Facile synthesis of homogeneous hollow microsphere Cu-Mn based catalysts for catalytic oxidation of toluene

Facile synthesis of homogeneous hollow microsphere Cu-Mn based catalysts for catalytic oxidation of toluene
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简便合成均质空心微球铜锰基催化剂用于甲苯催化氧化

DOI:
10.1016/j.chemosphere.2020.125812
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发表时间:
2020
期刊:
影响因子:
8.8
通讯作者:
et al
et al
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Xiao Zhe;Chu Wei;et al

文献摘要

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为了减少甲苯这一臭名昭著的空气污染物的排放,迫切需要增强的甲苯催化燃烧纳米催化剂。不幸的是,目前可获得的材料很少在低于250 °C时具有高催化性能,并且在高温下保持耐用。在此,我们展示了一个快速的盐水解驱动的氧化还原沉淀协议,其中H+捐赠的铜盐的水解被用来启动区域选择性还原KMnO 4通过H2 O2在受控的氧化还原动力学,以组装均匀的混合固溶体空心微球Cu-Mn基结构。多种表征技术揭示了在这种独特的纳米微球中,通过精细调节化学性质,在Cu-Mn块体上成功地产生了丰富的微米级孔。与没有尾孔的致密对应物形成鲜明对比的是,调谐的结晶度、具有不饱和配位的接近的边缘位点、快速氧化还原化学和反应期间增强的气体扩散协同作用以产生显著良好的甲苯氧化,在252 °C下具有完全消除活性,在237 °C下具有T90,并且在严格的反应气氛下具有突出的长期耐久性。我们目前的研究开创了一个可供选择的和易处理的竞技场,以设计用于各种催化实施的多孔氧化物材料。
There emerges an urgent stipulation towards the enhanced toluene catalytic combustion nanocatalysts for whittling down the footprint of toluene, a notorious air pollutant. Unfortunately, Few materials which are currently made accessible both present the high catalytic performance lower than 250 °C and keep durable at elevated temperatures. Herein, we demonstrate an expeditious salt hydrolysis-driven redox-precipitation protocol wherein H+donated by the hydrolysis of copper salt was used to initiate the regioselective reduction of KMnO4by H2O2under controlled redox kinetics in order to assemble the homogeneous mixed solid solution hollow microsphere Cu–Mn-based structure. Manifold characterization technologies unveil that in this unique nanbomicrosphere the abundant microscaled pores are successfully created across Cu–Mn bulks with fine-modulating the chemical properties. In sharp contrast with the compact counterparts without tailed porosity, the tuned crystallinity, accessed edge sites with the unsaturated coordination, fast redox chemistry, and boosted gaseous diffusion during reactions synergize to result in the signally good toluene oxidation, with the complete elimination activity at 252 °C, T90at 237 °C, and prominent long-term durability under the stringent reaction atmospheres. Our current study ushers in an alternative and tractable arena to excogitate the porous oxide materials for multifarious catalysis implementations.