Issue 33, 2024

Fluorinated polymer zwitterions on gold nanoparticles: patterned catalyst surfaces guide interfacial transport and electrochemical CO2 reduction

Abstract

We report the use of fluorinated polymer zwitterions to build hybrid systems for efficient CO2 electroreduction. The unique combination of hydrophilic phosphorylcholine and hydrophobic fluorinated moieties in these polymers creates a fractal structure with mixed branched cylinders on the surface of gold nanoparticles (AuNPs). In the presence of these polymers, the CO faradaic efficiency improves by 50–80% in the range of −0.7 V to −0.9 V. The fractal structures have a domain size of ∼3 nm, showing enhanced mass transfer kinetics of CO2 approaching the catalyst surfaces without limiting ion diffusion. The phase-separated hydrophilic and hydrophobic domains offer separated channeling to water and CO2, as confirmed by attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and molecule dynamic (MD) simulations. H2O molecules permeate extensively into the polymer layer that adsorbs on zwitterions, forming continuous chains, while CO2 molecules strongly associate with the fluorinated tails of fluorinated polyzwitterions, with oxygen facing the positively charged amine groups. Overall, this coupling of zwitterion and fluorocarbon in a polymer material creates new opportunities for defining microenvironments of metallic nanocatalysts in hybrid structures.

Graphical abstract: Fluorinated polymer zwitterions on gold nanoparticles: patterned catalyst surfaces guide interfacial transport and electrochemical CO2 reduction

Supplementary files

Article information

Article type
Paper
Submitted
04 Apr 2024
Accepted
28 Jul 2024
First published
29 Jul 2024
This article is Open Access
Creative Commons BY-NC license

Nanoscale, 2024,16, 15558-15567

Fluorinated polymer zwitterions on gold nanoparticles: patterned catalyst surfaces guide interfacial transport and electrochemical CO2 reduction

Q. Luo, J. Tapia, L. Zhou, C. Liu, M. Liaqat, H. Duan, Z. Yang, M. Nieh, T. Emrick, P. Bai and J. He, Nanoscale, 2024, 16, 15558 DOI: 10.1039/D4NR01484G

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