Abstract

Efficient electrocatalysts for hydrogen evolution reaction are key to realize clean hydrogen production through water splitting. As an important family of functional materials, transition metal oxides are generally believed inactive towards hydrogen evolution reaction, although many of them show high activity for oxygen evolution reaction. Here we report the remarkable electrocatalytic activity for hydrogen evolution reaction of a layered metal oxide, Ruddlesden−Popper-type Sr2RuO4 with alternative perovskite layer and rock-salt SrO layer, in an alkaline solution, which is comparable to those of the best electrocatalysts ever reported. By theoretical calculations, such excellent activity is attributed mainly to an unusual synergistic effect in the layered structure, whereby the (001) SrO-terminated surface cleaved in rock-salt layer facilitates a barrier-free water dissociation while the active apical oxygen site in perovskite layer promotes favorable hydrogen adsorption and evolution. Moreover, the activity of such layered oxide can be further improved by electrochemistry-induced activation.

Highlights

  • Efficient electrocatalysts for hydrogen evolution reaction are key to realize clean hydrogen production through water splitting

  • Since RuO2 has only modest activity for hydrogen evolution reaction (HER) in the alkaline solution, the electrocatalytic activity of several Ru-based oxides with different crystal structures was characterized to determine the effect of crystal structure on activity

  • All diffraction peaks of the three oxide samples match well with those of the corresponding standard patterns (JCPDS No 71-2273, 89-5713, and 81-1978, respectively), indicating their phase purity without observable impurities. This is confirmed by the Rietveld refinement of the X-ray diffraction (XRD) patterns (Supplementary Fig. 1); the space group is P42/mnm for RuO2, Pnma for SrRuO3, and I4/mmm for Sr2RuO4

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Summary

Introduction

Efficient electrocatalysts for hydrogen evolution reaction are key to realize clean hydrogen production through water splitting. We report the remarkable electrocatalytic activity for hydrogen evolution reaction of a layered metal oxide, Ruddlesden−Popper-type Sr2RuO4 with alternative perovskite layer and rock-salt SrO layer, in an alkaline solution, which is comparable to those of the best electrocatalysts ever reported. By theoretical calculations, such excellent activity is attributed mainly to an unusual synergistic effect in the layered structure, whereby the (001) SrO-terminated surface cleaved in rock-salt layer facilitates a barrier-free water dissociation while the active apical oxygen site in perovskite layer promotes favorable hydrogen adsorption and evolution. As a large and important class of inorganic compounds, transition metal oxides (TMOs) have attracted great interest in many fields (e.g., efficient oxygen evolution reaction (OER)

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