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Abstract
The preparation of Ru nanoparticles supported on γ-Al2O3 followed by chemical reduction using RuCl3 as a precursor is demonstrated, and their properties are compared to Ru nanoparticles supported on γ-Al2O3 prepared by impregnation of γ-Al2O3 with Ru3(CO)12 and subsequent thermal decomposition. The Ru nanoparticles resulting from chemical reduction of RuCl3 are slightly larger (1.2 vs. 0.8 nm). In addition, Ru nanoparticles were deposited on Stöber SiO2 using both deposition techniques. These particles were larger than the ones deposited on γ-Al2O3 (2.5 and 3.4 nm for chemical reduction and thermal decomposition, respectively). Taking into account the size differences between the Ru nanoparticles, all catalysts display similar activity (0.14–0.63 mol·gRu−1·h−1) and selectivity (≥99%) in the sunlight-powered Sabatier reaction. Ergo, the use of toxic and volatile Ru3(CO)12 can be avoided, since catalysts prepared by chemical reduction of RuCl3 display similar catalytic performance.
Highlights
IntroductionWe are currently facing two major challenges: reducing CO2 emissions and the replacement of fossil fuels with green and sustainable energy sources and carriers
Catalysts comprising metal nanoparticles with a plasmonic resonance in the UVvis-NIR region are of interest for sunlight-powered reactions [6]. Based on their localized surface plasmon resonance (LSPR), light illumination induces a resonant response of free electrons in metallic nanoparticles [7,8]
Two different methods were used for decoration of the supports, viz. γ-Al2O3 and Stöber SiO2, with Ru nanoparticles: (1) deposition-precipitation followed by chemical reduction using RuCl3 as a precursor (CR), and (2) impregnation with Ru3(CO)12 and subsequent high-temperature decomposition (TD)
Summary
We are currently facing two major challenges: reducing CO2 emissions and the replacement of fossil fuels with green and sustainable energy sources and carriers. Ni promotes CH4 formation with a selectivity close to 100% [2–4] These and other supported metal catalysts for the Sabatier reaction, such as Ru and Rh, require thermal activation at temperatures between 300 and 500 ◦C [5]. Catalysts comprising metal nanoparticles with a plasmonic resonance in the UVvis-NIR region are of interest for sunlight-powered reactions [6]. Based on their localized surface plasmon resonance (LSPR), light illumination induces a resonant response of free electrons in metallic nanoparticles [7,8]. This coherent oscillation dephases non-radiatively and generates hot electrons. The LSPR of metallic nanoparticles can be tuned by varying the type of metal, size, shape and architecture of the particle, which makes this concept interesting for visible light and sunlight catalysis [9]
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