Title: Ion-dependent protein–surface interactions from intrinsic solvent response

Abstract

The phyllosilicate mineral muscovite mica is widely used as a surface template for the patterning of macromolecules, yet a molecular understanding of its surface chemistry under varying solution conditions, required to predict and control the self-assembly of adsorbed species, is lacking. We utilize all-atom molecular dynamics simulations in conjunction with an electrostatic analysis based in local molecular field theory that affords a clean separation of long-range and short-range electrostatics. Using water polarization response as a measure of the electric fields that arise from patterned, surface-bound ions that direct the adsorption of charged macromolecules, we apply a Landau theory of forces induced by asymmetrically polarized surfaces to compute protein–surface interactions for two muscovite-binding proteins (DHR10-mica6 and ^C98RhuA). Comparison of the pressure between surface and protein in high-concentration KCl and NaCl aqueous solutions reveals ion-specific differences in far-field protein–surface interactions, neatly capturing the ability of ions to modulate the surface charge of muscovite that in turn selectively attracts one binding face of each protein over all others.

Authors:

Prelesnik, Jesse L.  ^[1];

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• Search DOE PAGES for ORCID "0000-0002-5089-5215"

Alberstein, Robert G.  ^[2];

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• Search DOE PAGES for ORCID "0000-0002-6655-8811"

Zhang, Shuai  ^[3];

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• Search DOE PAGES for ORCID "0000-0003-0170-6470"

Pyles, Harley ^[4]; Baker, David  ^[5];

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Pfaendtner, Jim  ^[6];

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• Search DOE PAGES for ORCID "0000-0001-6727-2957"

De Yoreo, James J. ^[3]; Tezcan, F. Akif  ^[7];

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• Search DOE PAGES for ORCID "0000-0002-4733-6500"

Remsing, Richard C. ^[8]; Mundy, Christopher J.  ^[9]

• Search DOE PAGES for author "Mundy, Christopher J."
• Search DOE PAGES for ORCID "0000-0003-1378-5241"

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+ Show Author Affiliations

1. Department of Chemistry, University of Washington, Seattle, WA 98195,
2. Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093,
3. Physical Sciences Division, Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, Richland, WA 99354,, Materials Science and Engineering, University of Washington, Seattle, WA 98195,
4. Department of Biochemistry, University of Washington, Seattle, WA 98195,, Institute for Protein Design, University of Washington, Seattle, WA 98195,
5. Department of Biochemistry, University of Washington, Seattle, WA 98195,, Institute for Protein Design, University of Washington, Seattle, WA 98195,, HHMI, University of Washington, Seattle, WA 98195,
6. Department of Chemistry, University of Washington, Seattle, WA 98195,, Department of Chemical Engineering, University of Washington, Seattle, WA 98195,
7. Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093,, Materials Science and Engineering, University of California, San Diego, La Jolla, CA 92093,
8. Department of Chemistry and Chemical Biology, Rutgers University, Piscataway, NJ 08854,
9. Department of Chemical Engineering, University of Washington, Seattle, WA 98195,, Chemical Physics Theory Team, Pacific Northwest National Laboratory, Richland, WA 99354

Publication Date:

Fri Jun 25 00:00:00 EDT 2021

Research Org.:

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Univ. of Washington, Seattle, WA (United States)

Sponsoring Org.:

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

OSTI Identifier:

1798553

Alternate Identifier(s):

OSTI ID: 1810291; OSTI ID: 1821486

Report Number(s):

PNNL-SA-158527
Journal ID: ISSN 0027-8424; e2025121118

Grant/Contract Number:  

SC0019288; AC05-76RL01830

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 118 Journal Issue: 26; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

Country of Publication:

United States

Language:

English

Subject:

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; soft matter; solution assembly; specific ion effects; electrostatics; Landau theory