Intermolecular Interactions in Highly Disordered, Confined Dense N-2

Year: 2017

Authors: Santoro M., Gorelli FA., Bini R., Haines J.

Autors Affiliation: CNR, INO, I-50019 Sesto Fiorentino, Italy; European Lab Non Linear Spect LENS, I-50019 Sesto Fiorentino, Italy; Univ Florence, Dipartimento Chim, I-50019 Sesto Fiorentino, Italy; Univ Montpellier, ENSCM, CNRS, ICGM, F-34090 Montpellier, France.

Abstract: Molecular nitrogen is a benchmark system for condensed matter and, in particular, for looking at universal properties of strongly confined dense systems. We conducted Raman and X-ray diffraction measurements on a dense and disordered form of molecular nitrogen subnanoconfined in a noncatalytic pure SiO2 zeolite under pressure, up to 50 GPa. In this form, N-2-N-2 interactions and, consequently, distances are found to be very dose to those of bulk N-2 and intramolecular interactions progressively weaken upon increasing pressure. Surprisingly, the filled zeolite is still crystalline at 50 GPa with silicon in tetrahedral coordination by oxygen, which is a record pressure for this type of coordination among all the known forms of silica. We have thus found a rationale for the polymerization of a number molecules occurring in the microchannels of noncatalytic zeolites under pressure, where the pressure threshold is found to be very similar to that observed in bulk samples.

Journal/Review: JOURNAL OF PHYSICAL CHEMISTRY LETTERS

Volume: 8 (11)      Pages from: 2406  to: 2411

More Information: We acknowledge the PRIN project ZAPPING, number 2015HK93L7, granted by the Italian Ministry of Education, Universities and Research, MIUR. We are also grateful for the support from PICS bilateral project CNR/CNRS (Italy/France), 2014-2016: Multifunctional zeolite/polymer nano composites. We also thank the Deep Carbon Observatory (DCO) initiative under the project Physics and Chemistry of Carbon at Extreme Conditions and the Ente Cassa di Risparmio di Firenze under the project Firenze Hydrolab 2.
KeyWords: HIGH-PRESSURE SYNTHESIS; SOLID NITROGEN; ATOMIC PHASES; 1 MBAR; GPA; SILICALITE; ZEOLITE; ZSM-5; RAMAN
DOI: 10.1021/acs.jpclett.7b00902

ImpactFactor: 8.709
Citations: 9
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