Yang, L.Jiao, Y.Xu, X.Pan, Y.Su, C.Duan, X.Sun, H.Liu, S.Wang, S.Shao, Z.2022-02-242022-02-242022ACS Sustainable Chemistry and Engineering, 2022; 10(5):1899-19092168-04852168-0485https://hdl.handle.net/2440/134441Perovskite-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.en© 2022, American Chemical SocietyRuddlesden−Popper layered perovskite; non-free radical pathway; reactive oxygen species; interstitial oxygen; peroxymonosulfateJournal article10.1021/acssuschemeng.1c076052022-02-24600140Duan, X. [0000-0001-9635-5807]Wang, S. [0000-0002-1751-9162]