Density Functional Theory Study on the Re Cluster/HZSM-5 Catalysis for Direct Phenol Synthesis from Benzene and Molecular Oxygen: Active Re Structure and Reaction Mechanism
Density Functional Theory Study on the Re Cluster/HZSM-5 Catalysis for Direct Phenol Synthesis from Benzene and Molecular Oxygen: Active Re Structure and Reaction Mechanism
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DOI：
10.1007/s11244-009-9225-1
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发表时间：
2009-04
影响因子：
3.6
通讯作者：
Takehiko Sasaki;Mizuki Tada;Y. Iwasawa
中科院分区：
文献类型：
--
作者：
Takehiko Sasaki;Mizuki Tada;Y. Iwasawa
通过DFT计算，得到了具有苯和分子氧直接合成苯酚活性的Re簇/HZSM-5催化剂的活性结构模型。与EXAFS分析结果一致，由两个相互共享的稀土八面体组成的间隙N原子组成的re10簇是一种稳定的活性结构。考察了苯、氧原子、分子和苯酚在Re簇上的吸附和行为，得到了苯酚合成的中间态和过渡态能量图，说明了苯酚合成的反应步骤。
DFT calculations have been achieved to obtain a convincing model for the active structure in a Re cluster/HZSM-5 catalyst active for direct phenol synthesis from benzene and molecular oxygen. Re10clusters with interstitial N atoms composed of two Re octahedra edge-shared with each other were concluded as a stable active structure in agreement with the EXAFS analysis. The adsorption and behavior of benzene, oxygen atom and molecule and phenol on the Re cluster were examined to obtain the energy diagram for the phenol synthesis including intermediate and transition states, which explains the reaction steps for the phenol synthesis.