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镧改性的具有类珊瑚分级结构纳米球的氧化锰对甲苯的增强催化氧化

Enhanced Catalytic Oxidation of Toluene over Manganese Oxide Modified by Lanthanum with a Coral-Like Hierarchical Structure Nanosphere.

作者信息

Li Mingyang, Zhang Cheng, Fan Liman, Lian Yongfu, 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, P. R. China.

出版信息

ACS Appl Mater Interfaces. 2021 Mar 3;13(8):10089-10100. doi: 10.1021/acsami.0c22297. Epub 2021 Feb 16.

Abstract

Coral-like lanthanum manganese oxides (LaMnO) with a hierarchical structure nanosphere were successfully prepared using a simple method, which presented a high-efficiency catalytic performance for toluene combustion. Among them, LaMnO with the MnO phase exhibits superior catalytic activity, such as a lower value (218 °C), excellent HO resistance, and catalytic stability. The effects of La addition on the bulk and surface physicochemical properties of LaMnO were investigated by sorts of characterization including X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N adsorption-desorption, temperature-programmed reduction with H, temperature-programmed desorption of O, X-ray photoelectron spectroscopy, and so forth. The results demonstrate that the doping of La can induce the variation of physicochemical properties and the formation of more surface oxygen species and high valence state amorphous manganese oxides, improving low-temperature reducibility, which facilitates good catalytic activity for LaMnO. A series of in situ diffuse reflectance infrared Fourier transform spectroscopy experiments for toluene adsorption were performed on the LaMnO catalyst pretreated under different atmosphere conditions to investigate the role of oxygen species and the reaction processes. The results indicate that the abundant surface oxygen species over LaMnO can make the rapid formation of benzoic acid species, further transfer into CO and HO, which is considered as the key factor in the activation and oxidation of toluene.

摘要

采用一种简单的方法成功制备了具有分级结构纳米球的珊瑚状镧锰氧化物(LaMnO),其对甲苯燃烧表现出高效的催化性能。其中,具有MnO相的LaMnO表现出优异的催化活性,如较低的 值(218℃)、出色的抗HO性能和催化稳定性。通过X射线衍射、扫描电子显微镜、透射电子显微镜、N吸附-脱附、H程序升温还原、O程序升温脱附、X射线光电子能谱等多种表征手段,研究了La添加对LaMnO体相和表面物理化学性质的影响。结果表明,La的掺杂可引起物理化学性质的变化,形成更多的表面氧物种和高价态无定形锰氧化物,提高低温还原性,从而有利于LaMnO具有良好的催化活性。对在不同气氛条件下预处理的LaMnO催化剂进行了一系列甲苯吸附的原位漫反射红外傅里叶变换光谱实验,以研究氧物种的作用和反应过程。结果表明,LaMnO上丰富的表面氧物种可使苯甲酸物种快速形成,进一步转化为CO和HO,这被认为是甲苯活化和氧化的关键因素。

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