首页|Synthesis and characterization of iron clusters with an icosahedral[Fe@Fe12]16+ Core
Synthesis and characterization of iron clusters with an icosahedral[Fe@Fe12]16+ Core
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Iron-metal clusters are crucial in a variety of critical biological and material systems,including metalloenzymes,catalysts,and magnetic storage devices.However,a synthetic high-nuclear iron cluster has been absent due to the extreme difficulty in stabilizing species with direct iron-iron bonding.In this work,we have synthesized,crystallized,and characterized a(Tp*)4W4S12(Fe@Fe12)cluster(Tp*=tris(3,5-dimethyl-l-pyrazolyl)borate(1-)),which features a rare trideca-nuclear,icosahedral[Fe@Fe12]cluster core with direct multicenter iron-iron bonding between the interstitial iron(Fei)and peripheral irons(Fep),as well as Fep…Fep ferromagnetic coupling.Quantum chemistry studies reveal that the stability of the cluster arises from the 18-electron shell-closing of the[Fe@Fe 12]16+core,assisted by its bonding interactions with the peripheral tridentate[(Tp*)WS3]4-ligands which possess both S→Fe donation and spin-polarized Fe-W σ bonds.The ground-state electron spin is theoretically predicted to be S=32/2 for the cluster.The existence of low oxidation-state(OS～+1.23)iron in this compound may find interesting applications in magnetic storage,spintronics,redox chemistry,and cluster catalysis.
Gan Xu、Yun-Shu Cui、Xue-Lian Jiang、Cong-Qiao Xu、Jun Li、Xu-Dong Chen
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Jiangsu Collaborative Innovation Center of Biomedical Functional Materials and Jiangsu Key Laboratory of New Power Batteries,School of Chemistry and Materials Science,Nanjing Normal University,Nanjing 210023,China
Department of Chemistry and Guangdong Provincial Key Laboratory of Catalytic Chemistry,Southern University of Science and Technology,Shenzhen 518055,China
Department of Chemistry and Engineering Research Center of Advanced Rare-Earth Materials of Ministry of Education,Tsinghua University,Beijing 100084,China
State Key Laboratory of Coordination Chemistry,Nanjing University,Nanjing 210093,China
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国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家自然科学基金国家重点研发计划国家重点研发计划国家重点研发计划Guangdong Basic and Applied Basic Research FoundationGuangdong Provincial Key Laboratory of CatalysisPriority Academic Program Development of Jiangsu Higher Educational InstitutionsJiangsu Collaborative Innovation Center of Biomedical Functional MaterialsState Key Laboratory of Coordination Chemistry in Nanjing University
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