Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-09-12 , DOI: 10.1016/j.cej.2020.127003 Yibo Zhang , Peng Hu , Yaseen Muhammad , Ying Tang , Shan Shao , Zhu Gao , Jiaxing Wang , Ruimeng Wang , Yang Hu , Lihan Kuang , Zhongxing Zhao , Zhenxia Zhao
Hollow nano-sphere NH2-MIL88(Fe) (HS NMIL88(Fe)) with interfacial defects was fabricated to load laccase as a host. Through metal multi-coordination, dopamine engineered large amount of defective pores with large size on NH2-MIL88(Fe) interface. This defect-interfacial structure provided a high-density host for laccases, which efficiently protected enzyme from structure deformation and then inhibited inactivation. Besides, the unique hollow structure will help to fasten reactant diffusivity, and thus improved the catalytic reaction process. Experimental results showed that the maximum immobilized capacity and maximum activity recovery for laccase reached up to 213.2 mg/g and 75.8% beyond many state-of-the-art enzyme hosts, respectively. Meanwhile, the immobilized laccase exhibited better pH, thermal and storage stabilities on HS NMIL88(Fe) than free and loaded on NMIL88(Fe) ones. Thermal deactivation kinetics analysis showed that HS NMIL88(Fe)-Lac had much higher apparent activation energies of (105.2 kJ/mol) than that of free laccase (89.2 kJ/mol). Catalyzing decolorization performance of dye Remazol Brilliant Blue R (RBBR) was finally carried out and exhibited the decolorization rate of 1.8 times and 2.6 times faster than solid NMIL88(Fe)-Lac and free laccase, respectively. Moreover, the interaction mechanism of laccase for RBBR was investigated and revealed by molecular docking.
中文翻译:
高密度固定化漆酶在具有界面缺陷的空心纳米球NH 2 -MIL88(Fe)基质上,以提高酶活性和Remazol亮蓝R脱色的稳定性
制备具有界面缺陷的空心纳米球NH 2 -MIL88(Fe)(HS NMIL88(Fe))以负载漆酶作为基质。通过金属多配位,多巴胺在NH 2上修饰出大量大尺寸的缺陷孔-MIL88(Fe)接口。这种缺陷界面结构为漆酶提供了高密度宿主,可有效保护酶免于结构变形,然后抑制失活。此外,独特的中空结构将有助于加快反应物的扩散性,从而改善催化反应过程。实验结果表明,漆酶的最大固定化容量和最大活性回收率分别比许多最先进的酶宿主高出213.2 mg / g和75.8%。同时,固定的漆酶在HS NMIL88(Fe)上表现出比游离和负载在NMIL88(Fe)上更好的pH,热稳定性和储存稳定性。热失活动力学分析表明,HS NMIL88(Fe)-Lac的表观活化能(105.2 kJ / mol)比游离漆酶(89.2 kJ / mol)高得多。最终实现了染料Remazol亮蓝R(RBBR)的催化脱色性能,其脱色速率分别比固体NMIL88(Fe)-Lac和游离漆酶快1.8倍和2.6倍。此外,通过分子对接研究了漆酶与RBBR的相互作用机理。