High pressure decomposition of a sandwich compound

Author:

Fanetti Samuele12ORCID,Romi Sebastiano3ORCID,Berretti Enrico1ORCID,Hanfland Michael4ORCID,Mijit Emin4ORCID,Alabarse Frederico5ORCID,Dalladay-Simpson Philip6ORCID,Gorelli Federico236ORCID,Bini Roberto1237ORCID,Santoro Mario23ORCID

Affiliation:

1. Consiglio Nazionale delle Ricerche - Istituto di Chimica dei Composti OrganoMetallici, CNR-ICCOM 1 , Via Madonna del Piano 10, 50019 Sesto Fiorentino, FI, Italy

2. European Laboratory for Nonlinear Spectroscopy, LENS 2 , via Nello Carrara 1, 50019 Sesto Fiorentino, FI, Italy

3. Consiglio Nazionale delle Ricerche - Istituto Nazionale di Ottica, CNR-INO 3 , Via Nello Carrara 1, 50019 Sesto Fiorentino, FI, Italy

4. European Synchrotron Radiation Facility, ESRF 4 , 71 Avenue des Martyrs, CS40220, 38043 Cedex 9 Grenoble, France

5. Elettra Sincrotrone Trieste S.C.p.A, in AREA Science Park 5 , 34149 Basovizza TS, Italy

6. Center for High Pressure Science and Technology Advanced Research 6 , Shanghai 201203, China

7. Dipartimento di Chimica “Ugo Schiff,” Università di Firenze 7 , via della Lastruccia 3, 50019 Sesto Fiorentino, FI, Italy

Abstract

While it is widely recognized that purely organic molecular systems with multiple bonds undergo chemical condensation at sufficiently high pressures (from tenths to tens of GPa), the fate of organometallics at extreme conditions remains largely underexplored. We have investigated the high pressure (up to 41 GPa) chemical transformations in a simple molecular system known as nickelocene, (C5H5)2Ni, which serves as a representative example of a class of organometallics called sandwich compounds. Nickelocene decomposed above 13 GPa, at room temperature, while lower pressure thresholds have been observed at higher temperatures (295–573 K). The products were identified as nanocomposite materials, primarily composed of disordered, nickel-rich nanoparticles segregated within an extended, amorphous matrix of hydrogenated carbon (a-C:H). The investigation was conducted by means of diamond anvil cells in combination with optical spectroscopies and microscopy, synchrotron x-ray absorption spectroscopy and diffraction, as well as transmission electron microscopy. Our findings have the potential to stimulate further research into the high-pressure chemical reactivity of organometallics and open up new synthesis routes for the production of metal-based nanoparticles, which find a wide range of applications.

Publisher

AIP Publishing

Subject

Physical and Theoretical Chemistry,General Physics and Astronomy

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