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真菌漆酶引导的铜纳米花组装可实现将5-羟甲基糠醛完全转化为2,5-呋喃二甲酸。

Fungal laccase-guided copper nanoflower assembly enables complete conversion of HMF to FDCA.

作者信息

Yang Lei, Duan Anbang, Ding Yuan, Song Xiquan, Ma Qianli, Liu Zhanyin, Wei Tingying, Wang Zhixing, Liu Chunzhao

机构信息

State Key Laboratory of Bio-fibers and Eco-Textiles, Institute of Biochemical Engineering, The 3rd Clinical College of Qingdao University, College of Materials Science and Engineering, Qingdao University Qingdao 266071 China

Department of Sports Medicine, Qingdao Municipal Hospital Qingdao 266071 China.

出版信息

RSC Adv. 2025 Aug 21;15(36):29692-29702. doi: 10.1039/d5ra04187b. eCollection 2025 Aug 18.

Abstract

The growing demand for sustainable biomanufacturing has driven significant interest in 2,5-furandicarboxylic acid (FDCA), a bio-based platform chemical for producing renewable polymers. The eco-friendly oxidoreductase laccase exhibits promising FDCA biosynthesis capacity yet is hampered by pH-dependent activity decay and susceptibility to proteolytic degradation. Herein, we developed a bio-enabled synthesis approach to fabricate three-dimensional laccase-integrated copper hybrid nanoflowers (Lac-NFs) through enzyme-metal coordination-driven self-assembly. The engineered Lac-NFs displayed high enzyme encapsulation efficiency (89.28%) and enhanced environmental robustness compared to free laccase. Furthermore, the Lac-NFs maintained prolonged storage stability with well-preserved activity relative to the native enzyme. Elevated catalytic efficiency and refined enzymatic kinetics were achieved copper-mediated electron transfer networks within the hybrid matrix. Remarkably, Lac-NFs demonstrate exceptional catalytic efficiency and selectivity in the conversion of HMF to FDCA, achieving complete substrate conversion under precisely controlled operational parameters. This nano-biohybrid design establishes a robust and efficient biocatalytic platform for biomass valorization into high-value-added chemicals, exhibiting promising scalability prospects for industrial implementation.

摘要

对可持续生物制造日益增长的需求引发了人们对2,5-呋喃二甲酸(FDCA)的浓厚兴趣,它是一种用于生产可再生聚合物的生物基平台化学品。环保型氧化还原酶漆酶展现出了有前景的FDCA生物合成能力,但受到pH依赖性活性衰减和蛋白水解降解敏感性的阻碍。在此,我们开发了一种生物合成方法,通过酶-金属配位驱动的自组装来制备三维漆酶整合铜杂化纳米花(Lac-NFs)。与游离漆酶相比,工程化的Lac-NFs表现出高酶包封效率(89.28%)和增强的环境稳定性。此外,相对于天然酶,Lac-NFs保持了延长的储存稳定性且活性良好。通过杂化基质内铜介导的电子转移网络实现了催化效率的提高和酶动力学的优化。值得注意的是,Lac-NFs在将HMF转化为FDCA的过程中表现出卓越的催化效率和选择性,在精确控制的操作参数下实现了底物的完全转化。这种纳米生物杂化设计建立了一个强大而高效的生物催化平台,用于将生物质转化为高附加值化学品,展现出了工业应用的良好可扩展性前景。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/cb99/12376868/84f03780b41a/d5ra04187b-f1.jpg

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