Layered double hydroxides (LDHs) are promising electrocatalytic
materials for the oxygen evolution reaction (OER) due to their tunable
composition and low cost. Here, we construct ultrathin Al-incorporated
Co LDH nanosheets on carbon cloth (CC) by a facile hydrothermal strategy.
Compared to Co LDH/CC, the optimized Co2Al1 LDH/CC
displays significantly improved OER performance, characterized by
low overpotentials of only 171 and 200 mV to reach current densities
of 10 mA cm–2 in alkaline and neutral media, respectively,
as well as good stability over an extended period. The introduced
Al3+ and CC support play a synergistic role in steering
the morphology of Co2Al1 LDH/CC while also increasing
the electrochemical active sites. X-ray absorption fine spectra (XAFS)
analyses uncover the critical role of Al in regulating the coordination
environment of Co atoms, with evidence affording highly active Co
oxidation states. Moreover, density functional theory (DFT) calculations
confirmed that the Al3+ incorporated into Co LDH/CC can
efficaciously modulate the electronic density of states of the d-band
center of Co atoms, optimize the Gibbs free energies of intermediates
toward OER, and thus accelerate the O2 evolution rate.