Investigation into the Enhanced Catalytic Oxidation of o-Xylene over MOF-Derived Co3O4 with Different Shapes: The Role of Surface Twofold-Coordinate Lattice Oxygen (O-2f)
文献类型：期刊论文
| 作者 | Ma, Ying; Wang, Lian; Ma, Jinzhu; Wang, Honghong; Zhang, Changbin; Deng, Hua; He, Hong
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| 刊名 | ACS CATALYSIS
 |
| 出版日期 | 2021-06-04 |
| 卷号 | 11期号:11页码:6614-6625 |
| 关键词 | MOF-derived Co3O4 VOC oxidation mechanism twofold-coordinate lattice oxygen in situ DRIFTS DFT calculations |
| ISSN号 | 2155-5435 |
| 英文摘要 | In the removal of volatile organic compounds (VOCs), Co3O4 catalysts with various morphologies are highly efficient due to rich active sites such as Co3+, adsorbed oxygen, and surface lattice oxygen species. It is worthwhile further disclosing the crucial roles and reaction mechanism of these active sites. The facile and uniform metal-organic framework (MOF) derivation method was selected to synthesize Co3O4 catalysts with different shapes for the catalytic oxidation of o-xylene: rod-like Co3O4-R exhibited a lower T-90% of 270 degrees C, superior stability, and water resistance compared with spherical Co3O4-S. The enhanced catalytic performance of Co3O4-R probably originated from its more active surface lattice oxygen, namely, twofold-coordinate lattice oxygen (O-2f), on exposed (220) planes, which gave rise to larger CO2 generation as revealed by HR-TEM, O-2-TPD, and o-xylene-TPD. In situ DRIFTS study also showed that Co3O4-R adsorbed and oxidized more oxylene via surface O-2f, forming intermediates including alkoxide, carboxylate, and anhydride species and leaving oxygen vacancy. After the introduction of gaseous oxygen, the disappearance of intermediates occurred more rapidly on Co3O4-R owing to the good oxygen mobility. The lower formation energy of oxygen vacancy (E-Ov, 2.61 eV) and higher adsorption energy of oxygen (E-ads,E-O2, -1.71 eV) on Co3O4-R theoretically confirmed the easier oxygen vacancy formation and gaseous oxygen replenishment on Co3O4-R due to the existence of active O-2f on the surface. Therefore, the role of surface O-2f in oxygen vacancy formation and gaseous oxygen replenishment crucially contributed to the enhanced catalytic oxidation of o-xylene over MOF-derived Co3O4 catalysts with different shapes. This study might shed light on the thorough understanding of active oxygen species in VOC catalytic oxidation and the preparation of efficient catalysts with various morphologies. |
| WOS研究方向 | Chemistry, Physical |
| 源URL | [http://ir.rcees.ac.cn/handle/311016/46050]  |
| 专题 | 生态环境研究中心_水污染控制实验室 |
| 作者单位 | 1.Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China 3.Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China |
| 推荐引用方式 GB/T 7714 | Ma, Ying,Wang, Lian,Ma, Jinzhu,et al. Investigation into the Enhanced Catalytic Oxidation of o-Xylene over MOF-Derived Co3O4 with Different Shapes: The Role of Surface Twofold-Coordinate Lattice Oxygen (O-2f)[J]. ACS CATALYSIS,2021,11(11):6614-6625. |
| APA | Ma, Ying.,Wang, Lian.,Ma, Jinzhu.,Wang, Honghong.,Zhang, Changbin.,...&He, Hong.(2021).Investigation into the Enhanced Catalytic Oxidation of o-Xylene over MOF-Derived Co3O4 with Different Shapes: The Role of Surface Twofold-Coordinate Lattice Oxygen (O-2f).ACS CATALYSIS,11(11),6614-6625. |
| MLA | Ma, Ying,et al."Investigation into the Enhanced Catalytic Oxidation of o-Xylene over MOF-Derived Co3O4 with Different Shapes: The Role of Surface Twofold-Coordinate Lattice Oxygen (O-2f)".ACS CATALYSIS 11.11(2021):6614-6625. |
入库方式： OAI收割
来源：生态环境研究中心
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