Controlling the Interfacial Charge Polarization of MOF-Derived 0D–2D vdW Architectures as a Unique Strategy for Bifunctional Oxygen Electrocatalysis

The design of alternative earth-abundant van der Waals (vdW) nanoheterostructures for bifunctional oxygen evolution/reduction (OER/ORR) electrocatalysis is of paramount importance to fabricate energy-related devices. Herein, we report a simple metal–organic framework (MOF)-derived synthetic strategy to fabricate low-dimensional (LD) nanohybrids formed by zero-dimensional (0D) ZrO2 nanoparticles (NPs) and heteroatom-doped two-dimensional (2D) carbon nanostructures. The 2D platforms controlled the electronic structures of interfacial Zr atoms, thus producing optimized electron polarization for boron and nitrogen-doped carbon (BCN)/ZrO2 nanohybrids. X-ray photoelectron spectroscopy (XPS) and theoretical studies revealed the key role of the synergistic couple effect of boron (B) and nitrogen (N) in interfacial electronic polarization. The BCN/ZrO2 nanohybrid showed excellent bifunctional electrocatalytic activity, delivering an overpotential (η10) of 301 mV to reach a current density of 10 mA–cm–2 for the OER process and a half-wave potential (E1/2) of 0.85 V vs reversible hydrogen electrode (RHE) for the ORR process, which are comparable to the state-of-the-art LD nanohybrids. Furthermore, BCN/ZrO2 also showed competitive performances for water-splitting and zinc–air battery devices. This work establishes a new route to fabricate highly efficient multifunctional electrocatalysts by tuning the electronic polarization properties of 0D–2D electrochemical interfaces.

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