Carbon-based bifunctional electrocatalysts for oxygen reduction and oxygen evolution reactions: Optimization strategies and mechanistic analysis

Tailoring of electrocatalyst interactions at interfacial level to benchmark the oxygen reduction reaction

Electronic structure regulation of noble metal-free materials toward alkaline oxygen electrocatalysis

2D black phosphorus (BP) is one promising electrocatalyst toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) catalysis. The too strong adsorption of oxygen intermediates during OER, while the too weak adsorption of hydrogen intermediate during HER, however, greatly compromise its practical water splitting applications with overpotentials as high as 450 mV for OER and 420 mV for HER to achieve 10 mA cm-2 under alkaline conditions. Herein, by rationally introducing the nanosized iridium (Ir) modifier together with optimized exposing surface toward electrolytes, an efficient Ir-modified BP electrocatalyst with much favorable adsorption energies toward catalytic intermediates possesses an outstanding pH-universal water splitting performance, surpassing the nearly all reported BP-based catalysts and the commercial noble-metal catalysts. The Ir-modified BP catalyst with the optimized exposed surfaces only requires an overall cell voltage of 1.54 and 1.57 V to achieve 10 mA cm-2 in acidic and alkaline electrolysers, respectively. This design uncovers the potential applications of 2D BP in practical electrocatalysis fields via decreasing reaction intermediate adsorption energy barriers and promoting the interfacial electron coupling for heterostructured catalysts, and offers new insights into the surface-dependent activity enhancement mechanism.

Surface-Dependent Intermediate Adsorption Modulation on Iridium-Modified Black Phosphorus Electrocatalysts for Efficient pH-Universal Water Splitting.

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.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/adma.202008752

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

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