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Unlocking the potential of graphene for water oxidation from orbital hybridization strategy

Abstract

Graphene-based electrocatalytic materials are potential low-cost electrocatalysts for the oxygen evolution reaction (OER). However, substantial overpotentials above thermodynamic requirements limit their efficiency and stability in OER-related energy conversion and storage technologies. Here, we embedded CrN crystals into graphene and in situ electrochemically oxidized them to construct graphene materials with encapsulated Cr6+ ions (Cr6+@G). These Cr6+@G exhibit the lowest OER overpotential of 197 mV at 10 mA cm-2 and excellent stability over 200 h at a high current density of about 120 mA cm-2 in alkaline electrolyte. Spectroscopic and computational studies confirm a stable ion coordination environment and significant downshift of graphene Fermi level via C p orbitals hybridizing with d orbitals of Cr6+ ions that enhance the OER activity and stability.

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Publication details

The article was received on 16 Oct 2017, accepted on 04 Jan 2018 and first published on 04 Jan 2018


Article type: Paper
DOI: 10.1039/C7EE02972A
Citation: Energy Environ. Sci., 2018, Accepted Manuscript
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    Unlocking the potential of graphene for water oxidation from orbital hybridization strategy

    Y. Yao, Z. xu, F. Cheng, W. Li, P. Cui, G. Xu, S. Xu, P. Wang, G. Sheng, Y. Yan, Z.T. Yu, S. C. Yan, Z. Chen and Z. Zou, Energy Environ. Sci., 2018, Accepted Manuscript , DOI: 10.1039/C7EE02972A

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