Imperial College London
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ProfessorAronWalsh

Faculty of Engineering, Department of Materials

Chair in Materials Design
 
 
 
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Contact

 

+44 (0)20 7594 1178a.walsh Website

 
 
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Location

 

2.10Royal School of MinesSouth Kensington Campus

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Summary

 

Publications

Citation

BibTex format

@article{Huang:2022:10.1039/d2ta02993f,
author = {Huang, J and Golomb, MJ and Kavanagh, SR and Tolborg, K and Ganose, AM and Walsh, A},
doi = {10.1039/d2ta02993f},
journal = {Journal of Materials Chemistry A},
pages = {13500--13507},
title = {Band gap opening from displacive instabilities in layered covalent-organic frameworks},
url = {http://dx.doi.org/10.1039/d2ta02993f},
volume = {10},
year = {2022}
}
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RIS format (EndNote, RefMan)

TY  - JOUR
AB  - Covalent organic frameworks (COFs) offer a high degree of chemical and structural flexibility. There is a large family of COFs built from 2D sheets that are stacked to form extended crystals. While it has been common to represent the stacking as eclipsed with one repeating layer (“AA”), there is growing evidence that a more diverse range of stacking sequences is accessible. Herein, we report a computational study using density functional theory of layer stacking in two prototypical COFs, Tp-Azo and DAAQ-TFP, which have shown high performance as Li-ion battery electrodes. We find a striking preference for slipped structures with horizontal offsets between layers ranging from 1.7 Å to 3.5 Å in a potential energy minimum that forms a low energy ring. The associated symmetry breaking results in a pronounced change in the underlying electronic structure. A band gap opening of 0.8–1.4 eV is found due to modifications of the underlying valence and conduction band dispersion as explained from changes in the π orbital overlap. The implications for the screening and selection of COF for energy applications are discussed.
AU  - Huang,J
AU  - Golomb,MJ
AU  - Kavanagh,SR
AU  - Tolborg,K
AU  - Ganose,AM
AU  - Walsh,A
DO  - 10.1039/d2ta02993f
EP  - 13507
PY  - 2022///
SN  - 2050-7488
SP  - 13500
TI  - Band gap opening from displacive instabilities in layered covalent-organic frameworks
T2  - Journal of Materials Chemistry A
UR  - http://dx.doi.org/10.1039/d2ta02993f
UR  - https://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000812304200001&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=1ba7043ffcc86c417c072aa74d649202
UR  - https://pubs.rsc.org/en/content/articlelanding/2022/TA/D2TA02993F
UR  - http://hdl.handle.net/10044/1/99159
VL  - 10
ER  -
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