en
Scientific article
English

On the Importance of Intermediate Internal Charge Repulsion for the Synthesis of Multifunctional Pores

Published inHelvetica chimica acta, vol. 85, no. 9, p. 2740-2753
Publication date2002
Abstract

Intermediate internal charge repulsion (ICR) is required to create synthetic pores with large, stable, transmembrane, and variably functionalized space. This conclusion is drawn from maximal transport and, in one case, catalytic activity of p-octiphenyl ß-barrel pores with internal lysine, aspartate, and histidine residues around pH 7, 6, and 4.5, respectively. pKa Simulations corroborate the experimental correlation of intermediate ICR with activity and suggest that insufficient ICR causes pore implosion' and excess ICR pore explosion'. Esterolysis experiments support the view that the formation of stable space within multifunctional p-octiphenyl ß-barrels requires more ICR in bilayer membranes than in H2O. Multivalency effects are thought to account for p-octiphenyl ß-barrel expansion with increasing number of ß-sheets, and proximity effects for unchanged pH profiles with increasing ß-sheet length. Q-TOF-nano-ESI-MS barrel-denaturation experiments indicate that contributions from internal counterion effects are not negligible. The overall characteristics of p-octiphenyl ß-barrel pores with internal lysine, aspartate, and histidine residues, unlike de novo a-barrels' and similarly to certain biological channels, underscore the usefulness of rigid-rod molecules to preorganize complex multifunctional supramolecular architecture.

Citation (ISO format)
BAUMEISTER, Bodo et al. On the Importance of Intermediate Internal Charge Repulsion for the Synthesis of Multifunctional Pores. In: Helvetica chimica acta, 2002, vol. 85, n° 9, p. 2740–2753. doi: 10.1002/1522-2675(200209)85:9<2740::AID-HLCA2740>3.0.CO;2-C
Main files (1)
Article
accessLevelRestricted
ISSN of the journal0018-019X
457views
0downloads

Technical informations

Creation06/21/2010 10:28:00 AM
First validation06/21/2010 10:28:00 AM
Update time03/14/2023 3:46:52 PM
Status update03/14/2023 3:46:52 PM
Last indexation02/12/2024 6:42:57 PM
All rights reserved by Archive ouverte UNIGE and the University of GenevaunigeBlack