4.8 Article

Atomically Dispersed Silver Atoms Embedded in NiCo Layer Double Hydroxide Boost Oxygen Evolution Reaction

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WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202301610

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density functional theory calculations; NiCo layered double hydroxide; oxygen evolution reaction; silver; single-atom

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A novel NiCo LDH electrocatalyst modified with single-atom silver on carbon cloth (Ag-SA-NiCo LDH/CC) is reported to exhibit exceptional OER activity and stability in 1.0 m KOH. The Ag-SA-NiCo LDH/CC catalyst shows a low overpotential of 192 mV to reach a current density of 10 mA cm(-2), significantly improving the OER activity of NiCo LDH/CC (410 mV@10 mA cm(-2)). Moreover, Ag-SA-NiCo LDH/CC can maintain its high activity for up to 500 h at a large current density of 100 mA cm(-2), exceeding most single-atom OER catalysts.
Bimetallic layered double hydroxides (LDHs) are promising catalysts for anodic oxygen evolution reaction (OER) in alkaline media. Despite good stability, NiCo LDH displays an unsatisfactory OER activity relative to the most robust NiFe LDH and CoFe LDH. Herein, a novel NiCo LDH electrocatalyst modified with single-atom silver grown on carbon cloth (Ag-SA-NiCo LDH/CC) that exhibits exceptional OER activity and stability in 1.0 m KOH is reported. The Ag-SA-NiCo LDH/CC catalyst only requires a low overpotential of 192 mV to reach a current density of 10 mA cm(-2), obviously boosting the OER activity of NiCo LDH/CC (410 mV@10 mA cm(-2)). Inspiringly, Ag-SA-NiCo LDH/CC can maintain its high activity for up to 500 h at a large current density of 100 mA cm(-2), exceeding most single-atom OER catalysts. In situ Raman spectroscopy studies uncover that the in situ formed NiCoOOH during OER is the real active species. Hard X-ray absorption spectrum (XAS) and density functional theory (DFT) calculations validate that single-atom Ag occupying Ni site increases the chemical valence of Ni elements, and then weakens the adsorption of oxygen-contained intermediates on Ni sites, fundamentally accounting for the enhanced OER performance.

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