Tuning The Intermolecular Electron Transfer Of Low-Dimensional And Metal-Free Bcn/C-60 Electrocatalysts Via Interfacial Defects For Efficient Hydrogen And Oxygen Electrochemistry

The development of low-dimensional (LD) supramolecular materials with multifunctional electrocatalytic properties has sparked the attention of the catalysis community. Herein, we report the synthesis of a new class of OD-2D heterostructures composed of boron carbon nitride nanosheets (BCN NSs) and fullerene molecules (C-60/F) that exhibit multifunctional electrocatalytic properties for the hydrogen evolution/oxidation reactions (HER/HOR) and the oxygen evolution/reduction reactions (OER/ORR). The electrocatalytic properties were studied with varying F:BCN weight ratios to optimize the intermolecular electron transfer (ET) from the BCN NSs to the electron-accepting C-6(0) molecules. The nanohybrid supramolecular material with 10 wt % F in BCN NSs (10% F/BCN) exhibited the largest Raman and C is binding energy shifts, which were associated with greater cooperativity interactions and enhanced ET processes at the F/BCN interface. This synergistic interfacial phenomenon resulted in highly active catalytic sites that markedly boosted electrocatalytic activity of the material. The 10% F/BCN showed the highest tetrafunctional catalytic performance, outperforming the OER catalytic activity of commercial RuO2 catalysts with a eta(10) of 390 mV and very competitive onset potential values of -0.042 and 0.92 V vs RHE for HER and ORR, respectively, and a current density value of 1.47 mA cm(-2) at 0.1 V vs RHE with an ultralow Delta G(H*) value of -0.03 eV toward the HOR process. Additionally, the 10% F/BCN catalyst was also used as both cathode and anode in a water splitting device, delivering a cell potential of 1.61 V to reach a current density of 10 mA cm(-)(2).