Issue 16, 2018

Synergistic effect of an atomically dual-metal doped catalyst for highly efficient oxygen evolution

Abstract

The oxygen evolution reaction (OER) involving multi-step electron transfer is a challenging approach for water-splitting due to its sluggish kinetics. It is desirable to explore more efficient electro-catalysts with earth-abundant elements. Herein, we employed a high-temperature polymerization method to develop a structure consisting of graphitic carbon nitride (g-C3N4) nanopatch enveloped carbon nanotubes (CNTs), where isolated Ni and Fe atoms were embedded into the tri-s-triazine units of g-C3N4 by forming a metal–Nx structure. The designed dual-metal catalyst exhibited remarkable OER performance with an extremely low overpotential (∼326 mV at 10 mA cm−2) and a small Tafel slope (67 mV per decade), which is superior to those of state-of-the-art electrocatalysts with metal–Nx coordination and the benchmark IrO2/C catalyst. In combination with atomic microscopy observations, our synchrotron-based X-ray absorption spectroscopy results revealed that, as compared to single-metal (Fe or Ni) doped hybrids, the electronic structures of both Ni and Fe atoms were reconfigured in the obtained dual-metal samples. Notably, increase of the oxidative state in Ni sites after multi-metal doping directly contributed to more active sites and favored the OER process, assisted by the porous structure and good electrical contacts between CNTs and g-C3N4. This investigation clearly demonstrated a unique synergistic effect in atomically dual-metal doped catalysts, thus it may provide a versatile route to regulate the electronic structures of single atomic catalysts through engineering of neighboring elements and coordination number.

Graphical abstract: Synergistic effect of an atomically dual-metal doped catalyst for highly efficient oxygen evolution

Supplementary files

Article information

Article type
Paper
Submitted
17 1 2018
Accepted
13 3 2018
First published
14 3 2018

J. Mater. Chem. A, 2018,6, 6840-6846

Synergistic effect of an atomically dual-metal doped catalyst for highly efficient oxygen evolution

D. Liu, S. Ding, C. Wu, W. Gan, C. Wang, D. Cao, Z. U. Rehman, Y. Sang, S. Chen, X. Zheng, Y. Wang, B. Ge and L. Song, J. Mater. Chem. A, 2018, 6, 6840 DOI: 10.1039/C8TA00550H

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