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调控中空钴锰亚纳米球上晶格氧的迁移率以增强甲苯和邻二甲苯的催化氧化

Regulating the mobility of lattice oxygen on hollow cobalt-manganese sub-nanospheres for enhanced catalytic oxidation of toluene and o-xylene.

作者信息

Li Mingyang, Liu Xinzhu, Niu Xiaoyu, Zhu Yujun

机构信息

Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, School of Chemistry and Materials, Heilongjiang University, Harbin, 150080 PR China.

Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, School of Chemistry and Materials, Heilongjiang University, Harbin, 150080 PR China.

出版信息

J Colloid Interface Sci. 2024 Oct;671:192-204. doi: 10.1016/j.jcis.2024.05.167. Epub 2024 May 23.

DOI:10.1016/j.jcis.2024.05.167
PMID:38797145
Abstract

Promoting lattice oxygen mobility of Co-based catalysts is crucial to making progress in catalytic oxidation technology. The addition of manganese, a transition metal with similar ionic radius to cobalt and variable valence, was supposed to enhance the mobility of lattice oxygen species of Co-based oxide. A range of hollow CoMnO sub-nanosphere catalysts with different Mn/Co ratios was synthesized via a template-sacrificed method, and the effects of different Mn/Co ratios on the structural properties of the catalysts and their catalytic performance for benzene series volatile organic compounds (VOCs) oxidation were investigated. Hollow CoMnO sub-nanosphere exhibited good catalytic activity for oxidation of toluene (T = 265 °C) and o-xylene (T = 297 °C), as well as excellent recycling ability and water resistance. By adjusting the Mn/Co ratio, metal ions enter into the different tetrahedral or octahedral active sites. Compared with CoO, the desorption temperature of surface lattice oxygen on CoMnO decreased by 110 °C. These results demonstrate that the addition of manganese can encourage the electron transfer on CoMnO, indicating that the introduction of the appropriate amount of manganese accelerates the activation of gas O and mobility of surface lattice oxygen species, thereby expediting the oxidation of benzene series VOCs.

摘要

提高钴基催化剂的晶格氧迁移率对于催化氧化技术的进展至关重要。添加锰,一种离子半径与钴相似且具有可变价态的过渡金属,被认为可以提高钴基氧化物晶格氧物种的迁移率。通过模板牺牲法合成了一系列具有不同Mn/Co比的中空CoMnO亚纳米球催化剂,并研究了不同Mn/Co比对催化剂结构性能及其对苯系挥发性有机化合物(VOCs)氧化催化性能的影响。中空CoMnO亚纳米球对甲苯(T = 265 °C)和邻二甲苯(T = 297 °C)的氧化表现出良好的催化活性,以及优异的循环利用能力和耐水性。通过调节Mn/Co比,金属离子进入不同的四面体或八面体活性位点。与CoO相比,CoMnO表面晶格氧的脱附温度降低了110 °C。这些结果表明,锰的添加可以促进CoMnO上的电子转移,表明引入适量的锰加速了气相O的活化和表面晶格氧物种的迁移,从而加快了苯系VOCs的氧化。

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