Interfacial Covalent Bonds Regulated Electron-Deficient 2D Black Phosphorus for Electrocatalytic Oxygen Reactions

Wang X, Raghupathy RKM, Querebillo CJ, Liao Z, Li D, Lin K, Hantusch M, Sofer Z, Li B, Zschech E, Weidinger IM, Kühne TD, Mirhosseini H, Yu M, Feng X (2021)

Publication Type: Journal article

Publication year: 2021

Journal

Advanced Materials Wiley

Book Volume: 33

Article Number: 2008752

Journal Issue: 20

DOI: 10.1002/adma.202008752

Abstract

Developing resource-abundant and sustainable metal-free bifunctional oxygen electrocatalysts is essential for the practical application of zinc–air batteries (ZABs). 2D black phosphorus (BP) with fully exposed atoms and active lone pair electrons can be promising for oxygen electrocatalysts, which, however, suffers from low catalytic activity and poor electrochemical stability. Herein, guided by density functional theory (DFT) calculations, an efficient metal-free electrocatalyst is demonstrated via covalently bonding BP nanosheets with graphitic carbon nitride (denoted BP-CN-c). The polarized P-N covalent bonds in BP-CN-c can efficiently regulate the electron transfer from BP to graphitic carbon nitride and significantly promote the OOH* adsorption on phosphorus atoms. Impressively, the oxygen evolution reaction performance of BP-CN-c (overpotential of 350 mV at 10 mA cm−2, 90% retention after 10 h operation) represents the state-of-the-art among the reported BP-based metal-free catalysts. Additionally, BP-CN-c exhibits a small half-wave overpotential of 390 mV for oxygen reduction reaction, representing the first bifunctional BP-based metal-free oxygen catalyst. Moreover, ZABs are assembled incorporating BP-CN-c cathodes, delivering a substantially higher peak power density (168.3 mW cm−2) than the Pt/C+RuO2-based ZABs (101.3 mW cm−2). The acquired insights into interfacial covalent bonds pave the way for the rational design of new and affordable metal-free catalysts.

Involved external institutions

Technische Universität Dresden DE Germany (DE) Universität Paderborn DE Germany (DE) Fraunhofer-Institut für Keramische Technologien und Systeme (IKTS) DE Germany (DE) Tsinghua University CN China (CN) Leibniz-Institut für Festkörper- und Werkstoffforschung Dresden e.V. (IFW) / Leibniz Institute for Solid State and Materials Research Dresden DE Germany (DE) University of Chemistry and Technology (UCT) / Vysoká škola chemicko-technologická (VŠCHT) CZ Czech Republic (CZ)

How to cite

APA:

Wang, X., Raghupathy, R.K.M., Querebillo, C.J., Liao, Z., Li, D., Lin, K.,... Feng, X. (2021). Interfacial Covalent Bonds Regulated Electron-Deficient 2D Black Phosphorus for Electrocatalytic Oxygen Reactions. Advanced Materials, 33(20). https://doi.org/10.1002/adma.202008752

MLA:

Wang, Xia, et al. "Interfacial Covalent Bonds Regulated Electron-Deficient 2D Black Phosphorus for Electrocatalytic Oxygen Reactions." Advanced Materials 33.20 (2021).

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