystals with a High Solar‐to‐Fuel Efficiency and Excellent Durability

Abstract

Catalytic CO2 reforming of CH4 (CRM) to produce syngas (H2 and CO) provides a promising approach to reducing global CO2 emissions and the extensive utilization of natural gas resources. However, the rapid deactivation of the reported catalysts due to severe carbon deposition at high reaction temperatures and the large energy consumption of the process hinder its industrial application. Here, a method for almost completely preventing carbon deposition is reported by modifying the surface of Ni nanocrystals with silica clusters. The obtained catalyst exhibits excellent durability for CRM with almost no carbon deposition and deactivation after reaction for 700 h. Very importantly, it is found that CRM on the catalyst can be driven by focused solar light, thus providing a promising new approach to the conversion of renewable solar energy to fuel due to the highly endothermic characteristics of CRM. The reaction yields high production rates of H2 and CO (17.1 and 19.9 mmol min−1 g−1, respectively) with a very high solar‐to‐fuel efficiency (η, 12.5%). Even under focused IR irradiation with a wavelength above 830 nm, the η of the catalyst remains as high as 3.1%. The highly efficient catalytic activity arises from the efficient solar‐light‐driven thermocatalytic CRM enhanced by a novel photoactivation effect.

Selective light absorber-assisted single nickel atom catalysts for ambient sunlight-driven CO2 methanation

“…Converting CO 2 into synthetic natural gas through methanation has great significance for mitigating CO 2 emissions 6,7 and realizing hydrogen storage 8,9 , as the excess electric power generated at night can be used for H 2 production 9–11 . For CO 2 methanation, a temperature of at least 200 °C is needed to activate the catalytic reaction 12,13 , thus requiring a secondary energy source 14,15 . Solar-driven CO 2 methanation via a photothermal effect represents a promising strategy to produce CH 4 without secondary energy input 16–20 .…”

Solar- versus Thermal-Driven Catalysis for Energy Conversion

“…32 Recent developments in solardriven photothermal CH 4 oxidation have allowed the generation of CO 2 and H 2 using composite materials (Ni/SiO 2 and Rh/TiO 2 ). 40,41 Under solar irradiation, the surface temperature of the catalysts can reach up to 400 C-500 C. An H 2 O 2 strategy based on single-atom catalysts permitted CH 4 conversion to CH 3 OH under mild conditions (room temperature and 2 MPa), providing an exciting route to CH 4 conversion. 42 Furthermore, photocatalytic (one sun) conversion of CH 4 to CH 3 OH with a high selectivity of over 90% in alcohols has been reported over FeO x -TiO 2 using H 2 O 2 at room temperature and pressure.…”

Von Sonnenlicht zu Brennstoffen: aktuelle Fortschritte der C1‐Solarchemie

“…[198] Aufd er Grundlage dieser Information entwickelte die Gruppe von Li auf mesoporçsem Siliciumdioxid fixierte,S iliciumdioxidcluster-modifizierte Ni-Nanokristalle (als SCM-Ni/SiO 2 bezeichnet), die die Kohlenstoffabscheidung bei der DRM vollständig unterdrückten und so einen DRM-Katalysator mit ausgezeichneter Aktivitätu nd Beständigkeit ergaben. [199] Anschließend beschrieb die Arbeitsgruppe wirkungsvolle DRM in einem kontinuierlichen Durchflussreaktor unter Sonnenlichtbestrahlung [199] mit sehr hohen Produktionsraten von H 2 (17.1 mmol min À1 g À1 )u nd CO (19.9 mmol min À1 g À1 ). Der Sonnenlicht-zu-Brennstoff-Wirkungsgrad des SCM-Ni/SiO 2 -Katalysators erreichte einen hohen Wert von 12.5 %.…”