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Title: Engineering the entropy-driven free-energy landscape of a dynamic nanoporous protein assembly

Abstract

De novo design and construction of stimuli-responsive protein assemblies that predictably switch between discrete conformational states remains an essential but highly challenging goal in biomolecular design. We previously reported synthetic, two dimensional protein lattices self-assembled via disulfide bonding interactions, which endows them with a unique capacity to undergo coherent conformational changes without losing crystalline order. Here, we carried out all-atom molecular dynamics simulations to map the free-energy landscape of these lattices, validated this landscape through extensive structural characterization by electron microscopy and established that it is predominantly governed by solvent reorganization entropy. Subsequent redesign of the protein surface with conditionally repulsive electrostatic interactions enabled us to predictably perturb the free-energy landscape and obtain a new protein lattice whose conformational dynamics can be chemically and mechanically toggled between three different states with varying porosities and molecular densities.

Authors:
ORCiD logo [1];  [1];  [1]; ORCiD logo [1]
  1. Univ. of California, San Diego, CA (United States). Dept. of Chemistry and Biochemistry
Publication Date:
Research Org.:
Univ. of California, San Diego, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF)
OSTI Identifier:
1507492
Grant/Contract Number:  
SC0003844; CHE-1453204; T32-GM08326
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Chemistry
Additional Journal Information:
Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1755-4330
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Alberstein, Robert, Suzuki, Yuta, Paesani, Francesco, and Tezcan, F. Akif. Engineering the entropy-driven free-energy landscape of a dynamic nanoporous protein assembly. United States: N. p., 2018. Web. doi:10.1038/s41557-018-0053-4.
Alberstein, Robert, Suzuki, Yuta, Paesani, Francesco, & Tezcan, F. Akif. Engineering the entropy-driven free-energy landscape of a dynamic nanoporous protein assembly. United States. doi:10.1038/s41557-018-0053-4.
Alberstein, Robert, Suzuki, Yuta, Paesani, Francesco, and Tezcan, F. Akif. Mon . "Engineering the entropy-driven free-energy landscape of a dynamic nanoporous protein assembly". United States. doi:10.1038/s41557-018-0053-4. https://www.osti.gov/servlets/purl/1507492.
@article{osti_1507492,
title = {Engineering the entropy-driven free-energy landscape of a dynamic nanoporous protein assembly},
author = {Alberstein, Robert and Suzuki, Yuta and Paesani, Francesco and Tezcan, F. Akif},
abstractNote = {De novo design and construction of stimuli-responsive protein assemblies that predictably switch between discrete conformational states remains an essential but highly challenging goal in biomolecular design. We previously reported synthetic, two dimensional protein lattices self-assembled via disulfide bonding interactions, which endows them with a unique capacity to undergo coherent conformational changes without losing crystalline order. Here, we carried out all-atom molecular dynamics simulations to map the free-energy landscape of these lattices, validated this landscape through extensive structural characterization by electron microscopy and established that it is predominantly governed by solvent reorganization entropy. Subsequent redesign of the protein surface with conditionally repulsive electrostatic interactions enabled us to predictably perturb the free-energy landscape and obtain a new protein lattice whose conformational dynamics can be chemically and mechanically toggled between three different states with varying porosities and molecular densities.},
doi = {10.1038/s41557-018-0053-4},
journal = {Nature Chemistry},
issn = {1755-4330},
number = 7,
volume = 10,
place = {United States},
year = {2018},
month = {4}
}

Journal Article:
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Works referenced in this record:

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