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. 2024 Jan 15;16(2):241.
doi: 10.3390/polym16020241.

Preparation and Characterization of Acrylic and Methacrylic Phospholipid-Mimetic Polymer Hydrogels and Their Applications in Optical Tissue Clearing

Nanako Dei  1 , Kazuhiko Ishihara  2 , Akikazu Matsumoto  1 , Chie Kojima  1
Affiliations

Preparation and Characterization of Acrylic and Methacrylic Phospholipid-Mimetic Polymer Hydrogels and Their Applications in Optical Tissue Clearing

Nanako Dei et al. Polymers (Basel). .

Abstract

The 2-methacryloyloxyethyl phosphorylcholine (MPC) polymers are mimetic to phospholipids, being widely used as biocompatible polymers. In our previous study, MPC polymer hydrogels proved more effective for optical tissue clearing compared to acrylamide (AAm) polymer hydrogels. In the present study, 2-acryloyloxyethyl phosphorylcholine (APC) was synthesized and employed to create hydrogels for a comparative analysis with methacrylic MPC-based hydrogels. APC, an acrylic monomer, was copolymerized with AAm in a similar reactivity. In contrast, MPC, as a methacrylic monomer, demonstrated higher copolymerization reactivity than AAm, leading to a spontaneously delayed two-step polymerization behavior. This suggests that the polymer sequences and network structures became heterogeneous when both methacrylic and acrylic monomers, as well as crosslinkers, were present in the copolymerization system. The molecular weight of the APC polymers was considerably smaller than that of the MPC polymers due to the formation of mid-chain radicals and subsequent β-scission during polymerization. The swelling ratios in water and strain sweep profiles of hydrogels prepared using acrylic and methacrylic compounds differed from those of hydrogels prepared using only acrylic compounds. This implies that copolymerization reactivity influences the polymer network structures and crosslinking density in addition to the copolymer composition. APC-based hydrogels are effective for the optical clearing of tumor tissues and are applicable to both passive and electrophoretic methods.

Keywords: copolymerization; hydrogel; optical tissue clearing; phosphorylcholine; viscoelasticity.

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Conflict of interest statement

The authors declare no conflicts of interest.

Figures

Figure 1
Figure 1
Structures of monomers and crosslinkers used in this study.
Figure 2
Figure 2
Time-conversion relationship for the (A) homopolymerization and (B) copolymerization systems of AAm, MPC, and APC.
Figure 3
Figure 3
Swelling ratios of various polymer hydrogels in water. The results of the PAAm, PMPC50, PMPC75, and PMPC-b hydrogels were referred to from [19]. ND: not determined.
Figure 4
Figure 4
Storage modulus (G′) and loss modulus (G″) of the (A) PMPC50 and (B) PAPC50 hydrogels versus strain sweep.
Figure 5
Figure 5
Elastic moduli of the PAAm, PAPC, and PMPC-b and PMPC-t hydrogels prepared at different crosslinker concentrations.
Figure 6
Figure 6
Elastic moduli of the (A) PMPC-b, (B) PAPC, and (C) PMPC-t hydrogels prepared at 19.5 mM crosslinker concentration versus strain sweep.
Figure 7
Figure 7
Optical clearing of tumor tissues using PAAm, PMPC75, PMPC-b, PAPC75, and PAPC hydrogels by the passive CLARITY method. The results in the left panel were referred to from [19].
Figure 8
Figure 8
Optical clearing of tumor tissues using PAPC and PMPC-b hydrogels by the electrophoresis-used CLARITY method.
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