{"title":"Effects of Carbon Spacer Length on Conformational Transitions and Protein Adsorption of Polyzwitterions","authors":"Chenxu Zhang, Jiemei Zhou* and Yong Wang*, ","doi":"10.1021/acs.langmuir.4c00456","DOIUrl":null,"url":null,"abstract":"<p >The properties of polyzwitterions are closely linked to their carbon spacer length (CSL) between oppositely charged groups. A thorough understanding of the effect of CSL on the properties of polyzwitterion-functionalized membranes is important for their fouling resistance and separation performances. In this work, polyzwitterion-functionalized membranes with different CSLs are prepared by coupling selective swelling-induced pore generation with zwitterionization, and the investigation is focused on comprehending the molecular mechanisms underlying protein resistance and conformational transitions within polyzwitterions under varying CSLs. The zwitterionized films show an enhancement in the surface negative potential with the increase of CSL, attributed to the negatively charged groups distanced from the positively charged groups. Quartz crystal microbalance with dissipation (QCM-D) demonstrates that zwitterionized films with different CSLs display distinct levels of resistance to protein adsorption. The trimethylamine <i>N</i>-oxide-derived polymer (PTMAO, CSL = 0) zwitterionized film shows the highest resistance compared to the poly(3-[dimethyl(2′-methacryloyloxyethyl] ammonio) ethanesulfonate (PMAES, CSL = 2) zwitterionized film and the poly(sulfobetaine methacrylate) (PSBMA, CSL = 3) zwitterionized film, owing to its electrical neutrality and pronounced hydrophilicity. Moreover, analysis of the anti-polyelectrolyte behaviors reveals that PTMAO does not undergo a significant conformation transition in deionized water and salt solutions, while the conformations of PMAES and PSBMA display to be more salt-dependent as the CSL increases, attributed to their increased polarization and dipole moment. As a result, the permeability of zwitterionized membranes exhibits enhanced salt responsiveness with the increase in CSL. The findings of this study are expected to facilitate the design of adsorption-resistant surfaces desired in diverse fields.</p>","PeriodicalId":50,"journal":{"name":"Langmuir","volume":null,"pages":null},"PeriodicalIF":3.7000,"publicationDate":"2024-06-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Langmuir","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.langmuir.4c00456","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The properties of polyzwitterions are closely linked to their carbon spacer length (CSL) between oppositely charged groups. A thorough understanding of the effect of CSL on the properties of polyzwitterion-functionalized membranes is important for their fouling resistance and separation performances. In this work, polyzwitterion-functionalized membranes with different CSLs are prepared by coupling selective swelling-induced pore generation with zwitterionization, and the investigation is focused on comprehending the molecular mechanisms underlying protein resistance and conformational transitions within polyzwitterions under varying CSLs. The zwitterionized films show an enhancement in the surface negative potential with the increase of CSL, attributed to the negatively charged groups distanced from the positively charged groups. Quartz crystal microbalance with dissipation (QCM-D) demonstrates that zwitterionized films with different CSLs display distinct levels of resistance to protein adsorption. The trimethylamine N-oxide-derived polymer (PTMAO, CSL = 0) zwitterionized film shows the highest resistance compared to the poly(3-[dimethyl(2′-methacryloyloxyethyl] ammonio) ethanesulfonate (PMAES, CSL = 2) zwitterionized film and the poly(sulfobetaine methacrylate) (PSBMA, CSL = 3) zwitterionized film, owing to its electrical neutrality and pronounced hydrophilicity. Moreover, analysis of the anti-polyelectrolyte behaviors reveals that PTMAO does not undergo a significant conformation transition in deionized water and salt solutions, while the conformations of PMAES and PSBMA display to be more salt-dependent as the CSL increases, attributed to their increased polarization and dipole moment. As a result, the permeability of zwitterionized membranes exhibits enhanced salt responsiveness with the increase in CSL. The findings of this study are expected to facilitate the design of adsorption-resistant surfaces desired in diverse fields.
期刊介绍:
Langmuir is an interdisciplinary journal publishing articles in the following subject categories:
Colloids: surfactants and self-assembly, dispersions, emulsions, foams
Interfaces: adsorption, reactions, films, forces
Biological Interfaces: biocolloids, biomolecular and biomimetic materials
Materials: nano- and mesostructured materials, polymers, gels, liquid crystals
Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry
Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals
However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do?
Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*.
This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).