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Lateral-Size-Mediated Efficient Oxygen Evolution Reaction: Insights into the Atomically Thin Quantum Dot Structure of NiFe2O4

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State Key Laboratory of Applied Organic Chemistry (SKLAOC), The Key Laboratory of Catalytic Engineering of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou, Gansu, 730000, P. R. China
State Key Laboratory of Theoretical and Computational Cheistry, Institute of Theoretical Chemistry, Jilin University, Changchun 130023, P. R. China
*J.J. e-mail: [email protected]
*J.M. e-mail: [email protected]
Cite this: ACS Catal. 2017, 7, 8, 5557–5567
Publication Date (Web):July 21, 2017
https://doi.org/10.1021/acscatal.7b00007
Copyright © 2017 American Chemical Society
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Abstract

The study of high-performance electrocatalysts for driving the oxygen evolution reaction (OER) is important for energy storage and conversion systems. As a representative of inverse-spinel-structured oxide catalysts, nickel ferrite (NiFe2O4) has recently gained interest because of its earth abundance and environmental friendliness. However, the gained electrocatalytic performance of NiFe2O4 for the OER is still far from the state-of-the-art requirements because of its poor reactivity and finite number of surface active sites. Here, we prepared a series of atomically thin NiFe2O4 catalysts with different lateral sizes through a mild and controllable method. We found that the atomically thin NiFe2O4 quantum dots (AT NiFe2O4 QDs) show the highest OER performance with a current density of 10 mA cm–2 at a low overpotential of 262 mV and a small Tafel slope of 37 mV decade–1. The outstanding OER performance of AT NiFe2O4 QDs is even comparable to that of commercial RuO2 catalyst, which can be attributed to its high reactivity and the high fraction of active edge sites resulting from the synergetic effect between the atomically thin thickness and the small lateral size of the atomically thin quantum dot (AT QD) structural motif. The experimental results reveal a negative correlation between lateral size and OER performance in alkaline media. Specifically speaking, the number of low-coordinated oxygen atoms increases with decreasing lateral size, and this leads to significantly more oxygen vacancies that can lower the adsorption energy of H2O, increasing the catalytic OER efficiency of AT NiFe2O4 QDs.

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acscatal.7b00007.

  • Details of the estimation of electrochemically active surface area, electrochemical impedance spectroscopy (EIS) analysis, Faradaic efficiency measurements, and DFT calculations; AFM images, XRD spectra, and electrocatalytic mass activity of samples; ICP-OES measured value of the Ni:Fe mole ratio and the geometric values of series resistance (Rs) and charge transfer resistance (Rct) for samples; and comparison of the electrocatalytic performance of AT NiFe2O4 QDs versus OER electrocatalysts reported recently (PDF)

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