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一种柠檬酸辅助沉积策略,用于合成介孔SiO限制的高度分散的LaMnO钙钛矿纳米颗粒用于丁胺催化氧化。

A citric acid-assisted deposition strategy to synthesize mesoporous SiO-confined highly dispersed LaMnO perovskite nanoparticles for -butylamine catalytic oxidation.

作者信息

Chen Huawei, Yang Yanran, Liu Qing, Cui Mifen, Chen Xian, Fei Zhaoyang, Tao Zuliang, Wang Minghong, Qiao Xu

机构信息

State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University Nanjing 210009 PR China

出版信息

RSC Adv. 2019 Mar 14;9(15):8454-8462. doi: 10.1039/c8ra10636c. eCollection 2019 Mar 12.

Abstract

Catalytic oxidation can efficiently eliminate nitrogen-containing volatile organic compounds (NVOCs) and suppress the generation of toxic NO in order to avoid secondary pollution. In this study, mesoporous SiO-confined LaMnO perovskite nanoparticles with high dispersion were successfully prepared by a citric acid-assisted deposition method (LMO/SiO-SD) and tested for the oxidation of -butylamine. The method utilized the synergistic effect of abundant active hydroxyl groups existing on the SiO gel surface and citric acid, rendering the metal ions more uniformly scattered on the SiO surface. Strikingly, the LMO/SiO-SD sample exhibited the optimum catalytic performance ( at 246 °C) and the highest N selectivity, which was mainly ascribed to its abundant surface acid sites, superior low-temperature reducibility and higher ratio of surface Mn species. The apparent activation energy ( ) for -butylamine oxidation over LMO/SiO-SD sample was 29.0 kJ mol. Furthermore, the reaction mechanism of -butylamine oxidation was investigated by FITR and a reasonable reaction route for -butylamine oxidation over the LMO/SiO-SD sample was proposed.

摘要

催化氧化能够有效消除含氮挥发性有机化合物(NVOCs)并抑制有毒NO的生成,以避免二次污染。在本研究中,通过柠檬酸辅助沉积法(LMO/SiO-SD)成功制备了具有高分散性的介孔SiO负载LaMnO钙钛矿纳米颗粒,并对其氧化正丁胺的性能进行了测试。该方法利用了SiO凝胶表面存在的大量活性羟基与柠檬酸的协同作用,使金属离子更均匀地分散在SiO表面。引人注目的是,LMO/SiO-SD样品表现出最佳的催化性能(246℃时转化率为[具体转化率未给出])和最高的N选择性,这主要归因于其丰富的表面酸性位点、优异的低温还原性以及较高的表面Mn物种比例。LMO/SiO-SD样品上正丁胺氧化的表观活化能(Ea)为29.0 kJ/mol。此外,通过傅里叶变换红外光谱(FTIR)研究了正丁胺氧化的反应机理,并提出了LMO/SiO-SD样品上正丁胺氧化的合理反应途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/26fd/9061879/d0c246f56476/c8ra10636c-s1.jpg

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