化学
电化学
催化作用
电子转移
分子间力
阳极
析氧
化学工程
光化学
物理化学
电极
分子
有机化学
工程类
作者
Ariful Ahsan,Tianwei He,Kamel Eid,Aboubakr M. Abdullah,Michael L. Curry,Aijun Du,Alain R. Puente Santiago,Luís Echegoyen,Juan C. Noveron
摘要
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 0D–2D heterostructures composed of boron carbon nitride nanosheets (BCN NSs) and fullerene molecules (C60/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 C60 molecules. The nanohybrid supramolecular material with 10 wt % F in BCN NSs (10% F/BCN) exhibited the largest Raman and C 1s 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 η10 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 ΔGH* 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.
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