Enzyme cascade reaction involving lytic polysaccharide monooxygenase and dye-decolorizing peroxidase for chitosan functionalization
Enzyme cascade reaction involving lytic polysaccharide monooxygenase and dye-decolorizing peroxidase for chitosan functionalization
复制标题
涉及裂解多糖单加氧酶和染料脱色过氧化物酶的酶级联反应用于壳聚糖功能化
DOI：
10.1021/acs.jafc.0c06856
复制
发表时间：
2021
影响因子：
6.1
通讯作者：
Yu Hongbo
中科院分区：
文献类型：
--
作者：
Li Fei;Shao Ruijian;Mao Yingzheng;Yu Wen;Yu Hongbo
原位H2 O2生成系统对于H2 O2依赖的生物催化氧化反应是有效的。在这里，我们报告，溶解性多糖单加氧酶（LPMO），铜依赖性多糖单加氧酶，可以有效地提供过氧化氢原位染料脱色过氧化物酶（DyPs）使用底物没食子酸（GA）的壳聚糖功能化。由级联反应诱导的最大接枝率显着高于通过与初始外源H2 O2的反应实现的接枝率。当GA为12 g/L，DyP为5.6 mg/L，LPMO为20-30 mg/L，pH为4.5 ~ 5.0时，接枝率最高。紫外-可见光谱、傅里叶变换红外光谱和核磁共振氢谱证实了GA接枝到壳聚糖上。X射线衍射（XRD）分析和热重分析（TGA）表明，GA-壳聚糖偶联物的热稳定性和结晶度低于壳聚糖。GA-壳聚糖偶联物的抗氧化活性显著高于壳聚糖。该研究为实现壳聚糖功能化的酶促级联反应提供了一种绿色、高效的途径，在H2 O2依赖的生物催化氧化反应中具有潜在的应用价值。
In situH2O2generation systems are efficient for H2O2-dependent biocatalytic oxidation reactions. Here, we report that lytic polysaccharide monooxygenases (LPMOs), copper-dependent polysaccharide monooxygenases, can efficiently supply H2O2in situto dye-decolorizing peroxidases (DyPs) using substrate gallic acid (GA) for chitosan functionalization. The maximum grafting ratio induced by the cascade reaction was significantly higher than that achieved by a reaction with initial exogenous H2O2. The maximum grafting ratio was obtained with 12 g/L GA, 5.6 mg/L DyP, 20–30 mg/L LPMO, and pH 4.5–5.0. UV–vis, Fourier transform infrared (FT-IR), and nuclear magnetic resonance (1H NMR) spectroscopy confirmed GA grafting onto chitosan. X-ray diffraction (XRD) analysis and thermogravimetric analysis (TGA) indicated that GA–chitosan conjugates had lower thermal stability and crystallinity than chitosan. The GA–chitosan conjugates had significantly higher antioxidant activity than chitosan. This study supplies a green and high-efficiency approach to achieve an enzymatic cascade reaction for chitosan functionalization and has potential applications in H2O2-dependent biocatalytic oxidation reactions.