Issue 16, 2022

Development of a novel theory of pressure-induced nucleation in supercritical carbon dioxide

Abstract

Nucleation is the basis of the fabrication of two-dimensional materials in the bottom-up methods such as chemical vapor deposition and atomic layer deposition. Supercritical fluid deposition (SCFD) might provide an alternative to these techniques owing to the excellent physicochemical properties and adjustable solvent power of supercritical fluids. However, classical nucleation theory (CNT) was not suitable for the nucleation in supercritical fluid (SCF) because of the non-ideality of SCF. Herein, a dilute solution system composed of a nonvolatile solute and supercritical CO2 (scCO2) was established and the theory of pressure-induced supercritical phase nucleation (PI-SCPN) was proposed. A newly defined solute–solvent correlation function was found to influence the nucleation driving force a lot in this particular process, especially when the supersaturation was small. It was also found that at high temperature and high pressure, the barrier of nucleation was low, which was conducive to the formation of a nucleus. Furthermore, the corresponding experiments were conducted using MoO2(acac)2 as the solute and scCO2 as the solvent to verify the proposed theory. The solubility of MoO2(acac)2 was accurately measured by the static equilibrium method. The influence of supersaturation, temperature and pressure on nucleation was found to be consistent with that predicted using the proposed theory. The nucleation rates calculated by PI-SCPN were compared to the experimental values, showing good agreement, and the errors were within one order of magnitude.

Graphical abstract: Development of a novel theory of pressure-induced nucleation in supercritical carbon dioxide

Supplementary files

Article information

Article type
Paper
Submitted
10 Feb 2022
Accepted
16 Mar 2022
First published
17 Mar 2022

CrystEngComm, 2022,24, 3035-3048

Development of a novel theory of pressure-induced nucleation in supercritical carbon dioxide

Q. Wang, Q. Xu, J. Yin, H. Zhu, B. Liu and M. Yang, CrystEngComm, 2022, 24, 3035 DOI: 10.1039/D2CE00187J

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements