Abstract
Photothermocatalytic CO2 reduction by CH4 converts greenhouse gases into valuable syngas, but limited by high light intensity and carbon deposition. Here, we designed a nanocomposite supporting low content of Pd nanoparticles on Co and Al doped MgO (Pd/Co-Al1Mg3Ox), achieving high production rates of H2 (rH2, 73.04 mmol min−1 g−1) and CO (rCO, 84.80 mmol min−1 g−1) with light-to-fuel efficiency (η, 25.3 %) at relatively low light intensity (81.1 kW m−2). Compared to Pd/Al1Mg3Ox, Pd/Co-Al1Mg3Ox demonstrates improvements of rH2, rCO and η by 6.5, 6.2 and 6.7 times respectively with great durability of 48 hours. This originates from a synergetic effect between Pd and Co-Al1Mg3Ox that the participation of active oxygen from Co-Al1Mg3Ox greatly accelerates carbon species (C*) oxidation. Interestingly, light plays unique roles on Pd/Co-Al1Mg3Ox which not only expedites C* oxidation, activates the oxygen connected to Pd and Co-Al1Mg3Ox, but also reverses rapid thermocatalytic deactivation by boosting CO desorption.
Published Version
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