In Situ Ionically Cross-Linkable Benzaldehyde-Modified Alginate and Its Bilayer Structure as a Tissue Sealant for Dural Closure

I-Hsuan Yang; Natsuko F. Inagaki; Arvind K. Singh Chandel; Mifuyu Matsumoto; Mai Yamada; Kazuki Matsumiya; Yizhou Dai; Takaya Iwabuchi; Kotaro Onishi; Sonoko Fukushima; Seiichi Ohta; Akihiro Mizushima; Mitsuko Isaji; Satoshi Shimizu; Masahiko Takahata; Norimasa Iwasaki; Taichi Ito

doi:10.1021/acs.biomac.5c00748

In Situ Ionically Cross-Linkable Benzaldehyde-Modified Alginate and Its Bilayer Structure as a Tissue Sealant for Dural Closure

I-Hsuan Yang, Natsuko F. Inagaki, Arvind K. Singh Chandel, Mifuyu Matsumoto, Mai Yamada, Kazuki Matsumiya, Yizhou Dai, Takaya Iwabuchi, Kotaro Onishi, Sonoko Fukushima, Seiichi Ohta, Akihiro Mizushima, Mitsuko Isaji, Satoshi Shimizu, Masahiko Takahata, Norimasa Iwasaki, Taichi Ito

School of Engineering

Research output: Contribution to journal › Article › peer-review

Abstract

Effective tissue adhesives are vital for surgical applications. We synthesized p-aminobenzaldehyde-modified alginate (AL-ABA) with controlled degrees of substitution (DS, 3.8–13.7%) and cross-linked it ionically using CaCl₂. AL-ABA solutions (3 w/v %) gelled rapidly (3–50 s), similar to unmodified alginate. Increasing DS reduced hydrogel stiffness but enhanced dura adhesiveness via Schiff’s base formation with tissue amines, reaching 32 kPa at 9% DS. To optimize both adhesion and mechanical integrity, bilayer hydrogels were developed using an AL-ABA primer and AL cover layer, seamlessly bonded by ionic cross-linking. These AL-ABA/AL hydrogels showed strong dural adhesion and high burst pressure resistance (up to 406 mmHg). AL-ABA retained a low cytotoxicity and hemocompatibility. Ionically cross-linked AL-ABA and its bilayer configuration offer promising potential as biocompatible and efficient tissue sealants.

Original language	English
Pages (from-to)	5888-5902
Number of pages	15
Journal	Biomacromolecules
Volume	26
Issue number	9
DOIs	https://doi.org/10.1021/acs.biomac.5c00748
Publication status	Published - 8 Sep 2025

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Yang, I.-H., Inagaki, N. F., Chandel, A. K. S., Matsumoto, M., Yamada, M., Matsumiya, K., Dai, Y., Iwabuchi, T., Onishi, K., Fukushima, S., Ohta, S., Mizushima, A., Isaji, M., Shimizu, S., Takahata, M., Iwasaki, N., & Ito, T. (2025). In Situ Ionically Cross-Linkable Benzaldehyde-Modified Alginate and Its Bilayer Structure as a Tissue Sealant for Dural Closure. Biomacromolecules, 26(9), 5888-5902. https://doi.org/10.1021/acs.biomac.5c00748

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title = "In Situ Ionically Cross-Linkable Benzaldehyde-Modified Alginate and Its Bilayer Structure as a Tissue Sealant for Dural Closure",

abstract = "Effective tissue adhesives are vital for surgical applications. We synthesized p-aminobenzaldehyde-modified alginate (AL-ABA) with controlled degrees of substitution (DS, 3.8–13.7\%) and cross-linked it ionically using CaCl2. AL-ABA solutions (3 w/v \%) gelled rapidly (3–50 s), similar to unmodified alginate. Increasing DS reduced hydrogel stiffness but enhanced dura adhesiveness via Schiff{\textquoteright}s base formation with tissue amines, reaching 32 kPa at 9\% DS. To optimize both adhesion and mechanical integrity, bilayer hydrogels were developed using an AL-ABA primer and AL cover layer, seamlessly bonded by ionic cross-linking. These AL-ABA/AL hydrogels showed strong dural adhesion and high burst pressure resistance (up to 406 mmHg). AL-ABA retained a low cytotoxicity and hemocompatibility. Ionically cross-linked AL-ABA and its bilayer configuration offer promising potential as biocompatible and efficient tissue sealants.",

author = "I-Hsuan Yang and Inagaki, \{Natsuko F.\} and Chandel, \{Arvind K. Singh\} and Mifuyu Matsumoto and Mai Yamada and Kazuki Matsumiya and Yizhou Dai and Takaya Iwabuchi and Kotaro Onishi and Sonoko Fukushima and Seiichi Ohta and Akihiro Mizushima and Mitsuko Isaji and Satoshi Shimizu and Masahiko Takahata and Norimasa Iwasaki and Taichi Ito",

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year = "2025",

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day = "8",

doi = "10.1021/acs.biomac.5c00748",

language = "English",

volume = "26",

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Yang, I-H, Inagaki, NF, Chandel, AKS, Matsumoto, M, Yamada, M, Matsumiya, K, Dai, Y, Iwabuchi, T, Onishi, K, Fukushima, S, Ohta, S, Mizushima, A, Isaji, M, Shimizu, S, Takahata, M, Iwasaki, N & Ito, T 2025, 'In Situ Ionically Cross-Linkable Benzaldehyde-Modified Alginate and Its Bilayer Structure as a Tissue Sealant for Dural Closure', Biomacromolecules, vol. 26, no. 9, pp. 5888-5902. https://doi.org/10.1021/acs.biomac.5c00748

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T1 - In Situ Ionically Cross-Linkable Benzaldehyde-Modified Alginate and Its Bilayer Structure as a Tissue Sealant for Dural Closure

AU - Yang, I-Hsuan

AU - Inagaki, Natsuko F.

AU - Chandel, Arvind K. Singh

AU - Matsumoto, Mifuyu

AU - Yamada, Mai

AU - Matsumiya, Kazuki

AU - Dai, Yizhou

AU - Iwabuchi, Takaya

AU - Onishi, Kotaro

AU - Fukushima, Sonoko

AU - Ohta, Seiichi

AU - Mizushima, Akihiro

AU - Isaji, Mitsuko

AU - Shimizu, Satoshi

AU - Takahata, Masahiko

AU - Iwasaki, Norimasa

AU - Ito, Taichi

PY - 2025/9/8

Y1 - 2025/9/8

N2 - Effective tissue adhesives are vital for surgical applications. We synthesized p-aminobenzaldehyde-modified alginate (AL-ABA) with controlled degrees of substitution (DS, 3.8–13.7%) and cross-linked it ionically using CaCl2. AL-ABA solutions (3 w/v %) gelled rapidly (3–50 s), similar to unmodified alginate. Increasing DS reduced hydrogel stiffness but enhanced dura adhesiveness via Schiff’s base formation with tissue amines, reaching 32 kPa at 9% DS. To optimize both adhesion and mechanical integrity, bilayer hydrogels were developed using an AL-ABA primer and AL cover layer, seamlessly bonded by ionic cross-linking. These AL-ABA/AL hydrogels showed strong dural adhesion and high burst pressure resistance (up to 406 mmHg). AL-ABA retained a low cytotoxicity and hemocompatibility. Ionically cross-linked AL-ABA and its bilayer configuration offer promising potential as biocompatible and efficient tissue sealants.

AB - Effective tissue adhesives are vital for surgical applications. We synthesized p-aminobenzaldehyde-modified alginate (AL-ABA) with controlled degrees of substitution (DS, 3.8–13.7%) and cross-linked it ionically using CaCl2. AL-ABA solutions (3 w/v %) gelled rapidly (3–50 s), similar to unmodified alginate. Increasing DS reduced hydrogel stiffness but enhanced dura adhesiveness via Schiff’s base formation with tissue amines, reaching 32 kPa at 9% DS. To optimize both adhesion and mechanical integrity, bilayer hydrogels were developed using an AL-ABA primer and AL cover layer, seamlessly bonded by ionic cross-linking. These AL-ABA/AL hydrogels showed strong dural adhesion and high burst pressure resistance (up to 406 mmHg). AL-ABA retained a low cytotoxicity and hemocompatibility. Ionically cross-linked AL-ABA and its bilayer configuration offer promising potential as biocompatible and efficient tissue sealants.

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In Situ Ionically Cross-Linkable Benzaldehyde-Modified Alginate and Its Bilayer Structure as a Tissue Sealant for Dural Closure

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