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

Md Ariful Ahsan; Tianwei He; Kamel Eid; Aboubakr M Abdullah; Mohamed Fathi Sanad; Ali Aldalbahi; Bonifacio Alvarado-Tenorio; Aijun Du; Alain R Puente Santiago; Juan C Noveron

doi:10.1021/acsami.1c17283

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

ACS Appl Mater Interfaces. 2022 Jan 26;14(3):3919-3929. doi: 10.1021/acsami.1c17283. Epub 2022 Jan 11.

Authors

Md Ariful Ahsan^{1

2}, Tianwei He^{3

4}, Kamel Eid⁵, Aboubakr M Abdullah⁶, Mohamed Fathi Sanad⁷, Ali Aldalbahi⁸, Bonifacio Alvarado-Tenorio⁹, Aijun Du^{3

4}, Alain R Puente Santiago¹, Juan C Noveron^{1

2}

Affiliations

¹ Department of Chemistry and Biochemistry, University of Texas at El Paso, El Paso, Texas 79968, United States.
² Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment, Houston, Texas 77005, United States.
³ Centre for Materials Science, Queensland University of Technology, Gardens Point Campus, Brisbane, QLD 4000, Australia.
⁴ School of Chemistry and Physics, Science and Engineering Faculty, Queensland University of Technology, Gardens Point Campus, Brisbane, QLD 4000, Australia.
⁵ Gas Processing Center, College of Engineering, Qatar University, Doha 2713, Qatar.
⁶ Center for Advanced Materials, Qatar University, Doha 2713, Qatar.
⁷ Department of Environmental Sciences and Engineering, University of Texas at El Paso, El Paso, Texas 79968, United States.
⁸ Department of Chemistry, College of Science, King Saud University, Riyadh 11451, Saudi Arabia.
⁹ Universidad Autonoma de Ciudad Juarez, Ciudad Juarez 32310, Mexico.

PMID: 35014264
DOI: 10.1021/acsami.1c17283

Abstract

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 (E_1/2) 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.

Keywords: 0D−2D nanohybrid; metal−organic framework; overall water splitting; oxygen evolution reaction; oxygen reduction reaction; zinc−air battery.