title: Self-Supporting Metal-Organic Layers as Single-Site Solid Catalysts.
abstract: 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.
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China.
authors.forename: Lingyun
authors.initials: L
authors.lastname: Cao
authors.affiliation: Department of Chemistry, University of Chicago, Chicago, IL, 60637, USA.
authors.forename: Zekai
authors.initials: Z
authors.lastname: Lin
authors.affiliation: Berzelii Center EXCELLENT on Porous Materials, Department of Materials and Environmental Chemistry, Stockholm University, 10691, Stockholm, Sweden.
authors.forename: Fei
authors.initials: F
authors.lastname: Peng
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China.
authors.forename: Weiwei
authors.initials: W
authors.lastname: Wang
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China.
authors.forename: Ruiyun
authors.initials: R
authors.lastname: Huang
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China. wangchengxmu@xmu.edu.cn.
authors.forename: Cheng
authors.identifier: http://orcid.org/0000-0002-7906-8061
authors.initials: C
authors.lastname: Wang
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China.
authors.forename: Jiawei
authors.initials: J
authors.lastname: Yan
authors.affiliation: Berzelii Center EXCELLENT on Porous Materials, Department of Materials and Environmental Chemistry, Stockholm University, 10691, Stockholm, Sweden.
authors.forename: Jie
authors.initials: J
authors.lastname: Liang
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China.
authors.forename: Zhiming
authors.initials: Z
authors.lastname: Zhang
authors.affiliation: Department of Chemistry, University of Chicago, Chicago, IL, 60637, USA.
authors.forename: Teng
authors.initials: T
authors.lastname: Zhang
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China.
authors.forename: Lasheng
authors.initials: L
authors.lastname: Long
authors.affiliation: Berzelii Center EXCELLENT on Porous Materials, Department of Materials and Environmental Chemistry, Stockholm University, 10691, Stockholm, Sweden. junliang.sun@pku.edu.cn.|College of Chemistry and Molecular Engineering, Peking University, 100871, Beijing, China. junliang.sun@pku.edu.cn.
authors.forename: Junliang
authors.initials: J
authors.lastname: Sun
authors.affiliation: College of Chemistry and Chemical Engineering, iCHEM, PCOSS, Xiamen University, Xiamen, 361005, China. wenbinlin@uchicago.edu.|Department of Chemistry, University of Chicago, Chicago, IL, 60637, USA. wenbinlin@uchicago.edu.
authors.forename: Wenbin
authors.initials: W
authors.lastname: Lin
keywords: alkenes; hafnium; heterogeneous catalysis; hydrosilylation; metal-organic layers