Water Splitting with an Enhanced Bifunctional Double Perovskite

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Abstract

The rational design of highly active and durable electrocatalysts for overall water splitting is a formidable challenge. In this work, a double perovskite oxide, i.e., NdBaMn2O5.5, is proposed as a bifunctional electrode material for water electrolysis. Layered NdBaMn2O5.5 demonstrates significant improvement in catalyzing oxygen and hydrogen evolution reactions (OER and HER, respectively), in contrast to other related materials, including disordered Nd0.5Ba0.5MnO3−δ as well as NdBaMn2O5.5−δ and NdBaMn2O5.5+δ (δ < 0.5). Importantly, NdBaMn2O5.5 has an OER intrinsic activity (∼24 times) and a mass activity (∼2.5 times) much higher than those of the benchmark RuO2 at 1.7 V versus the reversible hydrogen electrode. In addition, NdBaMn2O5.5 achieves a better overall water splitting activity at large potentials (>1.75 V) and catalytic durability in comparison to those of Pt/C–RuO2, making it a promising candidate electrode material for water electrolyzers. The substantially enhanced performance is attributed to the approximately half-filled eg orbit occupancy, optimized O p-band center location, and distorted structure. Interestingly, for the investigated perovskite oxides, OER and HER activity seem to be correlated; i.e., the material achieving a higher OER activity is also more active in catalyzing HER.

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