TY - JOUR
T1 - Boosting performance of lanthanide magnetism perovskite for advanced oxidation through lattice doping with catalytically inert element
AU - Miao, Jie
AU - Duan, Xiaoguang
AU - Li, Jiang
AU - Dai, Jie
AU - Liu, Bo
AU - Wang, Shaobin
AU - Zhou, Wei
AU - Shao, Zongping
N1 - Publisher Copyright:
© 2018
PY - 2019/1/1
Y1 - 2019/1/1
N2 - ABO3-type perovskite oxides, characterized by high structural flexibility, have found potential applications in many redox processes, including as catalysts for advanced oxidation in wastewater remediation. Here, we demonstrated that by doping the generally believed catalytically inert A-site of LaMnO3 (LMO) perovskite with strontium, the catalytic performance for advanced oxidation is surprisingly boosted. Specifically, La0.4Sr0.6MnO3-δ (LSMO46) was designed which exhibited a high specific activity (0.0608 min−1 m−2) for peroxymonosulfate (PMS) activation, ∼6 times that of LMO and ∼41 times that of reported nanosized MnFe2O4 and Fe/Fe3C. The superior activity was also embodied by low activation energy (44.3 kJ mol−1). Moreover, LSMO46 displayed a lower metal leaching and a better reusability than LMO and Fe/Fe3C and easy catalyst recovery for its magnetic behavior. Such enhanced catalytic activity was attributed to the positively-charged surface (8.3 mV) that favored the adsorption of negatively-charged organics and the presence of a large amount of surface anion defects (oxygen vacancies), created by the doping, that induced the generation of considerable amount of singlet oxygen (1O2) which was demonstrated as the dominant reactive species by selective radical scavenging and EPR trapping. A coupled activation mechanism involving major singlet oxygen and minor free radicals was further proposed for the effective decomposition of organics in LSMO46/PMS system. The findings in this study thus provide us a new strategy for the development of efficient catalysts for advanced oxidation in environmental treatment.
AB - ABO3-type perovskite oxides, characterized by high structural flexibility, have found potential applications in many redox processes, including as catalysts for advanced oxidation in wastewater remediation. Here, we demonstrated that by doping the generally believed catalytically inert A-site of LaMnO3 (LMO) perovskite with strontium, the catalytic performance for advanced oxidation is surprisingly boosted. Specifically, La0.4Sr0.6MnO3-δ (LSMO46) was designed which exhibited a high specific activity (0.0608 min−1 m−2) for peroxymonosulfate (PMS) activation, ∼6 times that of LMO and ∼41 times that of reported nanosized MnFe2O4 and Fe/Fe3C. The superior activity was also embodied by low activation energy (44.3 kJ mol−1). Moreover, LSMO46 displayed a lower metal leaching and a better reusability than LMO and Fe/Fe3C and easy catalyst recovery for its magnetic behavior. Such enhanced catalytic activity was attributed to the positively-charged surface (8.3 mV) that favored the adsorption of negatively-charged organics and the presence of a large amount of surface anion defects (oxygen vacancies), created by the doping, that induced the generation of considerable amount of singlet oxygen (1O2) which was demonstrated as the dominant reactive species by selective radical scavenging and EPR trapping. A coupled activation mechanism involving major singlet oxygen and minor free radicals was further proposed for the effective decomposition of organics in LSMO46/PMS system. The findings in this study thus provide us a new strategy for the development of efficient catalysts for advanced oxidation in environmental treatment.
KW - Advanced oxidation
KW - Doping
KW - Perovskite
KW - Single oxygen
KW - Wastewater remediation
UR - http://www.scopus.com/inward/record.url?scp=85052757629&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2018.08.192
DO - 10.1016/j.cej.2018.08.192
M3 - 文章
AN - SCOPUS:85052757629
SN - 1385-8947
VL - 355
SP - 721
EP - 730
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
ER -