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Article ; Online: A Pro-Regenerative Supramolecular Prodrug Protects Against and Repairs Colon Damage in Experimental Colitis.

DeFrates, Kelsey G / Tong, Elaine / Cheng, Jing / Heber-Katz, Ellen / Messersmith, Phillip B

Advanced science (Weinheim, Baden-Wurttemberg, Germany)

2024 Volume 11, Issue 13, Page(s) e2304716

Abstract: Structural repair of the intestinal epithelium is strongly correlated with disease remission in inflammatory bowel disease (IBD); however, ulcer healing is not addressed by existing therapies. To address this need, this study reports the use of a small ... ...

Abstract	Structural repair of the intestinal epithelium is strongly correlated with disease remission in inflammatory bowel disease (IBD); however, ulcer healing is not addressed by existing therapies. To address this need, this study reports the use of a small molecule prolyl hydroxylase (PHD) inhibitor (DPCA) to upregulate hypoxia-inducible factor one-alpha (HIF-1α) and induce mammalian regeneration. Sustained delivery of DPCA is achieved through subcutaneous injections of a supramolecular hydrogel, formed through the self-assembly of PEG-DPCA conjugates. Pre-treatment of mice with PEG-DPCA is shown to protect mice from epithelial erosion and symptoms of dextran sodium sulfate (DSS)-induced colitis. Surprisingly, a single subcutaneous dose of PEG-DPCA, administered after disease onset, leads to accelerated weight gain and complete restoration of healthy tissue architecture in colitic mice. Rapid DPCA-induced restoration of the intestinal barrier is likely orchestrated by increased expression of HIF-1α and associated targets leading to an epithelial-to-mesenchymal transition. Further investigation of DPCA as a potential adjunctive or stand-alone restorative treatment to combat active IBD is warranted.
MeSH term(s)	Mice ; Animals ; Colitis/chemically induced ; Colitis/drug therapy ; Colitis/prevention & control ; Inflammatory Bowel Diseases ; Intestinal Mucosa/metabolism ; Disease Models, Animal ; Mammals
Language	English
Publishing date	2024-01-21
Publishing country	Germany
Document type	Journal Article
ZDB-ID	2808093-2
ISSN	2198-3844 ; 2198-3844
ISSN (online)	2198-3844
ISSN	2198-3844
DOI	10.1002/advs.202304716
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Rheology and Gelation of Hyaluronic Acid/Chitosan Coacervates.

Kayitmazer, A Basak / Comert, Fatih / Winter, Henning H / Messersmith, Phillip B

Biomolecules

2022 Volume 12, Issue 12

Abstract: Hyaluronic acid (HA) and chitosan (CHI) are biopolyelectrolytes which are interesting for both the medical and polymer physics communities due to their biocompatibility and semi-flexibility, respectively. In this work, we demonstrate by rheology ... ...

Abstract	Hyaluronic acid (HA) and chitosan (CHI) are biopolyelectrolytes which are interesting for both the medical and polymer physics communities due to their biocompatibility and semi-flexibility, respectively. In this work, we demonstrate by rheology experiments that the linear viscoelasticity of HA/CHI coacervates depends strongly on the molecular weight of the polymers. Moduli for coacervates were found significantly higher than those of individual HA and CHI physical gels. A remarkable 1.5-fold increase in moduli was noted when catechol-conjugated HA and CHI were used instead. This was attributed to the conversion of coacervates to chemical gels by oxidation of 3,4-dihydroxyphenylalanine (DOPA) groups in HA and CHI to di-DOPA crosslinks. These rheological results put HA/CHI coacervates in the category of strong candidates as injectable tissue scaffolds or medical adhesives.
Language	English
Publishing date	2022-12-05
Publishing country	Switzerland
Document type	Journal Article
ZDB-ID	2701262-1
ISSN	2218-273X ; 2218-273X
ISSN (online)	2218-273X
ISSN	2218-273X
DOI	10.3390/biom12121817
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Surface Force Measurements of Mussel-Inspired Pressure-Sensitive Adhesives.

Degen, George D / Delparastan, Peyman / Tiu, Brylee David B / Messersmith, Phillip B

ACS applied materials & interfaces

2022 Volume 14, Issue 4, Page(s) 6212–6220

Abstract: Translating fundamental studies of marine mussel adhesion into practical mussel-inspired wet adhesives remains an important technological challenge. To adhere, mussels secrete adhesive proteins rich in the catecholic amino acid 3,4-dihydroxyphenylalanine ...

Abstract	Translating fundamental studies of marine mussel adhesion into practical mussel-inspired wet adhesives remains an important technological challenge. To adhere, mussels secrete adhesive proteins rich in the catecholic amino acid 3,4-dihydroxyphenylalanine (Dopa) and positively charged lysine. Consequently, numerous synthetic adhesives incorporating catecholic and cationic functionalities have been designed. However, despite widespread research, uncertainties remain about the optimal design of synthetic mussel-inspired adhesives. Here, we present a study of the adhesion of mussel-inspired pressure-sensitive adhesives. We explore the effects of catechol content, molecular architecture, and solvent quality on pressure-sensitive adhesive (PSA) adhesion and cohesion measured in a surface forces apparatus. Our findings demonstrate that the influence of catechol content depends on the choice of solvent and that adhesive performance is dictated by film composition rather than molecular architecture. Our results also highlight the importance of electrostatic and hydrophobic interactions for adhesion and cohesion in aqueous environments. Together, our findings contribute to an improved understanding of the interplay between materials chemistry, environmental conditions, and adhesive performance to facilitate the design of bioinspired wet adhesives.
MeSH term(s)	Acrylic Resins/chemical synthesis ; Acrylic Resins/chemistry ; Adhesiveness ; Adhesives/chemical synthesis ; Adhesives/chemistry ; Catechols/chemical synthesis ; Catechols/chemistry ; Ethanol/chemistry ; Pressure ; Solvents/chemistry ; Water/chemistry
Chemical Substances	Acrylic Resins ; Adhesives ; Catechols ; Solvents ; Water (059QF0KO0R) ; Ethanol (3K9958V90M)
Language	English
Publishing date	2022-01-20
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.1c22295
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Pulling together to improve stability.

Higginson, Cody J / Messersmith, Phillip B

Nature chemistry

2019 Volume 11, Issue 4, Page(s) 295–296

Language	English
Publishing date	2019-03-22
Publishing country	England
Document type	Journal Article
ZDB-ID	2464596-5
ISSN	1755-4349 ; 1755-4330
ISSN (online)	1755-4349
ISSN	1755-4330
DOI	10.1038/s41557-019-0244-7
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Surface Force Measurements of Mussel-Inspired Pressure-Sensitive Adhesives

Degen, George D. / Delparastan, Peyman / Tiu, Brylee David B. / Messersmith, Phillip B.

ACS applied materials & interfaces. 2022 Jan. 20, v. 14, no. 4

2022

Abstract	Translating fundamental studies of marine mussel adhesion into practical mussel-inspired wet adhesives remains an important technological challenge. To adhere, mussels secrete adhesive proteins rich in the catecholic amino acid 3,4-dihydroxyphenylalanine (Dopa) and positively charged lysine. Consequently, numerous synthetic adhesives incorporating catecholic and cationic functionalities have been designed. However, despite widespread research, uncertainties remain about the optimal design of synthetic mussel-inspired adhesives. Here, we present a study of the adhesion of mussel-inspired pressure-sensitive adhesives. We explore the effects of catechol content, molecular architecture, and solvent quality on pressure-sensitive adhesive (PSA) adhesion and cohesion measured in a surface forces apparatus. Our findings demonstrate that the influence of catechol content depends on the choice of solvent and that adhesive performance is dictated by film composition rather than molecular architecture. Our results also highlight the importance of electrostatic and hydrophobic interactions for adhesion and cohesion in aqueous environments. Together, our findings contribute to an improved understanding of the interplay between materials chemistry, environmental conditions, and adhesive performance to facilitate the design of bioinspired wet adhesives.
Keywords	adhesion ; catechol ; cohesion ; dihydroxyphenylalanine ; hydrophobicity ; lysine ; mussels ; solvents
Language	English
Dates of publication	2022-0120
Size	p. 6212-6220.
Publishing place	American Chemical Society
Document type	Article
ISSN	1944-8252
DOI	10.1021/acsami.1c22295
Database	NAL-Catalogue (AGRICOLA)

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Article ; Online: Bioinspired Macromolecular Materials.

Webber, Matthew J / Kamat, Neha P / Messersmith, Phillip B / Lecommandoux, Sébastien

Biomacromolecules

2021 Volume 22, Issue 1, Page(s) 1–3

MeSH term(s)	Biomimetic Materials ; Biomimetics ; Macromolecular Substances
Chemical Substances	Macromolecular Substances
Language	English
Publishing date	2021-01-11
Publishing country	United States
Document type	Editorial
ISSN	1526-4602
ISSN (online)	1526-4602
DOI	10.1021/acs.biomac.0c01614
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Biomaterials in fetal surgery.

Winkler, Sally M / Harrison, Michael R / Messersmith, Phillip B

Biomaterials science

2019 Volume 7, Issue 8, Page(s) 3092–3109

Abstract: Fetal surgery and fetal therapy involve surgical interventions on the fetus in utero to correct or ameliorate congenital abnormalities and give a developing fetus the best chance at a healthy life. Historical use of biomaterials in fetal surgery has been ...

Abstract	Fetal surgery and fetal therapy involve surgical interventions on the fetus in utero to correct or ameliorate congenital abnormalities and give a developing fetus the best chance at a healthy life. Historical use of biomaterials in fetal surgery has been limited, and most biomaterials used in fetal surgeries today were originally developed for adult or pediatric patients. However, as the field of fetal surgery moves from open surgeries to minimally invasive procedures, many opportunities exist for innovative biomaterials engineers to create materials designed specifically for the unique challenges and opportunities of maternal-fetal surgery. Here, we review biomaterials currently used in clinical fetal surgery as well as promising biomaterials in development for eventual clinical translation. We also highlight unmet challenges in fetal surgery that could particularly benefit from novel biomaterials, including fetal membrane sealing and minimally invasive myelomeningocele defect repair. Finally, we conclude with a discussion of the underdeveloped fetal immune system and opportunities for exploitation with novel immunomodulating biomaterials.
MeSH term(s)	Biocompatible Materials ; Fetal Therapies/adverse effects ; Fetal Therapies/methods ; Fetus/immunology ; Fetus/surgery ; Humans ; Immunity ; Risk
Chemical Substances	Biocompatible Materials
Language	English
Publishing date	2019-05-17
Publishing country	England
Document type	Journal Article ; Review
ZDB-ID	2693928-9
ISSN	2047-4849 ; 2047-4830
ISSN (online)	2047-4849
ISSN	2047-4830
DOI	10.1039/c9bm00177h
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Marine-Inspired Polymers in Medical Adhesion.

Balkenende, Diederik W R / Winkler, Sally M / Messersmith, Phillip B

European polymer journal

2019 Volume 116, Page(s) 134–143

Abstract: Medical adhesives that are strong, easy to apply and biocompatible are promising alternatives to sutures and staples in a large variety of surgical and clinical procedures. Despite progress in the development and regulatory approval of adhesives for use ... ...

Abstract	Medical adhesives that are strong, easy to apply and biocompatible are promising alternatives to sutures and staples in a large variety of surgical and clinical procedures. Despite progress in the development and regulatory approval of adhesives for use in the clinic, adhesion to wet tissue remains challenging. Marine organisms have evolved a diverse set of highly effective wet adhesive approaches that have inspired the design of new medical adhesives. Here we provide an overview of selected marine animals and their chemical and physical adhesion strategies, the state of clinical translation of adhesives inspired by these organisms, and target applications where marine-inspired adhesives can have a significant impact. We will focus on medical adhesive polymers inspired by mussels, sandcastle worms, and cephalopods, emphasize the history of bioinspired medical adhesives from the peer reviewed and patent literature, and explore future directions including overlooked sources of bioinspiration and materials that exploit multiple bioinspired strategies.
Keywords	covid19
Language	English
Publishing date	2019-04-04
Publishing country	United States
Document type	Journal Article
ZDB-ID	1483529-0
ISSN	0014-3057
ISSN	0014-3057
DOI	10.1016/j.eurpolymj.2019.03.059
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Article ; Online: Imaging of adeno-associated viral capsids for purposes of gene editing using CEST NMR/MRI.

Lam, Bonnie / Velasquez, Mark / Ogiyama, Tomoko / Godines, Kevin / Szu, Fan-Yun / Velasquez-Mao, A J / AlGhuraibawi, Wissam / Wang, Jingshen / Messersmith, Phillip B / Vandsburger, Moriel H

Magnetic resonance in medicine

2024

Abstract: Purpose: Gene therapy using adeno-associated virus (AAV) vector-mediated gene delivery has undergone substantial growth in recent years with promising results in both preclinical and clinical studies, as well as emerging regulatory approval. However, ... ...

Abstract	Purpose: Gene therapy using adeno-associated virus (AAV) vector-mediated gene delivery has undergone substantial growth in recent years with promising results in both preclinical and clinical studies, as well as emerging regulatory approval. However, the inability to quantify the efficacy of gene therapy from cellular delivery of gene-editing technology to specific functional outcomes is an obstacle for efficient development of gene therapy treatments. Building on prior works that used the CEST reporter gene lysine rich protein, we hypothesized that AAV viral capsids may generate endogenous CEST contrast from an abundance of surface lysine residues. Methods: NMR experiments were performed on isolated solutions of AAV serotypes 1-9 on a Bruker 800-MHz vertical scanner. In vitro experiments were performed for testing of CEST-NMR contrast of AAV2 capsids under varying pH, density, biological transduction stage, and across multiple serotypes and mixed biological media. Reverse transcriptase-polymerase chain reaction was used to quantify virus concentration. Subsequent experiments at 7 T optimized CEST saturation schemes for AAV contrast detection and detected AAV2 particles encapsulated in a biocompatible hydrogel administered in the hind limb of mice. Results: CEST-NMR experiments revealed CEST contrast up to 52% for AAV2 viral capsids between 0.6 and 0.8 ppm. CEST contrast generated by AAV2 demonstrated high levels of CEST contrast across a variety of chemical environments, concentrations, and saturation schemes. AAV2 CEST contrast displayed significant positive correlations with capsid density (R Conclusion: AAV2 viral capsids exhibit strong capacity as an endogenous CEST contrast agent and can potentially be used for monitoring and evaluation of AAV vector-mediated gene therapy protocols.
Language	English
Publishing date	2024-04-23
Publishing country	United States
Document type	Journal Article
ZDB-ID	605774-3
ISSN	1522-2594 ; 0740-3194
ISSN (online)	1522-2594
ISSN	0740-3194
DOI	10.1002/mrm.30058
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Article ; Online: Supramolecular Cross-Links in Mussel-Inspired Tissue Adhesives.

Balkenende, Diederik W R / Winkler, Sally M / Li, Yiran / Messersmith, Phillip B

ACS macro letters

2020 Volume 9, Issue 10, Page(s) 1439–1445

Abstract: Here we introduce a tissue-adhesive patch with orthogonal cohesive and adhesive chemistries; supramolecular ureido-4-pyrimidinone (UPy) cross-links provide cohesive strength, and catechols provide mussel-inspired tissue adhesion. In the development of ... ...

Abstract	Here we introduce a tissue-adhesive patch with orthogonal cohesive and adhesive chemistries; supramolecular ureido-4-pyrimidinone (UPy) cross-links provide cohesive strength, and catechols provide mussel-inspired tissue adhesion. In the development of tissue-adhesive biomaterials, prior research has focused on forming strong adhesive interfaces in wet conditions, leaving the use of supramolecular cross-links for cohesive strength underexplored. In developing this adhesive patch, the influence of the comonomers' composition and amphiphilicity on adhesion was investigated by lap shear adhesion to wet tissue. We determined failed lap joints' failure mechanism using catechol-specific Arnow's stain and identified formulations with improved cohesive strength. The adhesive materials were cytocompatible in mammalian cell conditioned media viability studies. We found that using orthogonal motifs to independently control adhesives' cohesive and adhesive strengths resulted in stronger tissue adhesion. The design principles presented here advance the development of wet tissue adhesives and could allow for the future design of biomaterials with desirable stimuli-responsive properties.
Language	English
Publishing date	2020-09-21
Publishing country	United States
Document type	Journal Article
ISSN	2161-1653
ISSN (online)	2161-1653
DOI	10.1021/acsmacrolett.0c00520
Database	MEDical Literature Analysis and Retrieval System OnLINE

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