Da Wang, Kai Luo, Haole Tian, Haijun Cheng, Stefanos Giannakis, Yang Song, Zhiqiao He, Lizhang Wang, Shuang Song*, Jingyun Fang and Jun Ma,
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It achieved approximately 90% toluene degradation with 56% selectivity toward CO<sub>2</sub>, even under ambient temperature (35 °C) and a relatively humid environment (45%). Modulation of A-sites induced the elongation of Mn–O bonds and decrease in the coordination number of Mn–O (from 6 to 4.3) in LCMO/MnO<sub>2</sub>-4.5, resulting in the creation of abundant multivalent Mn and oxygen vacancies. Doping Cu into B-sites led to the preferential chemisorption of toluene on multivalent Cu (Cu(I)/Cu(II)), consistent with theoretical predictions. Effective electronic supplementary interactions enabled the cycling of multiple oxidation states of Mn for ozone decomposition, facilitating the production of reactive oxygen species and the regeneration of oxygen vacancies. This study establishes high-performance perovskites for the synergistic regulation of O<sub>3</sub> and toluene, contributing to cleaner and safer industrial activities.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8000,"publicationDate":"2024-06-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Transforming Plain LaMnO3 Perovskite into a Powerful Ozonation Catalyst: Elucidating the Mechanisms of Simultaneous A and B Sites Modulation for Enhanced Toluene Degradation\",\"authors\":\"Da Wang, Kai Luo, Haole Tian, Haijun Cheng, Stefanos Giannakis, Yang Song, Zhiqiao He, Lizhang Wang, Shuang Song*, Jingyun Fang and Jun Ma, \",\"doi\":\"10.1021/acs.est.4c00809\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Herein, we propose preferential dissolution paired with Cu-doping as an effective method for synergistically modulating the A- and B-sites of LaMnO<sub>3</sub> perovskite. 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引用次数: 0
摘要
在此,我们提出将优先溶解与掺铜配对作为协同调节 LaMnO3 包晶的 A-和 B-位点的有效方法。通过向 LaMnO3 的 B 盐基中掺入铜,特别是对 B 盐基进行改性,产生了双包晶石 La2CuMnO6。随后,使用 HNO3 蚀刻了 La2CuMnO6 A 盐基中的部分 La,形成了新型 La2CuMnO6/MnO2 (LCMO/MnO2)催化剂。优化催化剂的理想锰铜比为 4.5:1(LCMO/MnO2-4.5),具有优异的臭氧催化性能。即使在环境温度(35 °C)和相对湿度(45%)的环境下,它也能实现约 90% 的甲苯降解,对二氧化碳的选择性为 56%。在 LCMO/MnO2-4.5 中,对 A 位点的调节引起了锰-O 键的拉长和锰-O 配位数的降低(从 6 降至 4.3),从而产生了大量的多价锰和氧空位。在 B-位点中掺入铜会导致甲苯优先化学吸附在多价铜(Cu(I)/Cu(II))上,这与理论预测一致。有效的电子补充相互作用使锰的多种氧化态循环用于臭氧分解,促进了活性氧的产生和氧空位的再生。这项研究为协同调节臭氧和甲苯建立了高性能的过氧化物晶石,为更清洁、更安全的工业活动做出了贡献。
Transforming Plain LaMnO3 Perovskite into a Powerful Ozonation Catalyst: Elucidating the Mechanisms of Simultaneous A and B Sites Modulation for Enhanced Toluene Degradation
Herein, we propose preferential dissolution paired with Cu-doping as an effective method for synergistically modulating the A- and B-sites of LaMnO3 perovskite. Through Cu-doping into the B-sites of LaMnO3, specifically modifying the B-sites, the double perovskite La2CuMnO6 was created. Subsequently, partial La from the A-sites of La2CuMnO6 was etched using HNO3, forming novel La2CuMnO6/MnO2 (LCMO/MnO2) catalysts. The optimized catalyst, featuring an ideal Mn:Cu ratio of 4.5:1 (LCMO/MnO2-4.5), exhibited exceptional catalytic ozonation performance. It achieved approximately 90% toluene degradation with 56% selectivity toward CO2, even under ambient temperature (35 °C) and a relatively humid environment (45%). Modulation of A-sites induced the elongation of Mn–O bonds and decrease in the coordination number of Mn–O (from 6 to 4.3) in LCMO/MnO2-4.5, resulting in the creation of abundant multivalent Mn and oxygen vacancies. Doping Cu into B-sites led to the preferential chemisorption of toluene on multivalent Cu (Cu(I)/Cu(II)), consistent with theoretical predictions. Effective electronic supplementary interactions enabled the cycling of multiple oxidation states of Mn for ozone decomposition, facilitating the production of reactive oxygen species and the regeneration of oxygen vacancies. This study establishes high-performance perovskites for the synergistic regulation of O3 and toluene, contributing to cleaner and safer industrial activities.
期刊介绍:
Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences.
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