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

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

doi:10.1002/adfm.201705786

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

Journal Article · 21 January 2018 · Advanced Functional Materials

DOI: https://doi.org/10.1002/adfm.201705786 · OSTI ID:1417701

Gunawan, Maria A. ^[1]; Moncea, Oana ^[1]; Poinsot, Didier ^[2]; Keskes, Mariem ^[2]; Domenichini, Bruno ^[3]; Heintz, Olivier ^[3]; Chassagnon, Rémi ^[3]; Herbst, Frédéric ^[3]; Carlson, Robert M. K. ^[4]; Dahl, Jeremy E. P. ^[4]; Fokin, Andrey A. ^[5];

^[6];

^[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 für Organische Chemie Justus‐Liebig‐Universität Heinrich‐Buff‐Ring 17 35392 Giessen Germany
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
Laboratoire Interdisciplinaire Carnot de Bourgogne (ICB) UMR‐CNRS 6303 Université de Bourgogne Franche‐Comté (UBFC) 9 avenue Alain Savary 21078 Dijon France
Stanford Institute for Materials and Energy Sciences Stanford CA 94305 USA
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
Institut für Organische Chemie Justus‐Liebig‐Universität Heinrich‐Buff‐Ring 17 35392 Giessen Germany
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

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.

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Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; AC02-76SF00515

OSTI ID:: 1417701

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 13 Vol. 28; ISSN 1616-301X

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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Journal Article · 2014 · Journal of Chemical Physics · OSTI ID:22255267

Meinke, Reinhard; Thomsen, Christian; Maultzsch, Janina; +6 more

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

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