Facile preparation of alkali metal‐modified hollow nanotubular manganese‐based oxide catalysts and their excellent catalytic soot combustion performance

Chunlei Zhang, Siyu Gao, Xinyu Chen, Di Yu, Lanyi Wang, Xiaoqiang Fan, Ying Cheng, Xuehua Yu, Zhen Zhao
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Abstract

The soot emitted during the operation of diesel engine exhaust seriously threatens the human health and environment, so treating diesel engine exhaust is critical. At present, the most effective method for eliminating soot particles is post‐treatment technology. Preparation of economically viable and highly active soot combustion catalysts is a pivotal element of post‐treatment technology. In this study, different single‐metal oxide catalysts with fibrous structures and alkali metal‐modified hollow nanotubular Mn‐based oxide catalysts were synthesized using centrifugal spinning method. Activity evaluation results showed that the manganese oxide catalyst has the best catalytic activity among the prepared single‐metal oxide catalysts. Further research on alkali metal modification showed that doping alkali metals is beneficial for improving the oxidation state of manganese and generating a large number of reactive oxygen species. Combined with the structural effect brought by the hollow nanotube structure, the alkali metal‐modified Mn‐based oxide catalysts exhibit superior catalytic performance. Among them, the Cs‐modified Mn‐based oxide catalyst exhibits the best catalytic performance because of its rich active oxygen species, excellent NO oxidation ability, abundant Mn4+ ions (Mn4+/Mnn+ = 64.78%), and good redox ability. The T10, T50, T90, and CO2 selectivity of the Cs‐modified Mn‐based oxide catalyst were 267°C, 324°C, 360°C, and 97.8%, respectively.

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碱金属改性空心纳米管锰基氧化物催化剂的简便制备及其优异的烟尘催化燃烧性能
柴油发动机运行过程中排放的烟尘严重威胁人类健康和环境,因此柴油发动机尾气处理至关重要。目前,消除烟尘颗粒最有效的方法是后处理技术。制备经济可行的高活性烟尘燃烧催化剂是后处理技术的关键要素。本研究采用离心纺丝法合成了不同的纤维状单金属氧化物催化剂和碱金属改性空心纳米管锰基氧化物催化剂。活性评价结果表明,在所制备的单金属氧化物催化剂中,氧化锰催化剂的催化活性最好。对碱金属改性的进一步研究表明,掺杂碱金属有利于改善锰的氧化态,产生大量活性氧。结合空心纳米管结构带来的结构效应,碱金属改性的锰基氧化物催化剂表现出优异的催化性能。其中,Cs 改性 Mn 基氧化物催化剂具有丰富的活性氧物种、优异的 NO 氧化能力、丰富的 Mn4+ 离子(Mn4+/Mnn+ = 64.78%)和良好的氧化还原能力,因此催化性能最佳。Cs 改性锰基氧化物催化剂的 T10、T50、T90 和 CO2 选择性分别为 267°C、324°C、360°C 和 97.8%。
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