Abstract

Developing efficient bifunctional catalysts for overall water splitting that are earth-abundant, cost-effective, and durable is of considerable importance from the practical perspective to mitigate the issues associated with precious metal-based catalysts. Herein, we introduce a heterostructure comprising perovskite oxides (La0.5Sr0.5CoO3–δ) and molybdenum diselenide (MoSe2) as an electrochemical catalyst for overall water electrolysis. Interestingly, formation of the heterostructure of La0.5Sr0.5CoO3–δ and MoSe2 induces a local phase transition in MoSe2, 2 H to 1 T phase, and more electrophilic La0.5Sr0.5CoO3–δ with partial oxidation of the Co cation owing to electron transfer from Co to Mo. Together with these synergistic effects, the electrochemical activities are significantly improved for both hydrogen and oxygen evolution reactions. In the overall water splitting operation, the heterostructure showed excellent stability at the high current density of 100 mA cm−2 over 1,000 h, which is exceptionally better than the stability of the state-of-the-art platinum and iridium oxide couple.

Highlights

  • Developing efficient bifunctional catalysts for overall water splitting that are earth-abundant, cost-effective, and durable is of considerable importance from the practical perspective to mitigate the issues associated with precious metal-based catalysts

  • LSC&MoSe2 was prepared using the high-energy ball milling process with the optimum weight ratio of LSC:MoSe2:Ketjen black EC-600JD (KB) = 6:3:1 determined by the electrochemical analyses (Supplementary Figure 1–3; see Experimental Section for details)

  • Morphological and structural analyses of the composite electrocatalyst were first performed by transmission electron microscopy (TEM) and scanning electron microscopy (SEM)

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Summary

Introduction

Developing efficient bifunctional catalysts for overall water splitting that are earth-abundant, cost-effective, and durable is of considerable importance from the practical perspective to mitigate the issues associated with precious metal-based catalysts. ABO3 perovskite oxides (A: rare-earth or alkaline earth element, B: transition metal ion) have received significant attention as potential alternatives to precious metal-based catalysts (e.g., RuO2 and IrO2) owing to their strong catalytic activity, robust stability, and compositional flexibility[8,9]. Grimaud et al demonstrated that the O2 generated from the lattice oxygen of La1–xSrxCoO3–δ significantly influenced OER13 Both theoretical and experimental investigations on transition metal dichalcogenides (TMDs) have revealed the great potential of TMDs as hydrogen generation catalysts owing to their high catalytic activity; robustness to CO, CO2, and O2; affordability; and scalability[14,15]. MoSe2, MoSe2-based composite structures, such as MoSe2/carbon cloth[16], MoSe2/n+p-Si18, and MoSe2/graphene[19], have been typically used to improve the electrochemical activity of intrinsic

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