Levin and Bakhshandeh suggested in their comment that (1), we stated in our recent review that pH-pKA is a universal parameter for titrating systems, that (2), we omitted to mention in our review the broken symmetry of the constant pH algorithm, and that (3), a constant pH simulation must include a grand-canonical exchange of ions with the reservoir. As a reply to (1), we point out that Levin and Bakhshandeh misquoted and hence invalidated our original statement. We therefore explain in detail under which circumstances pH-pKA can be a universal parameter, and also demonstrate why their numerical example is not in contradiction to our statement. Moreover, the fact that pH-pKA is not a universal parameter for titrating systems is well known in the pertinent literature. Regarding (2), we admit that the symmetry-breaking feature of the constant pH algorithm has escaped our attention at the time of writing the review. We added some clarifying remarks to this behavior. Concerning (3), we point out that the grand-canonical coupling and the resultant Donnan potential are not features of single-phase systems, but are essential for two-phase systems, as was shown in a recent paper by some of us, see J. Landsgesell et al., Macromolecules, 2020, 53, 3007-3020.

Department of Physical and Macromolecular Chemistry Charles University Hlavova 8 128 00 Prague 2 Czech Republic

Faculty of Physics University of Vienna Boltzmanngasse 5 1090 Vienna Austria

Institute for Computational Physics University of Stuttgart Allmandring 3 Stuttgart Germany

Materials Science and Physical Chemistry Department and Research Institute of Theoretical and Computational Chemistry University of Barcelona 08028 Barcelona Catalonia Spain

Vienna Doctoral School in Physics University of Vienna Boltzmanngasse 5 1090 Vienna Austria

Soft Matter. 2019 Feb 6;15(6):1155-1185. doi: 10.1039/c8sm02085j. PubMed

Soft Matter. 2023 May 17;19(19):3519-3521. doi: 10.1039/d2sm01393b. PubMed

Zobrazit více v PubMed

Landsgesell J. Nová L. Rud O. Uhlík F. Sean D. Hebbeker P. Holm C. Košovan P. Soft Matter. 2019;15:1155–1185. doi: 10.1039/C8SM02085J. PubMed DOI

Landsgesell J. Holm C. Smiatek J. Eur. Phys. J.-Spec. Top. 2017;226:725–736. doi: 10.1140/epjst/e2016-60324-3. DOI

Reed C. E. Reed W. F. J. Chem. Phys. 1992;96:1609–1620. doi: 10.1063/1.462145. DOI

Labbez C. and Jönsson B., in Applied Parallel Computing. State of the Art in Scientific Computing, ed. B. Kågström, E. Elmroth, J. Dongarra and J. Wásniewski, Springer Berlin Heidelberg, Berlin, Heidelberg, 2007, vol. 4699, pp. 66–72

McNaught and Wilkinson, IUPAC, Compendium of Chemical Terminology, 2nd edn (the “Gold Book”), 1997

Buck R. P. Rondinini S. Covington A. K. Baucke F. G. K. Brett C. M. A. Camoes M. F. Milton M. J. T. Mussini R. Naumann R. Pratt K. W. Spitzer P. Wilson G. S. Pure Appl. Chem. 2002;74:2169. doi: 10.1351/pac200274112169. DOI

Briskot T. Hillebrandt N. Kluters S. Wang G. Studts J. Hahn T. Huuk T. Hubbuch J. J. Membr. Sci. 2022;648:120333. doi: 10.1016/j.memsci.2022.120333. DOI

Bakhshandeh A. Frydel D. Levin Y. J. Chem. Phys. 2022;156:014108. doi: 10.1063/5.0077956. PubMed DOI

Barr S. A. Panagiotopoulos A. Z. J. Chem. Phys. 2012;137:144704. doi: 10.1063/1.4757284. PubMed DOI

Landsgesell J. Hebbeker P. Rud O. Lunkad R. Košovan P. Holm C. Macromolecules. 2020;53:3007–3020. doi: 10.1021/acs.macromol.0c00260. DOI

Curk T. Luijten E. Phys. Rev. Lett. 2021;126:138003. doi: 10.1103/PhysRevLett.126.138003. PubMed DOI

Bakhshandeh A. Frydel D. Levin Y. Langmuir. 2022;38(45):13963–13971. doi: 10.1021/acs.langmuir.2c02313. PubMed DOI

Charge Regulation Triggers Condensation of Short Oligopeptides to Polyelectrolytes