Exploiting H-induced lattice expansion in β-palladium hydride for enhanced catalytic activities toward oxygen reduction reaction

We have developed an efficient strategy to synthesize an active and durable electrocatalyst of Pd hydride nanocubes (NCs). Instead of the traditional chemical method, the PdH 0.43 NCs are firstly prepared via a hydrogen diffusion procedure, followed by hydrothermal synthesis of an amorphous CuO layer encapsulating the PdH 0.43 NCs to prevent the hydrogen atoms from escaping. Obvious lattice expansion is demonstrated playing a pivotal role in the enhancement of their oxygen reduction reaction (ORR) activity and durability. The obtained PdH 0.43 @CuO NCs catalysts exhibit an ORR mass activity of 0.18 A mg −1 at 0.90 V versus reversible hydrogen electrode in an alkaline medium, which is about five times higher than that of commercial Pt/C. Accelerated durability tests show that there is only a 32 mV decay in half-wave potential even after 10,000 potential cycles, indicating the excellent stability of PdH 0.43 @CuO NCs. Density functional theory (DFT) calculations also indicate that, compared to Pd, PdH 0.43 has a lower limiting barrier to form OH − during the ORR process. The present study illustrates the importance of lattice expansion caused by hydrogen and offers an available strategy to design highly efficient and durable Pd-based electrocatalysts for alkaline fuel cells.