Self-Supporting Metal-Organic Layers as Single-Site Solid Catalysts

Journal Article · Tue Mar 08 00:00:00 EST 2016 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.201512054· OSTI ID:1330242

Cao, Lingyun ^[1]; Lin, Zekai ^[2]; Peng, Fei ^[3]; Wang, Weiwei ^[1]; Huang, Ruiyun ^[1]; Wang, Cheng  ^[1]; Yan, Jiawei ^[1]; Liang, Jie ^[3]; Zhang, Zhiming ^[1]; Zhang, Teng ^[2]; Long, Lasheng ^[1]; Sun, Junliang ^[4]; Lin, Wenbin ^[5]

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1. College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen 361005 China
2. Department of Chemistry, University of Chicago, Chicago IL 60637 USA
3. Berzelii Center EXCELLENT on Porous Materials, Department of Materials and Environmental Chemistry, Stockholm University, 10691 Stockholm Sweden
4. Berzelii Center EXCELLENT on Porous Materials, Department of Materials and Environmental Chemistry, Stockholm University, 10691 Stockholm Sweden; College of Chemistry and Molecular Engineering, Peking University, 100871 Beijing China
5. College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen 361005 China; Department of Chemistry, University of Chicago, Chicago IL 60637 USA

Metal–organic layers (MOLs) represent an emerging class of tunable and functionalizable two-dimensional materials. In this work, the scalable solvothermal synthesis of self-supporting MOLs composed of [Hf₆O₄(OH)₄(HCO₂)₆] secondary building units (SBUs) and benzene-1,3,5-tribenzoate (BTB) bridging ligands is reported. The MOL structures were directly imaged by TEM and AFM, and doped with 4'-(4-benzoate)-(2,2',2''-terpyridine)-5,5''-dicarboxylate (TPY) before being coordinated with iron centers to afford highly active and reusable single-site solid catalysts for the hydrosilylation of terminal olefins. MOL-based heterogeneous catalysts are free from the diffusional constraints placed on all known porous solid catalysts, including metal–organic frameworks. This work uncovers an entirely new strategy for designing single-site solid catalysts and opens the door to a new class of two-dimensional coordination materials with molecular functionalities.

• Research Organization: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
• Sponsoring Organization: USDOE
• OSTI ID: 1330242
• Journal Information: Angewandte Chemie (International Edition), Vol. 55, Issue 16; ISSN 1433-7851
• Publisher: Wiley
• Country of Publication: United States
• Language: ENGLISH

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY