Boosting total oxidation of acetone over spinel MCo2O4 (M = Co, Ni, Cu) hollow mesoporous spheres by cation-substituting effect.
Boosting total oxidation of acetone over spinel MCo2O4 (M = Co, Ni, Cu) hollow mesoporous spheres by cation-substituting effect.
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DOI：
10.1016/j.jcis.2018.12.061
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发表时间：
2019-03
影响因子：
9.9
通讯作者：
Chi Zhang;Jinguo Wang;S. Yang;Hao Liang;Yong Men
中科院分区：
文献类型：
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作者：
Chi Zhang;Jinguo Wang;S. Yang;Hao Liang;Yong Men
通过阳离子取代效应促进挥发性有机物（VOCs）在尖晶石型Co3O4上的完全氧化是一种有效的解决方案，但其机理尚未完全阐明。本文采用溶剂热醇解法合成了一系列尖晶石型MCo2O4（M = Co，Ni，Cu）中空介孔球（HMS），旨在研究阳离子取代对尖晶石型Co3O4催化氧化VOCs的影响。对尖晶石型MCo_2O_4（M = Co，Ni，Cu）HMS的物化性质进行了表征，并与其催化活性进行了关联。结果表明，CuCo 2 O 4 HMS对丙酮完全氧化的催化活性优于NiCo 2 O 4和CoCo 2 O 4 HMS，其催化活性大小顺序为CuCo 2 O 4> NiCo 2 O 4> CoCo 2 O 4。上级。这种现象可以归因于阳离子取代效应，这导致合成的催化剂具有不同数量的表面Co3+阳离子、活性氧物种、缺陷位和还原能力。同时，动力学研究为阳离子取代效应在催化剂活性中起决定性作用提供了直接证据，并通过构效关系的关联提出了其机理。此外，CuCo2O4HMS由于其高度稳定的晶相和坚固的形态结构，还表现出优异的长期稳定性和良好的耐水性，显示了其在VOCs去除领域的潜在应用。
Boosting total oxidation of volatile organic compounds (VOCs) over spinel Co3O4by cation-substituting effect is an effective solution, but the underlying mechanism has not yet been clearly elucidated. Herein, a series of spinel MCo2O4(M = Co, Ni, Cu) hollow mesoporous spheres (HMS) have been synthesized by solvothermal alcoholysis with goals to elaborate the cation-substituting effect on spinel Co3O4for total oxidation of VOCs. The physicochemical properties of spinel MCo2O4(M = Co, Ni, Cu) HMS have been well characterized and correlated with their catalytic activities. Results reveal that CuCo2O4HMS exhibited superior catalytic activity than those of NiCo2O4and CoCo2O4HMS for total oxidation of acetone and their catalytic activities followed the sequence of CuCo2O4> NiCo2O4> CoCo2O4. This phenomenon can be attributed to the cation-substituting effect, which resulted in the synthesized catalysts with different amounts of surface Co3+cations, active oxygen species, defective sites and reducible capabilities. Meanwhile, kinetics studies offer direct evidence to support that the cation-substituting effect played the decisive role in determining the catalytic activity, and the underlying mechanism has been proposed by correlating the structure-activity relationship. Moreover, CuCo2O4HMS also showed excellent long-term stability and good water tolerance due to its highly stable crystal phase and robust morphological structure, demonstrating its potential applications in the field of VOCs elimination.