Silica-surface reorganization during organotin grafting evidenced by 119Sn DNP SENS: a tandem reaction of gem-silanols and strained siloxane bridges

Literature Information

Publication Date 2014-06-12
DOI 10.1039/C4CP01973C
Impact Factor 3.676
Authors

Matthew P. Conley, Aaron J. Rossini, Aleix Comas-Vives, Maxence Valla, Gilles Casano, Olivier Ouari, Paul Tordo, Anne Lesage, Lyndon Emsley, Christophe Copéret


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Abstract

Grafting reactive molecular complexes on dehydroxylated amorphous silica is a strategy to develop “single-site” heterogeneous catalysts. In general, only the reactivity of isolated silanols is invoked for silica dehydroxylated at 700 °C ([SiO2-700]), though ca. 10% of the surface silanols are in fact geminal Q2-silanols. Here we report the reaction of allyltributylstannane with [SiO2-700] and find that the geminal Q2-silanols react to form products that would formally arise from vicinal Q3-silanols that are not present on [SiO2-700], indicating that a surface rearrangement occurs. The reorganization of the silica surface is unique to silica dehydroxylated at 700 °C or above. The findings were identified using Dynamic Nuclear Polarization Surface Enhanced NMR Spectroscopy (DNP SENS) combined with DFT calculations.

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Inside front cover

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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