Co3O4-δ quantum dots (Co3O4-δ-QDs) with a crystallite size of approximately 2 nm and oxygen vacancies were fabricated through multicycle lithiation/delithiation of mesoporous Co3O4 nanosheets. Used as an oxygen evolution reaction (OER) electrocatalyst for water splitting, the catalytic performance (an overpotential of 270 mV@10 mA cm-2 and no decay within 30 h) of Co3O4-δ-QDs is superior to that of previously reported Co-based catalysts and the state-of-the-art IrO2. Compared to that of the Co3O4 nanosheets, the enhanced OER activity of Co3O4-δ-QDs is attributed to two factors: one is the increased quantity of the Faradaic active sites, including the total active sites (q*Total), the most accessible active sites (q*Outer), and their ratio (q*Outer/q*Total); the other is the enhanced intrinsic electroactivity per active site evaluated by the turnover frequency and the current density normalized by the most accessible active sites (j/q*Outer) related to the OER. This multicycle lithiation/delithiation method can be applied to other transition metal oxides as well, offering a general approach to develop high-performance electrocatalysts for water splitting.
Keywords: Co3O4−δ quantum dots; electrocatalyst; lithiation/delithiation; oxygen evolution reaction; oxygen vacancies.