Nonstoichiometric perovskite for enhanced catalytic oxidation through excess A-site cation

Ximu Li; Mengran Li; Xue Ma; Jie Miao; Ran Ran; Wei Zhou; shaobin Wang; Zongping Shao

doi:10.1016/j.ces.2020.115596

Nonstoichiometric perovskite for enhanced catalytic oxidation through excess A-site cation

Ximu Li, Mengran Li, Xue Ma, Jie Miao, Ran Ran, Wei Zhou, shaobin Wang, Zongping Shao

Research output: Contribution to journal › Article › peer-review

35 Scopus citations

Abstract

Perovskite oxide has been emerging as one of the efficient heterogeneous catalysts for advanced oxidation of organic contaminants in wastewater because of their structural integrity and compositional tunability. Herein, we report a new perovskite oxide, La_1.15MnO_3+δ with excess La, for a lowered average oxidation state of Mn cations and abundant oxygen vacancies, which can be active sites for peroxymonosulfate (PMS) activation. The La_1.15MnO_3+δ did exhibit improving catalytic performance as compared to LaMnO_3+δ for the degradation of Rhodamine B by activating PMS. Besides, it also demonstrated high tolerance to variant water environments such as temperature, pH and impurity anions. A major non-radical activation mechanism dominated by ¹O₂ was further confirmed in La_1.15MnO_3+δ/PMS system, accompanied by a minor radical pathway. This work provides a new effective strategy to advance catalytic PMS oxidation processes by tailoring the oxidation state of B-site metals and defects of perovskite oxide through manipulating A-site cation stoichiometry.

Original language	English
Article number	115596
Journal	Chemical Engineering Science
Volume	219
DOIs	https://doi.org/10.1016/j.ces.2020.115596
State	Published - 29 Jun 2020

Keywords

LaMnO perovskite
Non-radical pathway
Oxygen vacancies
Peroxymonosulfate activation

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title = "Nonstoichiometric perovskite for enhanced catalytic oxidation through excess A-site cation",

abstract = "Perovskite oxide has been emerging as one of the efficient heterogeneous catalysts for advanced oxidation of organic contaminants in wastewater because of their structural integrity and compositional tunability. Herein, we report a new perovskite oxide, La1.15MnO3+δ with excess La, for a lowered average oxidation state of Mn cations and abundant oxygen vacancies, which can be active sites for peroxymonosulfate (PMS) activation. The La1.15MnO3+δ did exhibit improving catalytic performance as compared to LaMnO3+δ for the degradation of Rhodamine B by activating PMS. Besides, it also demonstrated high tolerance to variant water environments such as temperature, pH and impurity anions. A major non-radical activation mechanism dominated by 1O2 was further confirmed in La1.15MnO3+δ/PMS system, accompanied by a minor radical pathway. This work provides a new effective strategy to advance catalytic PMS oxidation processes by tailoring the oxidation state of B-site metals and defects of perovskite oxide through manipulating A-site cation stoichiometry.",

keywords = "LaMnO perovskite, Non-radical pathway, Oxygen vacancies, Peroxymonosulfate activation",

author = "Ximu Li and Mengran Li and Xue Ma and Jie Miao and Ran Ran and Wei Zhou and shaobin Wang and Zongping Shao",

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year = "2020",

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day = "29",

doi = "10.1016/j.ces.2020.115596",

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T1 - Nonstoichiometric perovskite for enhanced catalytic oxidation through excess A-site cation

AU - Li, Ximu

AU - Li, Mengran

AU - Ma, Xue

AU - Miao, Jie

AU - Ran, Ran

AU - Zhou, Wei

AU - Wang, shaobin

AU - Shao, Zongping

PY - 2020/6/29

Y1 - 2020/6/29

N2 - Perovskite oxide has been emerging as one of the efficient heterogeneous catalysts for advanced oxidation of organic contaminants in wastewater because of their structural integrity and compositional tunability. Herein, we report a new perovskite oxide, La1.15MnO3+δ with excess La, for a lowered average oxidation state of Mn cations and abundant oxygen vacancies, which can be active sites for peroxymonosulfate (PMS) activation. The La1.15MnO3+δ did exhibit improving catalytic performance as compared to LaMnO3+δ for the degradation of Rhodamine B by activating PMS. Besides, it also demonstrated high tolerance to variant water environments such as temperature, pH and impurity anions. A major non-radical activation mechanism dominated by 1O2 was further confirmed in La1.15MnO3+δ/PMS system, accompanied by a minor radical pathway. This work provides a new effective strategy to advance catalytic PMS oxidation processes by tailoring the oxidation state of B-site metals and defects of perovskite oxide through manipulating A-site cation stoichiometry.

AB - Perovskite oxide has been emerging as one of the efficient heterogeneous catalysts for advanced oxidation of organic contaminants in wastewater because of their structural integrity and compositional tunability. Herein, we report a new perovskite oxide, La1.15MnO3+δ with excess La, for a lowered average oxidation state of Mn cations and abundant oxygen vacancies, which can be active sites for peroxymonosulfate (PMS) activation. The La1.15MnO3+δ did exhibit improving catalytic performance as compared to LaMnO3+δ for the degradation of Rhodamine B by activating PMS. Besides, it also demonstrated high tolerance to variant water environments such as temperature, pH and impurity anions. A major non-radical activation mechanism dominated by 1O2 was further confirmed in La1.15MnO3+δ/PMS system, accompanied by a minor radical pathway. This work provides a new effective strategy to advance catalytic PMS oxidation processes by tailoring the oxidation state of B-site metals and defects of perovskite oxide through manipulating A-site cation stoichiometry.

KW - LaMnO perovskite

KW - Non-radical pathway

KW - Oxygen vacancies

KW - Peroxymonosulfate activation

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DO - 10.1016/j.ces.2020.115596

M3 - 文章

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SN - 0009-2509

VL - 219

JO - Chemical Engineering Science

JF - Chemical Engineering Science

M1 - 115596

ER -

Nonstoichiometric perovskite for enhanced catalytic oxidation through excess A-site cation

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Keywords

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