基于包埋法固定化漆酶的酶学性质及其催化氧化海水养殖废水中四环素的效能与途径  

Enzymatic Properties of Immobilized Laccase by Embedding Method and Its Catalytic Oxidation Efficiency and Pathway of Tetracycline in Marine Aquaculture Wastewater

作　　者：张思敏 金春姬[1,2] 吴香梅 赵阳国[1,2] 佘宗莲[1,2] Zhang Simin;JIN Chunji;Wu Xiangmei;Zhao Yangguo;She Zonglian(College of Environmental Science and Engineering,Ocean University of China,Qingdao 266100,China;The Key Laboratory of Marine Environmental Science and Ecology,Ministry of Education,Ocean University of China,Qingdao 266100,China)

机构地区：[1]中国海洋大学环境科学与工程学院,山东青岛266100 [2]中国海洋大学海洋环境与生态教育部重点实验室,山东青岛266100

出　　处：《中国海洋大学学报（自然科学版）》2023年第11期111-120,共10页Periodical of Ocean University of China

基　　金：中央高校基本科研业务费专项(201964004)资助。

摘　　要：本研究以海藻酸钠、聚乙烯醇、明胶作为包埋材料,活性炭作为吸附剂,采用吸附-包埋法固定化漆酶,研究了游离漆酶和固定化漆酶的酶学性质,探讨了氧化还原介体类型及浓度、盐度对固定化漆酶降解四环素的影响,考察了四环素可能的降解途径。结果表明:与游离漆酶相比,固定化酶对pH和温度的变化表现出出色的适应能力,制备的固定化酶具有良好的热稳定性,60℃培养3 h后保留了其初始催化活性的76.31%,而游离漆酶仅保留不到20%的活性;4℃储存30 d固定化酶保留了51.41%的相对活性,表明固定化酶具有优异的储存稳定性。漆酶-SA系统在去除四环素(Tetracycline, TC)方面表现的更加优越,在3 mmol·L-1丁香醛(Syringaldehyde, SA)存在的条件下,固定化漆酶对四环素的去除率为91.69%;盐度影响漆酶处理四环素的效果,但在30的盐度条件下,固定化酶能达到接近90%的TC去除率,满足水质净化的需要,漆酶催化氧化四环素的最佳pH为7。运用超高效液相色谱质谱联用仪,分析了降解产物,认为氧化、脱氢、脱甲基是漆酶氧化四环素的主要反应过程。In this study,sodium alginate,polyvinyl alcohol and gelatin were used as embedding materials and activated carbon was used as adsorbent to immobilize laccase by adsorption-embedding method.The enzymatic properties of free laccase and immobilized laccase were studied.The effects of the type,concentration of redox mediators and salinity on the degradation of tetracycline by immobilized laccase were investigated,and the possible degradation pathways of tetracycline were investigated.The results showed that compared with free laccase,the immobilized enzyme showed excellent adaptability to pH and temperature changes.The prepared immobilized enzyme had good thermal stability and retained its 76.31%of initial catalytic activity after culturing at 60℃for 3 h,while the free laccase only retained less than 20%of the activity.The immobilized enzyme retained 51.41%of the relative activity stored at 4℃for 30 days,indicating that the immobilized enzyme has excellent storage stability.The laccase-SA system performed better in the removal of tetracycline.In the presence of 3 mmol·L-1 syringaldehyde(SA),the removal rate of tetracycline by immobilized laccase was 91.69%;salinity significantly affected the effect of laccase to treat tetracycline.Under the condition of salinity of 30‰,the immobilized enzyme can achieve a TC removal rate of nearly 90%,which meets the needs of water purification.The degradation products were analyzed by ultra-high performance liquid chromatography-mass spectrometry,and it was concluded that oxidation,dehydrogenation and demethylation were the main reaction processes of laccase to oxidize tetracycline.

关 键 词：漆酶 固定化 酶学性质 稳定性 四环素 降解途径 

分 类 号：X55[环境科学与工程—环境工程]