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Reductive Electropolymerization of a Vinyl-containing Poly-pyridyl Complex on Glassy Carbon and Fluorine-doped Tin Oxide Electrodes
Published on: January 30, 2015
Ruthenium-molybdenum nanoparticles with multi-valence ruthenium species to drive redox electrocatalysis at high
Shuanglong Zhou1, Liang Zhao2, Yuanduo Li2
1Key Laboratory of Eco-chemical Engineering, Ministry of Education, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China; College of Chemistry and Chemical Engineering, Qilu Normal University, Jinan 250200, PR China.
Abstract:
Coupling furfural electrochemical hydrogenation (FEH) with hydrazine oxidation (HzOR) in an electrochemical process offers an effective pathway to obtain high-value products, while simultaneously addressing hydrazine contamination and lowering overall energy consumption. Although Ru has been recognized as an effective bifunctional catalyst toward both FEH and HzOR, challenges remain in achieving large current densities and fully clarifying the underlying activity and mechanism. In this work, a Ru-based device was engineered by introducing Mo dopants to regulate the proportion of Ru0 and Ru4+ species, which enabled a remarkable current density of 500 mA cm-2 at 0.31 V. Combined experimental and theoretical investigations demonstrate that Ru0 sites enhance water dissociation to generate active hydrogen for subsequent hydrogenation, while Ru4+ sites stabilize the (C4H3O)CH2O* intermediate during FEH. For HzOR, Ru4+ lowers the barrier of the rate-determining step, thus accelerating the overall process, whereas Ru0 facilitates dehydrogenation and the release of N2. Notably, the integrated FEH-HzOR system dramatically reduces the electricity demand for converting furfural to furfuryl alcohol, requiring only 32,711 kWh per ton of FA, which corresponds to a 69.5 % energy saving compared with conventional FEH (97,766 kWh per ton).
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