Amino Acid Sequence Controls Enhanced Electron Transport in Heme-Binding Peptide Monolayers

Yang, Hao; Liu, Xiaolin; Meigooni, Moeen; Zhang, Li; Ren, Jitong; Chen, Qian; Losego, Mark; Tajkhorshid, Emad; Moore, Jeffrey S.; Schroeder, Charles M.

doi:10.1021/acscentsci.4c01849

Amino Acid Sequence Controls Enhanced Electron Transport in Heme-Binding Peptide Monolayers

Journal Article · Wed Apr 02 00:00:00 EDT 2025 · ACS Central Science

DOI:https://doi.org/10.1021/acscentsci.4c01849· OSTI ID:2545107

Yang, Hao ^[1]; ^[1]; Meigooni, Moeen ^[1]; ^[2]; Ren, Jitong ^[1]; ^[3]; ^[2]; ^[1]; ^[1]; ^[1]

University of Illinois at Urbana-Champaign, IL (United States)
Georgia Institute of Technology, Atlanta, GA (United States)
University of Illinois at Urbana-Champaign, IL (United States); Chan Zuckerberg Biohub Chicago, IL (United States)

Metal-binding proteins have the exceptional ability to facilitate long-range electron transport in nature. Despite recent progress, the sequence-structure–function relationships governing electron transport in heme-binding peptides and protein assemblies are not yet fully understood. In this work, the electronic properties of a series of heme-binding peptides inspired by cytochrome bc1 are studied using a combination of molecular electronics experiments, molecular modeling, and simulation. Self-assembled monolayers (SAMs) are prepared using sequence-defined heme-binding peptides capable of forming helical secondary structures. Following monolayer formation, the structural properties and chemical composition of assembled peptides are determined using atomic force microscopy and X-ray photoelectron spectroscopy, and the electronic properties (current density–voltage response) are characterized using a soft contact liquid metal electrode method based on eutectic gallium–indium alloys (EGaIn). Our results show a substantial 1000-fold increase in current density across SAM junctions upon addition of heme compared to identical peptide sequences in the absence of heme, while maintaining a constant junction thickness. These findings show that amino acid composition and sequence directly control enhancements in electron transport in heme-binding peptides. Overall, this study demonstrates the potential of using sequence-defined synthetic peptides inspired by nature as functional bioelectronic materials.

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Research Organization:: University of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0022035

OSTI ID:: 2545107

Alternate ID(s):: OSTI ID: 2562135

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Journal Issue: 4 Vol. 11; ISSN 2374-7943

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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