Influence of graphene on the electronic and magnetic properties of an iron(III) porphyrin chloride complex

被引:0
|
作者
Song, Young-Joon [1 ]
Gallenkamp, Charlotte [2 ]
Lleopart, Genis [3 ,4 ]
Krewald, Vera [2 ]
Valenti, Roser [1 ]
机构
[1] Goethe Univ Frankfurt, Inst Theoret Phys, Max von Laue Str 1, D-60438 Frankfurt, Germany
[2] Dept Chem, Quantum Chem, Peter Grunberg Str 4, D-64287 Darmstadt, Germany
[3] Univ Barcelona, Dept Ciencia Mat & Quim Fis, C Marti i Franques 1-11, Barcelona 08028, Spain
[4] Univ Barcelona, Inst Quim Teor & Computac IQTC, C Marti i Franques 1-11, Barcelona 08028, Spain
关键词
DENSITY-FUNCTIONAL THEORY; N-C CATALYSTS; GROUND-STATE; IRON; INTERMEDIATE; REDUCTION; SITES;
D O I
10.1039/d4cp01551g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Although iron-based single atom catalysts are regarded as a promising alternative to precious metal catalysts, their precise electronic structures during catalysis still pose challenges for computational descriptions. A particularly urgent issue to be addressed is the influence of the environment on the electronic structure, and how to describe this accurately using computational methods. Here, we study an iron porphyrin chloride complex adsorbed on a graphene sheet using density functional theory calculations to probe how much the electronic structure is influenced by the presence of a graphene layer. Our results indicate that weak interactions due to van der Waals forces dominate between the porphyrin complex and graphene, and only a small amount of charge is transferred between the two entities. Furthermore, the interplay of the ligand field environment, strong p-d hybridization, and correlation effects within the complex are strongly involved in determining the spin state of the iron ion. By bridging molecular chemistry and solid state physics, this study provides first steps towards a joint analysis of the properties of iron-based catalysts from first principles.
引用
收藏
页码:26370 / 26376
页数:7
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