Volume 1, 2023

Phase shuttling-enhanced electrochemical ozone production

Abstract

Ozone can be produced by the electrochemical oxidation of water, which provides a technical solution to on-demand ozone production for disinfection and sterilization. Lead oxides have been found to be unique in catalyzing such a process. However, the fundamental understanding of these catalysts’ mechanisms remains limited, hindering the development of high-performance catalysts for electrochemical ozone production (EOP). Herein, the effect of phase shuttling on the reactivity of Pb3O4 was systematically investigated during the EOP process by in situ/ex situ characterizations. It was found that Pb3O4 undergoes a phase shuttle towards β-PbO2via the lattice oxygen oxidation mechanism (LOM) pathway, and the reconstructed β-PbO2 shows enhanced EOP activity and stability compared to commercial β-PbO2. The ex situ characterization of materials combined with theoretical calculations reveals that the performance enhancement is mainly attributed to the stable presence of (101) and (110) surfaces in the reconstructed β-PbO2 with undercoordinated Pb–O. Pourbaix diagrams of lead oxides calculated by DFT demonstrate that the phase shuttling to β-PbO2 is thermodynamically favorable under EOP conditions. Surface Pourbaix diagrams of β-PbO2(101) and Pb3O4(110) further reveal the adsorption behavior of O*/OH* intermediates and explain the observed change of EOP kinetics at ∼1.6 V vs. RHE. The catalyst is integrated and assembled in a membrane electrode assembly (MEA) electrolyzer, and the produced ozonated water successfully inactivated severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2). This work provides a new insight into EOP catalysts and demonstrates the possibilities of further optimization of electrochemical approaches for on-demand ozone generation.

Graphical abstract: Phase shuttling-enhanced electrochemical ozone production

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Article information

Article type
Paper
Submitted
25 ינו 2023
Accepted
07 מרץ 2023
First published
13 מרץ 2023
This article is Open Access
Creative Commons BY-NC license

EES. Catal., 2023,1, 301-311

Phase shuttling-enhanced electrochemical ozone production

J. Liu, S. Wang, Z. Yang, C. Dai, G. Feng, B. Wu, W. Li, L. Shu, K. Elouarzaki, X. Hu, X. Li, H. Wang, Z. Wang, X. Zhong, Z. J. Xu and J. Wang, EES. Catal., 2023, 1, 301 DOI: 10.1039/D3EY00015J

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