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Title: Nanodiamond‐Palladium Core–Shell Organohybrid Synthesis: A Mild Vapor‐Phase Procedure Enabling Nanolayering Metal onto Functionalized sp 3 ‐Carbon

Abstract

Abstract A novel approach for the bottom‐up construction of hybrid organic–inorganic nanocomposites with an intimate arrangement between sp 3 ‐carbon 3D molecular‐size nanodiamonds (diamondoids) and a coated palladium surface as nanolayer is reported. The construction process is conducted stepwisely from the gas phase, using first controlled vapor‐phase self‐assembly of tailor‐made functionalized diamantane derivatives, followed by low‐temperature (45 °C) chemical vapor deposition of an organometallic complex in a reducing H 2 atmosphere over the self‐assembled diamondoid scaffold. The use of self‐assemblies of primary diamantane phosphine and phosphine oxide, which are produced with high structural uniformity and reproducibility, yields new hybrid diamondoid‐palladium materials incorporating PdOPHdiamantane bonding motifs. Additional investigations provide evidence for a very challenging issue in the intimate construction of sp 3 ‐C/metal scaffolds. Scanning electron microscopy and transmission electron microscopy microscopies combined with X‐ray photoelectron spectroscopy surface analysis and EDX bulk analysis confirm the formation of diamondoid‐palladium organohybrids with unique surface layering. The vapor phase‐controlled mild synthetic process allows excellent control over nanocomposite formation and morphology from molecular‐level modifications. As such, this bottom‐up composite building process bridges scales from the molecular (functionalized diamondoids) over nanoscopic (self‐assemblies) to microscopic regime (hybrids), in the challenging association of transition metals with an electronicallymore » saturated sp 3 ‐carbon organic host material.« less

Authors:
 [1];  [1];  [2];  [2];  [3];  [3];  [3];  [3];  [4];  [4];  [5]; ORCiD logo [6]; ORCiD logo [7]
+ Show Author Affiliations
  1. Institut de Chimie Moléculaire de l'Université de Bourgogne (ICMUB) UMR‐CNRS 6302 Université de Bourgogne Franche‐Comté (UBFC) 9 avenue Alain Savary 21078 Dijon France, Institut für Organische Chemie Justus‐Liebig‐Universität Heinrich‐Buff‐Ring 17 35392 Giessen Germany
  2. Institut de Chimie Moléculaire de l'Université de Bourgogne (ICMUB) UMR‐CNRS 6302 Université de Bourgogne Franche‐Comté (UBFC) 9 avenue Alain Savary 21078 Dijon France
  3. Laboratoire Interdisciplinaire Carnot de Bourgogne (ICB) UMR‐CNRS 6303 Université de Bourgogne Franche‐Comté (UBFC) 9 avenue Alain Savary 21078 Dijon France
  4. Stanford Institute for Materials and Energy Sciences Stanford CA 94305 USA
  5. Institut für Organische Chemie Justus‐Liebig‐Universität Heinrich‐Buff‐Ring 17 35392 Giessen Germany, Department of Organic Chemistry Kiev Polytechnic Institute Pr. Pobedy 37 03056 Kiev Ukraine
  6. Institut für Organische Chemie Justus‐Liebig‐Universität Heinrich‐Buff‐Ring 17 35392 Giessen Germany
  7. Institut de Chimie Moléculaire de l'Université de Bourgogne (ICMUB) UMR‐CNRS 6302 Université de Bourgogne Franche‐Comté (UBFC) 9 avenue Alain Savary 21078 Dijon France, Institut Universitaire de France (IUF) 103 Bd. Saint Michel 75005 Paris Cedex 5 France
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1417701
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Name: Advanced Functional Materials Journal Volume: 28 Journal Issue: 13; Journal ID: ISSN 1616-301X
Publisher:
Wiley Blackwell (John Wiley & Sons)
Country of Publication:
Germany
Language:
English

Citation Formats

Gunawan, Maria A., Moncea, Oana, Poinsot, Didier, Keskes, Mariem, Domenichini, Bruno, Heintz, Olivier, Chassagnon, Rémi, Herbst, Frédéric, Carlson, Robert M. K., Dahl, Jeremy E. P., Fokin, Andrey A., Schreiner, Peter R., and Hierso, Jean‐Cyrille. Nanodiamond‐Palladium Core–Shell Organohybrid Synthesis: A Mild Vapor‐Phase Procedure Enabling Nanolayering Metal onto Functionalized sp 3 ‐Carbon. Germany: N. p., 2018. Web. doi:10.1002/adfm.201705786.
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Gunawan, Maria A., Moncea, Oana, Poinsot, Didier, Keskes, Mariem, Domenichini, Bruno, Heintz, Olivier, Chassagnon, Rémi, Herbst, Frédéric, Carlson, Robert M. K., Dahl, Jeremy E. P., Fokin, Andrey A., Schreiner, Peter R., & Hierso, Jean‐Cyrille. Nanodiamond‐Palladium Core–Shell Organohybrid Synthesis: A Mild Vapor‐Phase Procedure Enabling Nanolayering Metal onto Functionalized sp 3 ‐Carbon. Germany. https://doi.org/10.1002/adfm.201705786
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Gunawan, Maria A., Moncea, Oana, Poinsot, Didier, Keskes, Mariem, Domenichini, Bruno, Heintz, Olivier, Chassagnon, Rémi, Herbst, Frédéric, Carlson, Robert M. K., Dahl, Jeremy E. P., Fokin, Andrey A., Schreiner, Peter R., and Hierso, Jean‐Cyrille. Mon . "Nanodiamond‐Palladium Core–Shell Organohybrid Synthesis: A Mild Vapor‐Phase Procedure Enabling Nanolayering Metal onto Functionalized sp 3 ‐Carbon". Germany. https://doi.org/10.1002/adfm.201705786.
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@article{osti_1417701,
title = {Nanodiamond‐Palladium Core–Shell Organohybrid Synthesis: A Mild Vapor‐Phase Procedure Enabling Nanolayering Metal onto Functionalized sp 3 ‐Carbon},
author = {Gunawan, Maria A. and Moncea, Oana and Poinsot, Didier and Keskes, Mariem and Domenichini, Bruno and Heintz, Olivier and Chassagnon, Rémi and Herbst, Frédéric and Carlson, Robert M. K. and Dahl, Jeremy E. P. and Fokin, Andrey A. and Schreiner, Peter R. and Hierso, Jean‐Cyrille},
abstractNote = {Abstract A novel approach for the bottom‐up construction of hybrid organic–inorganic nanocomposites with an intimate arrangement between sp 3 ‐carbon 3D molecular‐size nanodiamonds (diamondoids) and a coated palladium surface as nanolayer is reported. The construction process is conducted stepwisely from the gas phase, using first controlled vapor‐phase self‐assembly of tailor‐made functionalized diamantane derivatives, followed by low‐temperature (45 °C) chemical vapor deposition of an organometallic complex in a reducing H 2 atmosphere over the self‐assembled diamondoid scaffold. The use of self‐assemblies of primary diamantane phosphine and phosphine oxide, which are produced with high structural uniformity and reproducibility, yields new hybrid diamondoid‐palladium materials incorporating PdOPHdiamantane bonding motifs. Additional investigations provide evidence for a very challenging issue in the intimate construction of sp 3 ‐C/metal scaffolds. Scanning electron microscopy and transmission electron microscopy microscopies combined with X‐ray photoelectron spectroscopy surface analysis and EDX bulk analysis confirm the formation of diamondoid‐palladium organohybrids with unique surface layering. The vapor phase‐controlled mild synthetic process allows excellent control over nanocomposite formation and morphology from molecular‐level modifications. As such, this bottom‐up composite building process bridges scales from the molecular (functionalized diamondoids) over nanoscopic (self‐assemblies) to microscopic regime (hybrids), in the challenging association of transition metals with an electronically saturated sp 3 ‐carbon organic host material.},
doi = {10.1002/adfm.201705786},
journal = {Advanced Functional Materials},
number = 13,
volume = 28,
place = {Germany},
year = {Mon Jan 22 00:00:00 EST 2018},
month = {Mon Jan 22 00:00:00 EST 2018}
}
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Diamonds are a Chemist's Best Friend: Diamondoid Chemistry Beyond Adamantane
journal, January 2008

  • Schwertfeger, Hartmut; Fokin, Andrey A.; Schreiner, Peter R.
  • Angewandte Chemie International Edition, Vol. 47, Issue 6
  • DOI: 10.1002/anie.200701684
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