Abstract
Rh is recently regarded as the promising electrocatalyst for ethanol oxidation into CO2 due to its high activity of splitting C–C bond, whereas the further oxidation of as-generated C1 species (CO and CHx) is pretty sluggish at Rh surface. To solve this, here the oxophile Pb skin-layer is inhabited at Rh nanoparticles to obtain the Pb@Rh core-shell structure with controllable Pb coverage (θPb), expecting to tune the surface reactivity of ethanol oxidation reaction (EOR) according to the Langmuir-Hinshelwood Mechanism as well as the strain effect. Fortunately, the as-obtained Pb@Rh/C catalysts indeed significantly enhance the catalysis performance of EOR, the optimal mass activity is ca. 1450 mA mg-1 metal when θPb is ca. 0.53 (Pb0.53@Rh), being ca. 13 times higher than pristine Rh catalyst. Meanwhile, as much as ca. 57% of the initial EOR current remains even after a 20,000-s durability measurement. And the apparent C1 pathway faraday efficiency (CO2 selectivity) is also estimated to be ca. 21% at Pb0.53@Rh surface. This work can provide a simple and promising protocol to tune the surface reactivity by interfacial engineering manipulation.
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