Theoretical Prediction of a Bi-Doped β-Antimonene Monolayer as a Highly Efficient Photocatalyst for Oxygen Reduction and Overall Water Splitting.

Deobrat Singh,Rajeev Ahuja

doi:10.1021/acsami.1c18191

Abstract

The photo-/electrocatalysts with high activities for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and the oxygen reduction reaction (ORR) are of significance for the advancement of photo-/electrochemical energy systems such as solar energy to resolve the global energy crisis, reversible water electrolyzers, metal–air batteries, and fuel cells. In the present work, we have systematically investigated the photochemical performance of the 2D β-antimonene (β-Sb) monolayer. From density functional theory investigations, β-Sb with single-atom doping possesses a trifunctional photocatalyst with high energetics and thermal stabilities. In particular, it is predicted that the performance of the HER activity of β-Sb will be superior to most of the 2D materials. Specifically, β-Sb with single atom replacement has even superior that the reference catalysts IrO2(110) and Pt(111) with relatively low overpotential values for ORR and OER mechanisms. The superior catalytic performance of β-Sb has been described by its electronic structures, charge transfer mechanism, and suitable valence and conduction band edge positions versus normal hydrogen electrode. Meanwhile, the low overpotential of multifunctional photocatalysts of the Bi@β-Sb monolayer makes them show a remarkable performance in overall water splitting (0.06 V for HER, 0.25 V for OER, and 0.31 V for ORR). In general, the Bi@β-Sb monolayer may be an excellent trifunctional catalyst that exhibits high activity toward all electrode reactions of hydrogen and oxygen.

Highlights

The rapid development of modern society needs cost-effective and high-performance photo-/electrocatalysts, which play critical roles in the storage and conversion of renewable energy, for example, hydrogen production from water electrolysis, rechargeable metal−air batteries, and fuel cells, including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) mechanisms.[1−5] So far, the advanced catalysts are still dominated by expensive noble metal or their oxides such as Pt for HER and ORR and RuO2, IrO2, and so forth for OER.[6,7]
We have checked that the β-Sb monolayer has been energetically, dynamically, and thermally stable, which is confirmed by cohesive energy, phonon dispersion spectra, and Ab initio molecular dynamics (AIMD) calculations
The 2D β-Sb monolayers are energetically, dynamically, and thermally stable, and it is confirmed on the basis of cohesive energy, phonon band structure, and AIMD simulations

Summary

Introduction

The rapid development of modern society needs cost-effective and high-performance photo-/electrocatalysts, which play critical roles in the storage and conversion of renewable energy, for example, hydrogen production from water electrolysis, rechargeable metal−air batteries, and fuel cells, including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) mechanisms.[1−5] So far, the advanced catalysts are still dominated by expensive noble metal or their oxides such as Pt for HER and ORR and RuO2, IrO2, and so forth for OER.[6,7] In particular, the multistep proton and electron transfer process of oxygen electrode reactions such as OER/ORR with scale relationships is usually kinetically slow and proceeds with a high overpotential, which severely hamper their commercial applications.[8] it is of great consequence and necessity to explore alternative nonprecious catalysts that are more efficient and durable.

Methods

Results

Conclusion