Facile synthesis of ultrafine iron-cobalt (FeCo) nanocrystallite-embedded boron/nitrogen-codoped porous carbon nanosheets: Accelerated water splitting catalysts.

Designing two-dimensional (2D) porous carbon nanosheets is expected to boost the water splitting efficiency of low-cost iron (Fe) and cobalt (Co)-based catalysts. Nevertheless, the aggregations, tedious preparation procedures, and expensive precursors for synthesizing 2D porous carbon nanosheets have hindered their widespread application. Herein, for the first time, we developed a low-cost method for large-scale and rapid synthesis of the three-dimensional (3D) hierarchically porous architectures self-assembled by the ultrafine FeCo nanoparticles embedded and boron/nitrogen-codoped 2D porous carbon nanosheets (denoted as FeCo@BNPCNS). The optimal FeCo@BNPCNS-900 exhibited abundant porous channels, a large surface area, and vast carbon edges/defects. Therefore, 8.10 at% electrochemically active boron (B)/nitrogen (N) centers were doped into the porous carbon nanosheets. In an alkaline solution, the optimal FeCo@BNPCNS-900 nanosheets revealed excellent hydrogen evolution reaction (HER) electrocatalytic activity, surpassing commercial 20 wt% Pt/C. For instance, the HER potential at 10 mA cm-2 [-50.6 mV vs. reversible hydrogen electrode (RHE)] of FeCo@BNPCNS-900 was even 19.3 mV more positive than that of commercial 20 wt% Pt/C (-69.9 mV vs. RHE). Meanwhile, its oxygen evolution reaction (OER) catalytic activity was just a little worse than ruthenium oxide (RuO2). The water electrolysis cell of FeCo@BNPCNS-900 nanosheets just required a small voltage of 1.589 V for full water splitting to achieve 10 mA cm-2, even 70.3 mV more negative than that of the state-of-the-art 20 wt% Pt/C||RuO2 benchmark (1.660 V) with outstanding stability. The perfect 3D hierarchically porous and honeycomb-like architecture, abundant porous channels/mesopores, and uniformly dispersed electrocatalytically active sites on FeCo@BNPCNS-900 nanosheets were responsible for the outstanding water splitting performance. Finally, this study provides an efficient strategy for the large-scale, rapid, and low-cost synthesis of 2D porous carbon nanosheets without using any template, surfactant, or expensive precursors.