Interfacial Yield Stress Response in Synthetic Mucin Solutions
Abstract The solution rheology of a fully synthetic, monodisperse mucin that mimics the glycosylated domains of natural mucins, poly(β‐Gal‐Thr)22, is studied to systematically explore relationships between polymer structure, solution conditions, and rheological properties. Using standard cone‐plate...
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| Format: | Article |
| Language: | English |
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Wiley-VCH
2025-06-01
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| Series: | Advanced Materials Interfaces |
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| Online Access: | https://doi.org/10.1002/admi.202500066 |
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| author | Sumit Sunil Kumar Travis Leadbetter J. Brandon McClimon Manuel A. Lema Farhana M. Khan Prashant K. Purohit Adam B. Braunschweig Robert W. Carpick |
| author_facet | Sumit Sunil Kumar Travis Leadbetter J. Brandon McClimon Manuel A. Lema Farhana M. Khan Prashant K. Purohit Adam B. Braunschweig Robert W. Carpick |
| author_sort | Sumit Sunil Kumar |
| collection | DOAJ |
| description | Abstract The solution rheology of a fully synthetic, monodisperse mucin that mimics the glycosylated domains of natural mucins, poly(β‐Gal‐Thr)22, is studied to systematically explore relationships between polymer structure, solution conditions, and rheological properties. Using standard cone‐plate rheometry, shear thinning is observed over a range of concentrations, with an apparent yield stress—typical for gels—evident at the highest concentrations. This is surprising given the dilute, weakly interacting nature of the solutions and the lack of observable structure in cryogenic electron microscopy and particle tracking microrheology. However, interfacial rheometry demonstrates that the gel‐like behavior is attributable to a thin structured layer at the air–water interface, without any bulk gelation. This is attributed to an interfacial layer formed by inter‐mucin H‐bonds that yields when sheared. A computational model using kinetic Monte Carlo (kMC) simulations qualitatively reproduces the yield stress response of such a network through an intermolecular bonding potential. An analytical model of stochastic bond formation and breaking, validated by the kMC simulations, demonstrates that having multiple bonding sites per mucin with a force‐dependent debonding rate aligns with experiments, consistent with intermolecular interactions for other mucin proteins. This suggests that in mucin solutions, gelation may begin at the air–water interface, and emphasizes the need for multitechnique validation when exploring structural cues of mucus gelation through rheometry. |
| format | Article |
| id | doaj-art-047219b7e0914a448dfcd042d994be25 |
| institution | OA Journals |
| issn | 2196-7350 |
| language | English |
| publishDate | 2025-06-01 |
| publisher | Wiley-VCH |
| record_format | Article |
| series | Advanced Materials Interfaces |
| spelling | doaj-art-047219b7e0914a448dfcd042d994be252025-08-20T02:38:18ZengWiley-VCHAdvanced Materials Interfaces2196-73502025-06-011212n/an/a10.1002/admi.202500066Interfacial Yield Stress Response in Synthetic Mucin SolutionsSumit Sunil Kumar0Travis Leadbetter1J. Brandon McClimon2Manuel A. Lema3Farhana M. Khan4Prashant K. Purohit5Adam B. Braunschweig6Robert W. Carpick7Department of Mechanical Engineering and Applied Mechanics University of Pennsylvania Philadelphia PA 19104 USAGraduate Group in Applied Mathematics and Computational Science University of Pennsylvania Philadelphia PA 19104 USADepartment of Mechanical Engineering and Applied Mechanics University of Pennsylvania Philadelphia PA 19104 USAAdvanced Science Research Center Graduate Center at the City University of New York New York NY 10031 USAAdvanced Science Research Center Graduate Center at the City University of New York New York NY 10031 USADepartment of Mechanical Engineering and Applied Mechanics University of Pennsylvania Philadelphia PA 19104 USAAdvanced Science Research Center Graduate Center at the City University of New York New York NY 10031 USADepartment of Mechanical Engineering and Applied Mechanics University of Pennsylvania Philadelphia PA 19104 USAAbstract The solution rheology of a fully synthetic, monodisperse mucin that mimics the glycosylated domains of natural mucins, poly(β‐Gal‐Thr)22, is studied to systematically explore relationships between polymer structure, solution conditions, and rheological properties. Using standard cone‐plate rheometry, shear thinning is observed over a range of concentrations, with an apparent yield stress—typical for gels—evident at the highest concentrations. This is surprising given the dilute, weakly interacting nature of the solutions and the lack of observable structure in cryogenic electron microscopy and particle tracking microrheology. However, interfacial rheometry demonstrates that the gel‐like behavior is attributable to a thin structured layer at the air–water interface, without any bulk gelation. This is attributed to an interfacial layer formed by inter‐mucin H‐bonds that yields when sheared. A computational model using kinetic Monte Carlo (kMC) simulations qualitatively reproduces the yield stress response of such a network through an intermolecular bonding potential. An analytical model of stochastic bond formation and breaking, validated by the kMC simulations, demonstrates that having multiple bonding sites per mucin with a force‐dependent debonding rate aligns with experiments, consistent with intermolecular interactions for other mucin proteins. This suggests that in mucin solutions, gelation may begin at the air–water interface, and emphasizes the need for multitechnique validation when exploring structural cues of mucus gelation through rheometry.https://doi.org/10.1002/admi.202500066biomimeticbiopolymergelationmucusrheologysynthetic mucins |
| spellingShingle | Sumit Sunil Kumar Travis Leadbetter J. Brandon McClimon Manuel A. Lema Farhana M. Khan Prashant K. Purohit Adam B. Braunschweig Robert W. Carpick Interfacial Yield Stress Response in Synthetic Mucin Solutions Advanced Materials Interfaces biomimetic biopolymer gelation mucus rheology synthetic mucins |
| title | Interfacial Yield Stress Response in Synthetic Mucin Solutions |
| title_full | Interfacial Yield Stress Response in Synthetic Mucin Solutions |
| title_fullStr | Interfacial Yield Stress Response in Synthetic Mucin Solutions |
| title_full_unstemmed | Interfacial Yield Stress Response in Synthetic Mucin Solutions |
| title_short | Interfacial Yield Stress Response in Synthetic Mucin Solutions |
| title_sort | interfacial yield stress response in synthetic mucin solutions |
| topic | biomimetic biopolymer gelation mucus rheology synthetic mucins |
| url | https://doi.org/10.1002/admi.202500066 |
| work_keys_str_mv | AT sumitsunilkumar interfacialyieldstressresponseinsyntheticmucinsolutions AT travisleadbetter interfacialyieldstressresponseinsyntheticmucinsolutions AT jbrandonmcclimon interfacialyieldstressresponseinsyntheticmucinsolutions AT manuelalema interfacialyieldstressresponseinsyntheticmucinsolutions AT farhanamkhan interfacialyieldstressresponseinsyntheticmucinsolutions AT prashantkpurohit interfacialyieldstressresponseinsyntheticmucinsolutions AT adambbraunschweig interfacialyieldstressresponseinsyntheticmucinsolutions AT robertwcarpick interfacialyieldstressresponseinsyntheticmucinsolutions |