The DOI matches its Crossref record; 32 of the 32 references it cites were found in a registry or an index.
Phase Behavior and Salt Partitioning in Polyelectrolyte Complex Coacervates
Abstract
Polyelectrolyte complexes are omnipresent both in nature and in the technological world, including nucleotide condensates, biological marine adhesives, food stabilizers, encapsulants, and carriers for gene therapy. However, the true phase behavior of complexes, resulting from associative phase separation of oppositely charged polyelectrolytes, remains poorly understood. Here, we rely on complementary experimental and simulation approaches to create a complete quantitative description of the phase behavior of polyelectrolyte complexes that represents a significant advance in our understanding of the underlying physics of polyelectrolyte complexation. Experiments employing multiple approaches with model polyelectrolytes—oppositely charged polypeptides poly( l -lysine) and poly( d, l -glutamic acid) of matched chain lengths—led to phase diagrams with compositions of the complex and the supernatant that were in excellent agreement with simulation results. Contrary to the widely accepted theory for complexation, we found preferential partitioning of salt ions into the supernatant phase. Additionally, the salt partitioning into the supernatant phase was found to initially increase and then decrease on increasing the salt concentrations, manifesting as a distinct minimum in the salt partition coefficients. These trends were shown by simulations to be strongly influenced by the excluded volume interactions in the complex phase, which were not accounted for in their entirety in earlier theories. We believe the comprehensive data we present will be conducive to the development of an accurate physical theory for polyelectrolyte complexation with predictive capabilities.
Overview
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Integrity signals
Registry
Cites
Statistics
Verification
Claims the paper makes
The claims and statistics of this paper haven’t been checked yet.
Run the check — free, no account needed. It reads the open-access text and checks the sources it cites.
Self-check
Percentages, sums and reported differences re-computed from the paper’s own numbers.
The self-check needs the paper’s full text.
Citations
Cites
Liquid-Liquid Phase Separation in Biology
Hyman, A. A., Weber, C. A., & Jülicher, F. (2014) · Annual Review of Cell and Developmental Biology · doi:10.1146/annurev-cellbio-100913-013325 · Cited by 3,155
Accumulation of sub-100 nm polymeric micelles in poorly permeable tumours depends on size
Cabral, H., Matsumoto, Y., Mizuno, K., Chen, Q., Murakami, M., Kimura, M., Terada, Y., Kano, M. R., Miyazono, K., Uesaka, M., et al. (2011) · Nature Nanotechnology · doi:10.1038/nnano.2011.166 · Cited by 2,429
Polymer physics of intracellular phase transitions
Brangwynne, C. P., Tompa, P., & Pappu, R. V. (2015) · Nature Physics · doi:10.1038/nphys3532 · Cited by 1,553
General purpose molecular dynamics simulations fully implemented on graphics processing units
Anderson, J. A., Lorenz, C. D., & Travesset, A. (2008) · Journal of Computational Physics · doi:10.1016/j.jcp.2008.01.047 · Cited by 1,481
Phase separation in polyelectrolyte solutions. Theory of complex coacervation
Overbeek, J. T. G., & Voorn, M. J. (1957) · Journal of Cellular and Comparative Physiology · doi:10.1002/jcp.1030490404 · Cited by 625
Aumiller, W. M., & Keating, C. D. (2016) · Nature Chemistry · doi:10.1038/nchem.2414 · Cited by 612
The Polyelectrolyte Complex/Coacervate Continuum
Wang, Q., & Schlenoff, J. B. (2014) · Macromolecules · doi:10.1021/ma500500q · Cited by 585
Zhao, Q., Lee, D. W., Ahn, B. K., Seo, S., Kaufman, Y., Israelachvili, J. N., & Waite, J. H. (2016) · Nature Materials · doi:10.1038/nmat4539 · Cited by 503
Binodal Compositions of Polyelectrolyte Complexes
Spruijt, E., Westphal, A. H., Borst, J. W., Cohen Stuart, M. A., & van der Gucht, J. (2010) · Macromolecules · doi:10.1021/ma101031t · Cited by 429
Phase behaviour and complex coacervation of aqueous polypeptide solutions
Priftis, D., & Tirrell, M. (2012) · Soft Matter · doi:10.1039/c2sm25604e · Cited by 374
Self-citationEntropy and enthalpy of polyelectrolyte complexation: Langevin dynamics simulations
Ou, Z., & Muthukumar, M. (2006) · The Journal of Chemical Physics · doi:10.1063/1.2178803 · Cited by 351
Protein Encapsulation via Polypeptide Complex Coacervation
Black, K. A., Priftis, D., Perry, S. L., Yip, J., Byun, W. Y., & Tirrell, M. (2014) · ACS Macro Letters · doi:10.1021/mz500529v · Cited by 316
Self-citationChirality-selected phase behaviour in ionic polypeptide complexes
Perry, S. L., Leon, L., Hoffmann, K. Q., Kade, M. J., Priftis, D., Black, K. A., Wong, D., Klein, R. A., Pierce, C. F., Margossian, K. O., et al. (2015) · Nature Communications · doi:10.1038/ncomms7052 · Cited by 300
Self-citationOligonucleotide–Peptide Complexes: Phase Control by Hybridization
Vieregg, J. R., Lueckheide, M., Marciel, A. B., Leon, L., Bologna, A. J., Rivera, J. R., & Tirrell, M. V. (2018) · Journal of the American Chemical Society · doi:10.1021/jacs.7b03567 · Cited by 273
Self-citationPhase Behavior and Coacervation of Aqueous Poly(acrylic acid)−Poly(allylamine) Solutions
Chollakup, R., Smitthipong, W., Eisenbach, C. D., & Tirrell, M. (2010) · Macromolecules · doi:10.1021/ma902144k · Cited by 265
Self-citationSmith, J., Calidas, D., Schmidt, H., Lu, T., Rasoloson, D., & Seydoux, G. (2016) · eLife · doi:10.7554/elife.21337 · Cited by 221
PHASE SEPARATION IN POLYELECTROLYTE SYSTEMS. I. COMPLEX COACERVATES OF GELATIN
Veis, A., & Aranyi, C. (1960) · The Journal of Physical Chemistry · doi:10.1021/j100838a022 · Cited by 204
Chollakup, R., Beck, J. B., Dirnberger, K., Tirrell, M., & Eisenbach, C. D. (2013) · Macromolecules · doi:10.1021/ma202172q · Cited by 197
Self-citationA review of the early development of the thermodynamics of the complex coacervation phase separation
Veis, A. (2011) · Advances in Colloid and Interface Science · doi:10.1016/j.cis.2011.01.007 · Cited by 192
Theory of polyelectrolyte complexation—Complex coacervates are self-coacervates
Delaney, K. T., & Fredrickson, G. H. (2017) · The Journal of Chemical Physics · doi:10.1063/1.4985568 · Cited by 169
PRISM-Based Theory of Complex Coacervation: Excluded Volume versus Chain Correlation
Perry, S. L., & Sing, C. E. (2015) · Macromolecules · doi:10.1021/acs.macromol.5b01027 · Cited by 160
pH and Salt Effects on the Associative Phase Separation of Oppositely Charged Polyelectrolytes
Jha, P. K., Desai, P. S., Li, J., & Larson, R. G. (2014) · Polymers · doi:10.3390/polym6051414 · Cited by 152
Krogstad, D. V., Lynd, N. A., Choi, S., Spruell, J. M., Hawker, C. J., Krämer, E. J., & Tirrell, M. (2013) · Macromolecules · doi:10.1021/ma302299r · Cited by 146
Self-citationSrivastava, S., & Tirrell, M. (2016) · Advances in chemical physics · doi:10.1002/9781119290971.ch7 · Cited by 116
Self-citationInhibition of atherosclerosis-promoting microRNAs via targeted polyelectrolyte complex micelles
Kuo, C., Leon, L., Chung, E. J., Huang, R., Sontag, T. J., Reardon, C. A., Getz, G. S., Tirrell, M., & Fang, Y. H. (2014) · Journal of Materials Chemistry B · doi:10.1039/c4tb00977k · Cited by 111
Self-citationSalting-Out and Salting-In of Polyelectrolyte Solutions: A Liquid-State Theory Study
Zhang, P., Alsaifi, N. M., Wu, J., & Wang, Z. (2016) · Macromolecules · doi:10.1021/acs.macromol.6b02160 · Cited by 101
Partitioning and Enhanced Self-Assembly of Actin in Polypeptide Coacervates
McCall, P. M., Srivastava, S., Perry, S. L., Kovar, D. R., Gardel, M. L., & Tirrell, M. (2018) · Biophysical Journal · doi:10.1016/j.bpj.2018.02.020 · Cited by 100
Self-citationMicrofluidic Formation of Membrane‐Free Aqueous Coacervate Droplets in Water
van Swaay, D., Tang, T. ‐. D., Mann, S., & deMello, A. J. (2015) · Angewandte Chemie International Edition · doi:10.1002/anie.201502886 · Cited by 95
Coarse-Grained Model of the Dynamics of Electrolyte Solutions
Andreev, M., Chremos, A., Pablo, J., & Douglas, J. F. (2017) · The Journal of Physical Chemistry B · doi:10.1021/acs.jpcb.7b04297 · Cited by 62
Self-citationZhao, M., Eghtesadi, S. A., Dawadi, M. B., Wang, C., Huang, S., Seymore, A. E., Vogt, B. D., Modarelli, D. A., Liu, T., & Zacharia, N. S. (2017) · Macromolecules · doi:10.1021/acs.macromol.6b02815 · Cited by 59
Bulk and nanoscale polypeptide based polyelectrolyte complexes
Marciel, A. B., Chung, E. J., Brettmann, B. K., & Leon, L. (2016) · Advances in Colloid and Interface Science · doi:10.1016/j.cis.2016.06.012 · Cited by 53
Self-citationIn Retrospect: The Origin of Life
Hyman, A. A., & Brangwynne, C. (2012) · Nature · doi:10.1038/491524a · Cited by 47
Cited by
Cakmak, F. P., Choi, S., Meyer, M. O., Bevilacqua, P. C., & Keating, C. D. (2020) · Nature Communications · doi:10.1038/s41467-020-19775-w · Cited by 185
Metadata
- Authors
- Li, L., Srivastava, S., Andreev, M., Marciel, A. B., de Pablo, J. J., & Tirrell, M. V.
- Venue
- Macromolecules
- Publisher
- American Chemical Society (ACS)
- Published
- 2018-04-05
- Volume
- 51
- Issue
- 8
- Pages
- 2988-2995
- ISSN
- 0024-9297 (ISSN-L)
- 1520-5835
- OpenAlex
- W2795682970
- Cited by
- 357
- References
- 32
- FWCI
- 25.33
- Type
- journal article
- Language
- en
- Open access
- closed
About these checks
Registry, retraction, Cites and statistics results are computed, not judged, with one exception: a printed reference that no index lists is read once by a model before it counts as a citation error. Claims are extracted by a model and kept only when their quote appears verbatim in the text; each cited source is then checked, with a model’s help, for whether it says what the claim relies on. Those verdicts can be wrong — read the claim’s quote and the cited source before relying on one.
Statistics and arithmetic are recomputed, not judged.
Confidence bands are shown only for fields calibrated on our annotated test set. None is calibrated yet, so no band is shown.
What counts as a claim ›How we measure confidence ›How we check this ›
Are you an author, or do you see a problem with this page? Request a review
Data sources
Bibliographic data: Semantic Scholar, OpenAlex, Crossref.
Contains information from the Semantic Scholar Academic Graph Datasets, made available under the ODC Attribution License (ODC-BY 1.0).
Semantic Scholar’s data is described in: Kinney, R., et al. (2023). The Semantic Scholar Open Data Platform. arXiv:2301.10140.