用于褐煤加氢裂解的铁硫化物催化剂结构与电子态的理论研究

曹东波 董梅

摘 要：采用九种DFT方法搭配七种基组对FeS0/-、FeS20/-、Fe2S20/-、Fe3S40/-和Fe4S40/- 进行了系统的研究。通过对比，发现B3LYP和B3PW91搭配6-311+G*和QZVP基组计算的绝热电子亲和能（AEA）与实验值吻合的很好。采用B3LYP/6-311+G*计算了，确定了以上各团簇结构的基态电子态；发现其中，Fe2S2、Fe3S4、Fe3S4-、Fe4S4和Fe4S4-具有反铁磁性。同时用自然价键轨道理论（NBO）对团簇的磁性进行了分析。

关键词：铁硫团簇；密度泛函理论；磁性

Abstract：The structures and energies of the electronic ground states of the FeS0/-， FeS20/-， Fe2S20/-， Fe3S40/- and Fe4S40/- neutral and anionic clusters have been computed systematically with nine computational methods in combination with seven basis sets in this thesis. The computed adiabatic electronic affinities （AEA） have been compared with the available experimental data. Most reasonable agreements between theory and experiment have been found for both hybrid B3LYP and B3PW91 functional in conjugation with the 6-311+G* and QZVP basis sets. Detailed comparisons between the available experimental and computed AEA data at B3LYP/6-311+G* identify the electronic ground state for the clusters involved. In addition， Fe2S2， Fe3S4， Fe3S4-， Fe4S4， and Fe4S4- are found to be antiferromagnetic at B3LYP/6-311+G* level. The magnetic properties have been discussed on the basis of natural bond orbital analysis.

Key word：Iron-sulfur Clusters；DFT；Magnetism

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