Iron Doped in the Subsurface of CuS Nanosheets by Interionic Redox: Highly Efficient Electrocatalysts toward the...

Modifying the electronic structure of electrocatalysts by metal doping is favorable to their electrocatalytic activity. Herein, by a facile one-pot redox process of Fe(III) and Cu(I), Fe(II) was successfully doped into the subsurface of CuS nanosheets (NSs) for the first time to obtain a novel electrocatalyst (Fe_sub-CuS NSs) that possesses not only subtle lattice defects but also an atomic-level coupled nanointerface, greatly enhancing the oxygen evolution reaction (OER) performances. Meanwhile, Fe(II) and Fe(III) coexisting in Fe_sub-CuS nanosheets are favorable to OER through valence regulation. As expected, by simultaneously controlling the abovementioned three factors to optimize Fe_sub-CuS nanosheets, they display a lower overpotential of 252 mV at a current density of 20 mA cm^-2 for OER, better than 389 mV for pristine CuS nanosheets. This discovery furnishes low-cost and efficient Cu-based electrocatalysts by metal doping. Density functional theory (DFT) calculations further verify that Fe_sub-CuS(100) is thermodynamically stable and is more active for OER. This research provides a strategy for the atomic-scale engineering of nanocatalysts and also sheds light on the design of novel and efficient electrocatalysts.