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Engineering Ag-O-Mn bridges with enhanced oxygen mobility over Ag substituted LaMnO3 perovskite catalyst for robustly boosting toluene combustion
Separation and Purification Technology ( IF 8.1 ) Pub Date : 2023-06-02 , DOI: 10.1016/j.seppur.2023.124240
Bing Li , Fulin Deng , Zheyu Li , Hao Xiong , Shuqu Zhang , Weili Dai , Jie Zhang , Lixia Yang , Jianping Zou , Xubiao Luo

Perovskite oxide, as a promising candidate for volatile organic compounds combustion, is incapable in practical application at present due to its low intrinsic activity resulting from inadequate active oxygen species. However, balancing the concentration of active oxygen species and robust structure for perovskite oxide is still challenging. Herein, an efficient perovskite-based catalyst (denoted as TA-La0.9Ag0.1MnO3) was constructed through Ag substitution and subsequently tartaric acid etching of LaMnO3, which exhibits robustly boosted catalytic performance for toluene combustion compared with pristine LaMnO3, causing a ∼100 °C lower T90. In this study, Ag substitution could weaken the La-O hybridization, which effectively facilitates La cations removal by subsequent acid etching, thus sufficiently exposing active Ag and Mn species and generating more surface lattice oxygen, but also constructs Ag-Mn-O bridges within the matrix of Ag substituted LaMnO3. Acid etching enables the activation of Ag-O-Mn bridges with strong electron transfer ability from O to Ag atom, promoting the mobility of lattice oxygen, and consequently the low-temperature oxidation ability. Additionally, the exposed Ag and Mn as Lewis acid sites can effectively improve the adsorption capacity toward toluene molecules, which synergistically facilitates the toluene abatement. Notably, TA-La0.9Ag0.1MnO3 also exhibits superb long-term stability, water-resistance, and high thermal stability up to 650 °C.



中文翻译:

设计 Ag-O-Mn 桥,在 Ag 取代的 LaMnO3 钙钛矿催化剂上具有增强的氧迁移率,可强力促进甲苯燃烧

钙钛矿氧化物作为挥发性有机化合物燃烧的有前途的候选者,由于活性氧不足导致其本征活性低,目前无法实际应用。然而,平衡钙钛矿氧化物的活性氧浓度和坚固结构仍然具有挑战性。在此,一种高效的基于钙钛矿的催化剂(表示为 TA-La 0.9 Ag 0.1 MnO 3 )通过 Ag 取代和随后的 LaMnO 3酒石酸蚀刻构建,与原始 LaMnO 3相比,它对甲苯燃烧表现出强劲的催化性能,导致~100 °C 低 T 90. 在这项研究中,Ag 取代可以削弱 La-O 杂化,这有效地促进了 La 阳离子通过随后的酸蚀刻去除,从而充分暴露活性 Ag 和 Mn 物种并产生更多的表面晶格氧,但也在内部构建 Ag-Mn-O 桥Ag基体取代了LaMnO 3。酸刻蚀能够激活具有从 O 到 Ag 原子的强电子转移能力的 Ag-O-Mn 桥,促进晶格氧的流动性,从而提高低温氧化能力。此外,暴露的Ag和Mn作为路易斯酸位点可以有效提高对甲苯分子的吸附能力,从而协同促进甲苯减排。值得注意的是,TA-La 0.9 Ag 0.1 MnO 3还表现出卓越的长期稳定性、防水性和高达 650 °C 的高热稳定性。

更新日期:2023-06-04
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