Research Article

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2018, 11(4): 1883–1894

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https://doi.org/10.1007/s12274-017-1806-x

Fast formation of single-unit-cell-thick and defect-rich layered double hydroxide nanosheets with highly enhanced oxygen evolution reaction for water splitting

Rui Gao1 and Dongpeng Yan1,2 (*)

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1 State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
2 Beijing Key Laboratory of Energy Conversion and Storage Materials, College of Chemistry, Beijing Normal University, Beijing 100875, China

Keywords: single-unit-cell, defect-rich, oxygen evolution reaction, water splitting
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ABSTRACT The development of high-efficiency electrocatalysts for oxygen evolution reactions (OERs) plays an important role in the water-splitting process. Herein, we report a facile way to obtain two-dimensional (2D) single-unit-cell-thick layered double hydroxide (LDH) nanosheets (NSs, ~1.3 nm) within only 5 min. These nanosheets presented significantly enhanced OER performance compared to bulk LDH systems fabricated using the conventional co-precipitation method. The current strategy further allowed control over the chemical compositions and electrochemical activities of the LDH NSs. For example, CoFe-LDH NSs presented the lowest overpotential of 0.28 V at 10 mA/cm2, and the NiFe-LDHs NSs showed Tafel slopes of 33.4 mV/decade and nearly 100% faradaic efficiency, thus outperforming state-of-the-art IrO2 water electrolysis catalysts. Moreover, positron annihilation lifetime spectroscopy and high-resolution transmission electron microscopy observations confirmed that rich defects and distorted lattices occurred within the 2D LDH NSs, which could supply abundant electrochemically active OER sites. Periodic calculations based on density functional theory (DFT) further showed that the CoFe- and NiFe-LDHs presented very low energy gaps and obvious spin-polarization behavior, which facilitated high electron mobility during the OER process. Therefore, this work presents a combined experimental and theoretical study on 2D single-unit-cell-thick LDH NSs with high OER activities, which have potential application in water splitting for renewable energy
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Fast formation of single-unit-cell-thick and defect-rich layered double hydroxide nanosheets with highly enhanced oxygen evolution reaction for water splitting. Nano Res. 2018, 11(4): 1883–1894 https://doi.org/10.1007/s12274-017-1806-x

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