The spatial arrangement of atoms is directly linked to chemical function. A fundamental challenge in surface chemistry and catalysis relates to the determination of three-dimensional structures with atomic-level precision. Here we determine the three-dimensional structure of an organometallic complex on an amorphous silica surface using solid-state NMR measurements, enabled through a dynamic nuclear polarization surface enhanced NMR spectroscopy approach that induces a 200-fold increase in the NMR sensitivity for the surface species. The result, in combination with EXAFS, is a detailed structure for the surface complex determined with a precision of 0.7 Å. We observe a single well-defined conformation that is folded toward the surface in such a way as to include an interaction between the platinum metal center and the surface oxygen atoms.
Three-Dimensional Structure Determination of Surface Sites / Berruyer, Pierrick; Lelli, Moreno; Conley, Matthew P; Silverio, Daniel L; Widdifield, Cory M; Siddiqi, Georges; Gajan, David; Lesage, Anne; Copéret, Christophe; Emsley, Lyndon. - In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. - ISSN 0002-7863. - STAMPA. - 139:(2017), pp. 849-855. [10.1021/jacs.6b10894]
Three-Dimensional Structure Determination of Surface Sites
LELLI, MORENOInvestigation
;
2017
Abstract
The spatial arrangement of atoms is directly linked to chemical function. A fundamental challenge in surface chemistry and catalysis relates to the determination of three-dimensional structures with atomic-level precision. Here we determine the three-dimensional structure of an organometallic complex on an amorphous silica surface using solid-state NMR measurements, enabled through a dynamic nuclear polarization surface enhanced NMR spectroscopy approach that induces a 200-fold increase in the NMR sensitivity for the surface species. The result, in combination with EXAFS, is a detailed structure for the surface complex determined with a precision of 0.7 Å. We observe a single well-defined conformation that is folded toward the surface in such a way as to include an interaction between the platinum metal center and the surface oxygen atoms.File | Dimensione | Formato | |
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