Revealing the mechanism of high water resistant and excellent active of CuMn oxide catalyst derived from Bimetal-Organic framework for acetone catalytic oxidation.
Revealing the mechanism of high water resistant and excellent active of CuMn oxide catalyst derived from Bimetal-Organic framework for acetone catalytic oxidation.
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DOI：
10.1016/j.jcis.2022.04.155
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发表时间：
2022-04
影响因子：
9.9
通讯作者：
Lei Wang-;Yong-gang Sun;Yinbo Zhu;Juanni Zhang;Jie Ding;Jing Gao;Wen-xin Ji;Yuanyuan Li;Liqiong Wang;Yulong Ma
中科院分区：
文献类型：
--
作者：
Lei Wang-;Yong-gang Sun;Yinbo Zhu;Juanni Zhang;Jie Ding;Jing Gao;Wen-xin Ji;Yuanyuan Li;Liqiong Wang;Yulong Ma
环境水是挥发性有机物(VOCs)低温催化氧化的影响因素，对反应过程和机理有重要影响。本文采用热解法制备了一系列棒状铜锰氧化物，并将其用于丙酮氧化。结果表明，与单相催化相比，多相界面的形成具有更优异的催化性能。这一现象可以归因于多相界面的形成，从而导致合成的催化剂具有更多的活性氧物种和缺陷中心。CuMn2Ox型催化剂具有优良的催化性能(T90=0.150℃)、高耐水性和长期稳定性。此外，漫反射红外光谱和热脱附-气相色谱-质谱联用结果表明，丙酮的降解路径为：丙酮((CH3)2CO*)、→烯醇络合物(CH2)、→-乙醛((CH3CHO*)、→乙酸乙酯(CH3COO*)、→甲酸盐(HCOO*)、→、CO2和H2O。在低温下，水蒸气在多相界面上解离了大量活化的羟基，促进了烯醇络合物和乙醛物种的解离。这种复合氧化物是一种在高湿度条件下脱除含氧VOCs的有前景的催化剂。
Environmental H2O is an influential factor in the low-temperature catalytic oxidation of volatile organic compounds (VOCs), and it significantly impacts the reaction process and mechanism. Here, a series of rod-like Cu-Mn oxides were synthesised by pyrolysing Cu/Mn-BTC for acetone oxidation. The results confirm that the formation of multiphase interfaces have more excellent catalytic performance compared to single-phase catalysis. This phenomenon can be attributed to the formation of multiphase interfaces, which resulted in the synthesized catalysts with more active oxygen species and defective sites. The CuMn2Oxcatalyst exhibited superior catalytic performance (T90= 150 °C), high water resistance and long-term stability. Furthermore,in situdiffuse reflectance infrared Fourier transform spectroscopy and thermal desorption-gas chromatography-mass spectrometry results indicated that the degradation pathway of acetone was as follows: acetone ((CH3)2CO*) → enolate complexes ((CH2) = C(CH3) O*) → acetaldehyde ((CH3CHO*) → acetate (CH3COO*) → formate (HCOO*) → CO2and H2O. At a low-temperature, water vapour dissociated a large number of activated hydroxyl groups on the multiphase interface, which promoted the dissociation of enolate complexes and acetaldehyde species. This composite oxide is a promising catalyst for removing oxygenated VOCs at high humidity.