{"title":"酶固定化氧铵纳米凝胶：增强酶稳定性和可重复使用的生物相容性和可注射平台。","authors":"Suman Basak, Tushar Kanti Das","doi":"10.1021/acs.biomac.5c01625","DOIUrl":null,"url":null,"abstract":"<p><p>We report redox-responsive, oxoammonium-functionalized nanogels for mild, injectable, noncovalent enzyme immobilization. Amphiphilic PEG-<i>b</i>-poly(PMA-<i>co</i>-GMA) prepared by Reversible Addition-Fragmentation Chain Transfer (RAFT) polymerization was oxidized to nitroxide/oxoammonium states, forming nanogels that electrostatically complex with anionic proteins. Increasing oxoammonium content (30-70%) boosted encapsulation (85-98%) and loading (26-47%). Lipase and paraoxonase-1 (PON1) retained or exceeded native activity; the highest-charge formulation delivered 2.5-5-fold higher specific activity and >80% activity after five reuse cycles. Circular dichroism (CD) and polymer-only controls verified preserved secondary structure and no background catalysis. Reduction of pendant oxoammonium groups with glutathione, followed by mild acidification (pH 6) regenerated neutral nitroxides and triggered release. The nanogels were colloidally stable, shear-thinning, and cytocompatible (>90% cell viability), and PON1-loaded gels showed potent antioxidant and lipid-protective effects. This tunable, biocompatible platform stabilizes and recycles enzymes under gentle aqueous conditions and enables on-demand release for therapeutic delivery and biocatalysis.</p>","PeriodicalId":30,"journal":{"name":"Biomacromolecules","volume":" ","pages":""},"PeriodicalIF":5.4000,"publicationDate":"2025-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enzyme-Immobilized Oxoammonium Nanogels: A Biocompatible and Injectable Platform for Enhanced Enzyme Stability and Reusability.\",\"authors\":\"Suman Basak, Tushar Kanti Das\",\"doi\":\"10.1021/acs.biomac.5c01625\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>We report redox-responsive, oxoammonium-functionalized nanogels for mild, injectable, noncovalent enzyme immobilization. Amphiphilic PEG-<i>b</i>-poly(PMA-<i>co</i>-GMA) prepared by Reversible Addition-Fragmentation Chain Transfer (RAFT) polymerization was oxidized to nitroxide/oxoammonium states, forming nanogels that electrostatically complex with anionic proteins. Increasing oxoammonium content (30-70%) boosted encapsulation (85-98%) and loading (26-47%). Lipase and paraoxonase-1 (PON1) retained or exceeded native activity; the highest-charge formulation delivered 2.5-5-fold higher specific activity and >80% activity after five reuse cycles. Circular dichroism (CD) and polymer-only controls verified preserved secondary structure and no background catalysis. Reduction of pendant oxoammonium groups with glutathione, followed by mild acidification (pH 6) regenerated neutral nitroxides and triggered release. The nanogels were colloidally stable, shear-thinning, and cytocompatible (>90% cell viability), and PON1-loaded gels showed potent antioxidant and lipid-protective effects. This tunable, biocompatible platform stabilizes and recycles enzymes under gentle aqueous conditions and enables on-demand release for therapeutic delivery and biocatalysis.</p>\",\"PeriodicalId\":30,\"journal\":{\"name\":\"Biomacromolecules\",\"volume\":\" \",\"pages\":\"\"},\"PeriodicalIF\":5.4000,\"publicationDate\":\"2025-10-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Biomacromolecules\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.biomac.5c01625\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"BIOCHEMISTRY & MOLECULAR BIOLOGY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Biomacromolecules","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.biomac.5c01625","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"BIOCHEMISTRY & MOLECULAR BIOLOGY","Score":null,"Total":0}
Enzyme-Immobilized Oxoammonium Nanogels: A Biocompatible and Injectable Platform for Enhanced Enzyme Stability and Reusability.
We report redox-responsive, oxoammonium-functionalized nanogels for mild, injectable, noncovalent enzyme immobilization. Amphiphilic PEG-b-poly(PMA-co-GMA) prepared by Reversible Addition-Fragmentation Chain Transfer (RAFT) polymerization was oxidized to nitroxide/oxoammonium states, forming nanogels that electrostatically complex with anionic proteins. Increasing oxoammonium content (30-70%) boosted encapsulation (85-98%) and loading (26-47%). Lipase and paraoxonase-1 (PON1) retained or exceeded native activity; the highest-charge formulation delivered 2.5-5-fold higher specific activity and >80% activity after five reuse cycles. Circular dichroism (CD) and polymer-only controls verified preserved secondary structure and no background catalysis. Reduction of pendant oxoammonium groups with glutathione, followed by mild acidification (pH 6) regenerated neutral nitroxides and triggered release. The nanogels were colloidally stable, shear-thinning, and cytocompatible (>90% cell viability), and PON1-loaded gels showed potent antioxidant and lipid-protective effects. This tunable, biocompatible platform stabilizes and recycles enzymes under gentle aqueous conditions and enables on-demand release for therapeutic delivery and biocatalysis.
期刊介绍：
Biomacromolecules is a leading forum for the dissemination of cutting-edge research at the interface of polymer science and biology. Submissions to Biomacromolecules should contain strong elements of innovation in terms of macromolecular design, synthesis and characterization, or in the application of polymer materials to biology and medicine.
Topics covered by Biomacromolecules include, but are not exclusively limited to: sustainable polymers, polymers based on natural and renewable resources, degradable polymers, polymer conjugates, polymeric drugs, polymers in biocatalysis, biomacromolecular assembly, biomimetic polymers, polymer-biomineral hybrids, biomimetic-polymer processing, polymer recycling, bioactive polymer surfaces, original polymer design for biomedical applications such as immunotherapy, drug delivery, gene delivery, antimicrobial applications, diagnostic imaging and biosensing, polymers in tissue engineering and regenerative medicine, polymeric scaffolds and hydrogels for cell culture and delivery.
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