Wilding, Martin C;
Benmore, Chris;
Headen, Thomas F;
Di Mino, Camilla;
Miller, Thomas S;
Suter, Theo M;
Corà, Furio;
... Howard, Christopher A; + view all
(2023)
The local ordering of polar solvents around crystalline carbon nitride nanosheets in solution.
Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences
, 381
(2259)
10.1098/rsta.2022.0337.
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Abstract
The crystalline graphitic carbon nitride, poly-triazine imide (PTI) is highly unusual among layered materials since it is spontaneously soluble in aprotic, polar solvents including dimethylformamide (DMF). The PTI material consists of layers of carbon nitride intercalated with LiBr. When dissolved, the resulting solutions consist of dissolved, luminescent single to multilayer nanosheets of around 60–125 nm in diameter and Li+ and Br− ions originating from the intercalating salt. To understand this unique solubility, the structure of these solutions has been investigated by high-energy X-ray and neutron diffraction. Although the diffraction patterns are dominated by inter-solvent correlations there are clear differences between the X-ray diffraction data of the PTI solution and the solvent in the 4–6 Å −1 range, with real space differences persisting to at least 10 Å. Structural modelling using both neutron and X-ray datasets as a constraint reveal the formation of distinct, dense solvation shells surrounding the nanoparticles with a layer of Br − close to the PTI-solvent interface. This solvent ordering provides a configuration that is energetically favourable underpinning thermodynamically driven PTI dissolution. This article is part of the theme issue 'Exploring the length scales, timescales and chemistry of challenging materials (Part 2)'.
| Type: | Article |
|---|---|
| Title: | The local ordering of polar solvents around crystalline carbon nitride nanosheets in solution |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1098/rsta.2022.0337 |
| Publisher version: | https://doi.org/10.1098/rsta.2022.0337 |
| Language: | English |
| Additional information: | © 2023 The Authors. Published by the Royal Society under the terms of the Creative Commons Attribution License http://creativecommons.org/licenses/by/4.0/, which permits unrestricted use, provided the original author and source are credited. |
| Keywords: | neutron diffraction, solvent ordering, liquid structure, carbon nitride, high-energy X-ray diffraction |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10176732 |
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