Yang Xue, Shi Fei, Su Xiaolei, Cavaco-Paulo Artur, Wang Hongbo, Su Jing
Jiangsu Engineering Technology Research Centre of Functional Textiles, Jiangnan University, Wuxi 214122, China.
Jiangsu Engineering Technology Research Centre of Functional Textiles, Jiangnan University, Wuxi 214122, China; Centre of Biological Engineering, University of Minho, Campus de Gualtar, 4710-057 Braga, Portugal.
Carbohydr Polym. 2023 Nov 15;320:121157. doi: 10.1016/j.carbpol.2023.121157. Epub 2023 Jun 28.
Enzymes with high catalytic activity and stability have been used for the sustainable development of green chemical applications, such as water remediation. Immobilized laccase can be used to construct a synergistic system for adsorption and degradation, which has great potential for water remediation. Herein, a hydrogen-bonded organic framework was installed onto laccase in-situ to form a net-carboxylate-arranged defective cage, which enhanced its catalytic stability. Thereafter, the CMC/PVA/Lac@HOF-101 hydrogel was fabricated by freeze-thaw cycles using sodium carboxymethylcellulose and polyvinyl alcohol as carriers and copper (II) as a cross-linker. Notably, the MOFs/hydrogel as a protective carrier of laccase maintain long-term recyclability and catalytic stability. After the fifth catalytic cycle, approximately 66.7 % activity of the CP-Lac@HOF-101 was retained. When both free laccase and CP-Lac@HOF-101 were used for decolorization of Acid Orange 7 (AO), the removal rates were 10.9 % and 82.5 % after 5 h, respectively. Furthermore, even in the presence of metal cations, almost 60.0 % of the AO removal efficiency was achieved. The relationship between the structure of the azo dyes and decolorization efficiency of the synergistic system was further investigated. This study offers a method for constructing enzyme@HOF-based composite hydrogels and provides a promising water remediation strategy.
具有高催化活性和稳定性的酶已被用于绿色化学应用的可持续发展,如水修复。固定化漆酶可用于构建吸附和降解的协同体系,在水修复方面具有巨大潜力。在此,一种氢键有机框架原位安装在漆酶上,形成了一种羧酸盐排列的缺陷笼状结构,提高了其催化稳定性。此后,以羧甲基纤维素钠和聚乙烯醇为载体、铜(II)为交联剂,通过冻融循环制备了CMC/PVA/Lac@HOF-101水凝胶。值得注意的是,作为漆酶保护载体的MOF/水凝胶保持了长期的可回收性和催化稳定性。在第五次催化循环后,CP-Lac@HOF-101仍保留了约66.7%的活性。当游离漆酶和CP-Lac@HOF-101都用于酸性橙7(AO)的脱色时,5小时后的去除率分别为10.9%和82.5%。此外,即使在存在金属阳离子的情况下,AO的去除效率也几乎达到了60.0%。进一步研究了偶氮染料结构与协同体系脱色效率之间的关系。本研究提供了一种构建基于酶@HOF的复合水凝胶的方法,并提供了一种有前景的水修复策略。