| 宋卫余,杨敏,王林哲.异金属铜-氧MAZ分子筛催化甲烷部分氧化反应DFT研究[J].分子催化,2021,35(5):404-414 |
| 异金属铜-氧MAZ分子筛催化甲烷部分氧化反应DFT研究 |
| Hetero-metallic Cu-MAZ Catalyzed Methane Partial Oxidation: A DFT Study |
| 投稿时间：2021-07-15 修订日期：2021-09-14 |
| DOI：10.16084/j.issn1001-3555.2021.05.002 |
| 中文关键词: 甲烷部分氧化 铜交换分子筛 MAZ分子筛 异金属 描述符 |
| 英文关键词:methane partial oxidation copper-exchanged zeolite MAZ zeolite hetero metals descriptors |
| 基金项目:国家自然科学基金（22178381，22035009） |
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| 中文摘要: |
| 已有研究证明了Cu-MAZ分子筛催化甲烷部分氧化的优异性且实验表征得出其活性结构含有三核铜结构.为进一步提高部分氧化活性，采用MAZ分子筛作为载体体系，用于［Cu3（μ-O）3］2+结构，分别掺杂Pd、Pt、Fe、Co、Ni、Au和Ag，构建［Cu2MO3］2+异金属活性位.通过密度泛函理论（DFT）研究不同金属对Cu-MAZ催化甲烷部分氧化反应的能量变化和反应活性的影响，并分析了活性位、反应中间体、过渡态等结构的几何和电子结构性质，根据以上结果进一步得到描述符. |
| 英文摘要: |
| The excellent methanol yield of methane partial oxidation catalyzed by Cu-MAZ zeolite were reported in previous experimental studies, and the structures of its active site contained di-nuclear and tri-nuclear copper based on experimental characterization. To further enhance the activity of partial oxidation, this study uses MAZ zeolite as the carrier system for[Cu3(μ-O)3]2+ structure. Active structures are doped with Pd, Pt, Fe, Co, Ni, Au and Ag to construct[Cu23]2+ hetero-metallic active sites. Through Density Functional Theory (DFT) to study the effect of different metals in the active sites on the energy changes and reaction activity of methane partial oxidation catalyzed by Cu-zeolite, and the geometric and electronic structural properties of active sites, reaction intermediates, transition states and other structures are analyzed. The descriptors are further obtained based on the above results. The calculation results give the law between catalytic reaction activity and active site properties in the catalytic system. Proton affinity is proved to be the most reliable descriptor of Cu-MAZ catalyzed methane partial oxidation. |
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