Title

Superstructures with atomic-level arranged perovskite and oxide layers for advanced oxidation with an enhanced non-free radical pathway

Document Type

Journal Article

Publication Title

ACS Sustainable Chemistry & Engineering

Publisher

ACS

School

School of Science

RAS ID

52736

Funders

Australian Research Council

Grant Number

ARC Number : DP200103332, DP200103315

Comments

Yang, L., Jiao, Y., Xu, X., Pan, Y., Su, C., Duan, X., . . . Shao, Z. (2022). Superstructures with atomic-level arranged perovskite and oxide layers for advanced oxidation with an enhanced non-free radical pathway. ACS Sustainable Chemistry & Engineering, 10(5), 1899-1909.

https://doi.org/10.1021/acssuschemeng.1c07605

Abstract

Perovskite-based oxides demonstrate a great catalytic efficiency in advanced oxidation processes (AOPs), where both free and non-free radical pathways may occur. The non-free radical pathway is preferable because it is less affected by the wastewater environment, yet little is known about its origin. Here, we exploit Ruddlesden-Popper (RP) layered perovskite oxides as an excellent platform for investigating the structure-property relationship for peroxymonosulfate (PMS) activation in AOPs. The atomic-level interaction of the perovskite and rock salt layers in RP oxides stabilizes the transition metals at low valences, causing the formation of abundant lattice oxygen/interstitial oxygen species. Unlike oxygen vacancies in conventional perovskites, which promote free-radical generation, these reactive oxygen species in RP perovskites have high activity and mobility and facilitate the formation of non-free radical singlet oxygen. This singlet oxygen reaction pathway is optimized by tailoring the oxygen species, leading to the discovery of LaSrCo0.8Fe0.2O4 with exceptionally efficient PMS activation.

DOI

10.1021/acssuschemeng.1c07605

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