Electrochemiluminescent Ion-Channeling Framework for Membrane Binding and Transmembrane Activity Assays

Anal Chem. 2022 Feb 1;94(4):2154-2162. doi: 10.1021/acs.analchem.1c04593. Epub 2022 Jan 18.

Abstract

Recent upgrades in the electrochemiluminescence (ECL) technique showcased its brilliant knack in probing microscopic biointerfacial events, many of which were actually underlain by the ionotropic membrane processes, yet not being ostensive. Here, by modeling an artificial lipoid-supported porin ensemble, we explore and establish the ECL potency in profiling ion-channel activities. A lipophilic hollowed construct dubbed ZnPC was made out of the dynamic covalent chemistry, and its unique geometry was characterized that configured stoichiometric ECL-emissive units in a cubic stance; while the aliphatic vertices of ZnPC helped it safely snorkel and steadily irradiate in a biofilm fusion. After expounding basic ECL properties, the brightness was traced out in response to halogen contents that was lit up by F-/Cl- but down by Br-/I-. The overall pattern fitted the Langmuir isotherm, from which the membrane-binding strengths of the four were analyzed, compared, and collaterally examined in impedimetrics. On the other hand, one could derive anionic transmembrane kinetics from the time-dependent ECL statistics that pinpointed the ECL signaling via the nanocage-directed mass-transfer pathway. More data mining unveiled an ECL-featured Hofmeister series and the thermodynamic governing force behind all scenes. Finally, combining with halide-selective fluorometry, the synthetic conduit was identified as an ECL symporter. In short, this work develops a novel ECL model for the evaluation of life-mimicking membrane permeation. It might intrigue the outreach of ECL applications in the measurement of diverse surface-confined transient scenarios, e.g., in vitro gated ion or molecule trafficking, which used to be handled by nanopore and electrofluorochromic assays.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Electrochemical Techniques* / methods
  • Luminescent Measurements* / methods
  • Photometry