Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Single-chain heteropolymers transport protons selectively and rapidly

Journal Article · · Nature (London)
 [1];  [2];  [2];  [3];  [4];  [2];  [2];  [5];  [6];  [2];  [4];  [7];  [8]
  1. Univ. of California, Berkeley, CA (United States); Xiamen Univ. (China)
  2. Univ. of California, Berkeley, CA (United States)
  3. Univ. of California, Santa Cruz, CA (United States); Quantapore Inc., South San Francisco, CA (United States)
  4. Northwestern Univ., Evanston, IL (United States)
  5. Univ. of California, Berkeley, CA (United States); Indiana Univ., Bloomington, IN (United States)
  6. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  7. Univ. of California, Santa Cruz, CA (United States)
  8. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Precise protein sequencing and folding are believed to generate the structure and chemical diversity of natural channels, both of which are essential to synthetically achieve proton transport performance comparable to that seen in natural systems. Geometrically defined channels have been fabricated using peptides, DNAs, carbon nanotubes, sequence-defined polymers and organic frameworks. However, none of these channels rivals the performance observed in their natural counterparts. Here we show that without forming an atomically structured channel, four-monomer-based random heteropolymers (RHPs) can mimic membrane proteins and exhibit selective proton transport across lipid bilayers at a rate similar to those of natural proton channels. Statistical control over the monomer distribution in an RHP leads to segmental heterogeneity in hydrophobicity, which facilitates the insertion of single RHPs into the lipid bilayers. It also results in bilayer-spanning segments containing polar monomers that promote the formation of hydrogen-bonded chains for proton transport. Our study demonstrates the importance of the adaptability that is enabled by statistical similarity among RHP chains and of the modularity provided by the chemical diversity of monomers, to achieve uniform behaviour in heterogeneous systems. Finally, our results also validate statistical randomness as an unexplored approach to realize protein-like behaviour at the single-polymer-chain level in a predictable manner.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
National Science Foundation (NSF); US Army Research Office (ARO); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231; AC05-00OR22725; FG02-08ER46539
OSTI ID:
1607221
Journal Information:
Nature (London), Journal Name: Nature (London) Journal Issue: 7789 Vol. 577; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (47)

Single-chain heteropolymers transport protons selectively and rapidly dataset January 2019
Synthetic Ion Channel Based on Metal–Organic Polyhedra journal July 2008
Selective Artificial Transmembrane Channels for Protons by Formation of Water Wires journal November 2011
PACKMOL: A package for building initial configurations for molecular dynamics simulations journal October 2009
Settle: An analytical version of the SHAKE and RATTLE algorithm for rigid water models journal October 1992
Structure of Fully Hydrated Fluid Phase Lipid Bilayers with Monounsaturated Chains journal January 2006
Colorimetric determination of phospholipids with ammonium ferrothiocyanate journal May 1980
A simple method for displaying the hydropathic character of a protein journal May 1982
VMD: Visual molecular dynamics journal February 1996
CHARMM-GUI Input Generator for NAMD, GROMACS, AMBER, OpenMM, and CHARMM/OpenMM Simulations Using the CHARMM36 Additive Force Field journal December 2015
Practical Prediction of Heteropolymer Composition and Drift journal December 2018
Reconstitution of functional water channels in liposomes containing purified red cell CHIP28 protein journal August 1992
Temperature jump as a new technique to study the kinetics of fast transport of protons across membranes journal October 1986
GROMACS 4:  Algorithms for Highly Efficient, Load-Balanced, and Scalable Molecular Simulation journal February 2008
Mimicry of Antimicrobial Host-Defense Peptides by Random Copolymers journal December 2007
Rigid Rod-Shaped Polyols:  Functional Nonpeptide Models for Transmembrane Proton Channels journal December 1997
Update of the CHARMM All-Atom Additive Force Field for Lipids: Validation on Six Lipid Types journal June 2010
All-Atom Empirical Potential for Molecular Modeling and Dynamics Studies of Proteins journal April 1998
Subnanometer Porous Thin Films by the Co-assembly of Nanotube Subunits and Block Copolymers journal January 2011
Artificial transmembrane ion channels from self-assembling peptide nanotubes journal May 1994
Self-assembly of amphiphilic dendritic dipeptides into helical pores journal August 2004
Structural basis for the function and inhibition of an influenza virus proton channel journal January 2008
Structure and mechanism of the M2 proton channel of influenza A virus journal January 2008
Stochastic transport through carbon nanotubes in lipid bilayers and live cell membranes journal October 2014
Electronic control of H+ current in a bioprotonic device with Gramicidin A and Alamethicin journal October 2016
CHARMM36m: an improved force field for folded and intrinsically disordered proteins journal November 2016
Ultrafast proton transport in sub-1-nm diameter carbon nanotube porins journal April 2016
Posing for a picture: vesicle immobilization in agarose gel journal May 2016
Long-living channels of well defined radius opened in lipid bilayers by polydisperse, hydrophobically-modified polyacrylic acids journal January 2007
Polymorphic transitions in single crystals: A new molecular dynamics method journal December 1981
Particle mesh Ewald: An N ⋅log( N ) method for Ewald sums in large systems journal June 1993
A smooth particle mesh Ewald method journal November 1995
COPI coat assembly occurs on liquid-disordered domains and the associated membrane deformations are limited by membrane tension journal October 2008
Highly permeable artificial water channels that can self-assemble into two-dimensional arrays journal July 2015
Molecular mechanisms for proton transport in membranes. journal January 1978
Amphipols: Polymers that keep membrane proteins soluble in aqueous solutions journal December 1996
Simulation of biomimetic recognition between polymers and surfaces journal October 1999
Deuterium Isotope Effects on Permeation and Gating of Proton Channels in Rat Alveolar Epithelium journal April 1997
The suite of small-angle neutron scattering instruments at Oak Ridge National Laboratory journal February 2018
A tutorial on hidden Markov models and selected applications in speech recognition journal January 1989
The viterbi algorithm journal January 1973
Aligned Multiwalled Carbon Nanotube Membranes journal January 2004
Synthetic Lipid Membrane Channels Formed by Designed DNA Nanostructures journal November 2012
De novo design of a transmembrane Zn 2+ -transporting four-helix bundle journal December 2014
Random heteropolymers preserve protein function in foreign environments journal March 2018
Definitive Assignment of Proton Selectivity and Attoampere Unitary Current to the M2 Ion Channel Protein of Influenza A Virus journal April 2001
Voltage-Gated Proton Channels and Other Proton Transfer Pathways journal April 2003

Cited By (1)

Single-chain heteropolymers transport protons selectively and rapidly dataset January 2019


Similar Records

Sequence Design of Random Heteropolymers as Protein Mimics
Journal Article · Thu Jan 12 19:00:00 EST 2023 · Biomacromolecules · OSTI ID:2470769

Mapping Composition Evolution through Synthesis, Purification, and Depolymerization of Random Heteropolymers
Journal Article · Wed Feb 21 19:00:00 EST 2024 · Journal of the American Chemical Society · OSTI ID:2469689

Population-based heteropolymer design to mimic protein mixtures
Journal Article · Tue Mar 07 19:00:00 EST 2023 · Nature (London) · OSTI ID:2229313