Enzyme-Immobilized Oxoammonium Nanogels: A Biocompatible and Injectable Platform for Enhanced Enzyme Stability and Reusability.

IF 5.4 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY

Biomacromolecules Pub Date : 2025-10-03 DOI:10.1021/acs.biomac.5c01625

Suman Basak, Tushar Kanti Das

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引用次数: 0

Abstract

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.

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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。

我们报道氧化还原反应，氧铵功能化纳米凝胶用于温和的，可注射的，非共价酶固定化。通过可逆加成-断裂链转移（RAFT）聚合制备的两亲性PEG-b-poly（PMA-co-GMA）被氧化为氮氧/氧铵态，形成与阴离子蛋白静电络合的纳米凝胶。增加氧铵含量（30-70%）可提高包封率（85-98%）和装填率（26-47%）。脂肪酶和对氧磷酶-1 （PON1）保持或超过天然活性；最高电荷的配方在5次重复使用循环后比活性提高2.5-5倍，活性达到80%。圆二色性（CD）和仅聚合物对照验证了保留的二级结构和无背景催化。用谷胱甘肽还原悬垂的氧铵基团，然后轻度酸化（pH 6）再生中性氮氧化物并触发释放。纳米凝胶具有胶体稳定性、剪切减薄性和细胞相容性（细胞存活率为90%），并且负载pon1的凝胶具有有效的抗氧化和脂质保护作用。这种可调的、生物相容的平台在温和的水条件下稳定和回收酶，并实现治疗递送和生物催化的按需释放。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Biomacromolecules 化学-高分子科学

CiteScore

10.60

自引率

4.80%

发文量

417

审稿时长

1.6 months

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.