Unassisted selective solar hydrogen peroxide production by an oxidised buckypaper-integrated perovskite photocathode

Rashmi Mehrotra,Ji-Wook Jang,Dongrak Oh

doi:10.1038/s41467-021-26832-5

Rashmi Mehrotra, Ji-Wook Jang + Show 1 more

Open Access

https://doi.org/10.1038/s41467-021-26832-5

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Abstract

Hydrogen peroxide (H2O2) is an eco-friendly oxidant and a promising energy source possessing comparable energy density to that of compressed H2. The current H2O2 production strategies mostly depend on the anthraquinone oxidation process, which requires significant energy and numerous organic chemicals. Photocatalyst-based solar H2O2 production comprises single-step O2 reduction to H2O2, which is a simple and eco-friendly method. However, the solar-to-H2O2 conversion efficiency is limited by the low performance of the inorganic semiconductor-based photoelectrodes and low selectivity and stability of the H2O2 production electrocatalyst. Herein, we demonstrate unassisted solar H2O2 production using an oxidised buckypaper as the H2O2 electrocatalyst combined with a high-performance inorganic-organic hybrid (perovskite) photocathode, without the need for additional bias or sacrificial agents. This integrated photoelectrode system shows 100% selectivity toward H2O2 and a solar-to-chemical conversion efficiency of ~1.463%.

Highlights

Hydrogen peroxide (H2O2) is an eco-friendly oxidant and a promising energy source possessing comparable energy density to that of compressed H2
Solar H2O2 production via the single-step reduction of O2 using a photocatalyst offers a simple, safe, and sustainable alternative[9,10,11].To date, several strategies have been reported for efficient solar H2O2 production[10,11], wherein the main focus lies in increasing the solar-to-chemical (H2O2) conversion efficiency (SCC; %) by improving the photoelectrode performance and electrocatalyst selectivity
We successfully passivated a high-performance PSK photoelectrode using oxidised buckypaper (O-BP), which acts as a selective electrocatalyst for H2O2 production and a protection layer when combined with Field’s metal (FM) to prevent water penetration

Summary

Introduction

Hydrogen peroxide (H2O2) is an eco-friendly oxidant and a promising energy source possessing comparable energy density to that of compressed H2. We demonstrate unassisted solar H2O2 production using an oxidised buckypaper as the H2O2 electrocatalyst combined with a high-performance inorganic-organic hybrid (perovskite) photocathode, without the need for additional bias or sacrificial agents This integrated photoelectrode system shows 100% selectivity toward H2O2 and a solar-to-chemical conversion efficiency of ~1.463%. Precious Pdbased catalysts and high-pressure H2 used during the hydrogenation reaction increase the cost of the process and introduce many safety issues[6,7,8] In this regard, solar H2O2 production via the single-step reduction of O2 using a photocatalyst offers a simple, safe, and sustainable alternative[9,10,11].To date, several strategies have been reported for efficient solar H2O2 production[10,11], wherein the main focus lies in increasing the solar-to-chemical (H2O2) conversion efficiency (SCC; %) by improving the photoelectrode performance and electrocatalyst selectivity. A H2O2 production rate of ~0.751 μmol min−1 cm−2 and an SCC of ~1.463% were achieved[29]

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