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In Situ Formation of Cobalt Nitrides/Graphitic Carbon Composites as Efficient Bifunctional Electrocatalysts for Overall Water Splitting

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Department of Materials Science and Department of Chemistry, Fudan University, Shanghai 200433, China
§ Shanghai Institute of Measurement and Testing Technology, Shanghai 200233, China
Cite this: ACS Appl. Mater. Interfaces 2018, 10, 8, 7134–7144
Publication Date (Web):February 8, 2018
https://doi.org/10.1021/acsami.7b18858
Copyright © 2018 American Chemical Society
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Abstract

Developing cost-effective and highly efficient bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is of great interest for overall water splitting but still remains a challenging issue. Herein, a self-template route is employed to fabricate a unique hybrid composite constructed by encapsulating cobalt nitride (Co5.47N) nanoparticles within three-dimensional (3D) N-doped porous carbon (Co5.47N [email protected]) polyhedra, which can be served as a highly active bifunctional electrocatalyst. To afford a current density of 10 mA cm–2, the as-fabricated Co5.47N [email protected] only requires overpotentials as low as 149 and 248 mV for HER and OER, respectively. Moreover, an electrolyzer with Co5.47N [email protected] electrodes as both the cathode and anode catalyst in alkaline solutions can drive a current density of 10 mA cm–2 at a cell voltage of only 1.62 V, superior to that of the Pt/IrO2 couple. The excellent electrocatalytic activity of Co5.47N [email protected] can be mainly ascribed to the high inherent conductivity and rich nitrogen vacancies of the Co5.47N lattice, the electronic modulation of the N-doped carbon toward Co5.47N, and the hierarchically porous structure design.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsami.7b18858.

  • XRD patterns of the ZIF-67 precursor, nitridated products at 600 and 800 °C; Rietveld refinement for the XRD pattern of the Co5.47N [email protected] composites; FESEM images of the broken Co5.47N [email protected] polyhedron, Co5.47N [email protected] composites after HER/OER processes and nitridated products at 600 and 800 °C; EDS results recorded from the representative Co5.47N [email protected] composite before and after the OER process; comparison of the high-resolution Co XPS spectrum from the Co5.47N [email protected] composites before and after the OER process; TEM image of the Co5.47N [email protected] composites after the OER process; and other electrochemical data including CV curves and LSV curves (PDF)

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