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Synergistic Effect of Atomically Dual-metal Doped Catalyst for Highly Efficient Oxygen Evolution


The oxygen evolution reaction (OER) involving multi-step electron transfer is a challenging in water-splitting due to its sluggish kinetics. It is desirable to explore more efficient electro-catalysts with abundant elements. Herein, we employed a high-temperature polymerization method to develop a structure of graphitic carbon nitride (g-C3N4) nanopatches enveloped carbon nanotube (CNT), where the isolated Ni and Fe atoms were embedded into the tri-s-triazine units of g-C3N4 by forming metal-Nx structure. The designed dual-metal catalyst exhibited a remarkable OER performance with an extremely low overpotential (~326 mV at 10 mA cm-2) and a small Tafel slope (67 mV decade-1), which is superior to those of the state-of-the-art electrocatalysts with metal-Nx coordination and the benchmark IrO2/C catalyst. In combiniation with atomic microscope 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, the increase of oxidative state in Ni sites after multi-metal doping directly contributed to more active sites and favored the OER process, assisting by porous structure and good electrical contacts between CNT and g-C3N4. This investigation clearly demonstrated a unique synergistic effect in atomically dual-metal doped catalyst, thus may provide a versatile route to regulate the electronic strusture of single atomic catalysts through engineering of neighboring element and coordination number.

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Publication details

The article was received on 17 Jan 2018, accepted on 13 Mar 2018 and first published on 14 Mar 2018

Article type: Paper
DOI: 10.1039/C8TA00550H
Citation: J. Mater. Chem. A, 2018, Accepted Manuscript
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    Synergistic Effect of 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, Accepted Manuscript , DOI: 10.1039/C8TA00550H

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