Three-Dimensional Structure Determination of Surface Sites

被引：79

作者：

Berruyer, Pierrick ^{[1
]}

Lelli, Moreno ^{[2
]}

Conley, Matthew P. ^{[3
,6
]}

Silverio, Daniel L. ^{[3
]}

Widdifield, Cory M. ^{[4
]}

Siddiqi, Georges ^{[3
]}

Gajan, David ^{[1
]}

Lesage, Anne ^{[1
]}

Coperet, Christophe ^{[3
]}

Emsley, Lyndon ^{[5
]}

机构：

[1] Univ Lyon 1, Ctr RMN Tres Hauts Champs, Inst Sci Analyt UMR 5280, CNRS,ENS Lyon, F-69100 Villeurbanne, France

[2] Univ Florence, Magnet Resonance Ctr CERM, I-50019 Sesto Fiorentino, FI, Italy

[3] Swiss Fed Inst Technol, Dept Chem & Appl Biosci, CH-8037 Zurich, Switzerland

[4] Univ Durham, Dept Chem, Durham DH1 3LE, England

[5] Ecole Polytech Fed Lausanne, Inst Sci & Ingn Chim, CH-1015 Lausanne, Switzerland

[6] Univ Calif Riverside, Dept Chem, Riverside, CA 92521 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2017年 / 139卷 / 02期

关键词：

DYNAMIC NUCLEAR-POLARIZATION; ENHANCED NMR-SPECTROSCOPY; ROTATIONAL-ECHO; SILICA; CATALYSTS; RESONANCE; APPROXIMATION; NANOPARTICLES; EFFICIENT; SOLVENTS;

D O I：

10.1021/jacs.6b10894

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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 angstrom. 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.

引用

页码：849 / 855

页数：7

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[11]

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[12] Tunable gold catalysts for selective hydrocarbon oxidation under mild conditions [J].