Understanding the contribution of crystal facets to the adsorption/desorption behavior of catalytic reaction intermediates is crucial for the design of high-performance electrocatalysts. In this work, we designed a synthesis strategy for ultrathin PdP nanosheets enclosed by different low-index facets, for example, {100}, {110}, and {111}, and studied their performance for electrocatalytic ethanol oxidation reaction (EOR). The results showed that the mass activity of the PdP nanosheets enclosed by the {100} facet was 4.07 A/mg, which was 1.43, 2.56, and 5.58 times as high as that of the PdP {110}, PdP {111}, and commercial Pd/C, respectively. Additionally, the PdP {100} displayed the best stability and the lowest activation energy (E a), which further proved that the atomic configuration on the crystallographic {100} facet was greatly beneficial for EOR. The universality of this synthesis strategy was shown by producing nanocrystals with various amounts of P doping and elemental compositions (e.g., {100}-exposed PdAgP, PdAuP, PdCuP, and PdPtP).

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