• 关键词：己烯雌酚  漆酶  分子对接  分子动力学模拟  响应面分析法

• 基金项目：国家自然科学基金（No.21467006）；广西壮族自治区特聘专家团队项目（厅发[2018]39）；广西环境污染控制理论与技术重点实验室研究基金（No.1701K003）

• 刘红艳
• 桂林理工大学化学与生物工程学院, 桂林 541006

• 谢世伟
• 桂林理工大学化学与生物工程学院, 桂林 541006

• 唐琳
• 桂林理工大学化学与生物工程学院, 桂林 541006

• 张文强
• 1. 桂林理工大学化学与生物工程学院, 桂林 541006;2. 广西环境污染控制理论与技术重点实验室, 桂林 541006

• 张国琴
• 桂林理工大学化学与生物工程学院, 桂林 541006

• 朱义年
• 广西环境污染控制理论与技术重点实验室, 桂林 541006

• 单杨
• 1. 桂林理工大学化学与生物工程学院, 桂林 541006;2. 湖南省农业科学院, 湖南农产品加工研究所, 长沙 410125

• 摘要：己烯雌酚（Diethylstilbestrol，DES）作为水环境中最具雌激素活性的合成化合物之一，其给生物体和环境带来的危害已经引起人们的关注.本研究首先通过分子对接与分子动力学模拟从理论上分析漆酶与DES的相互作用；其次通过实验分析其降解动力学模型及不同反应条件和介质对漆酶催化转化DES的影响；最后使用响应面分析方法优化漆酶-ABTS系统催化转化DES的最佳条件.计算结果表明，漆酶与DES的反应能够自发进行且它们之间主要存在氢键和疏水作用力.实验结果表明，反应6 h左右，50 mg·L^-1的DES的降解率达到93%以上；根据Michaelis-Menten模型得到的动力学参数K_m和V_max分别为36.18 mg·L^-1和45.98 mg·L^-1·h^-1，模型的R²为0.99.漆酶催化降解DES的最佳pH为6，最佳温度为55℃.几种介质中，ABTS对漆酶催化降解DES的作用最强.通过响应面分析发现，在pH=5.5、55.98℃、1.52 mmol·L^-1 ABTS、31.52 mg·L^-1 DES的条件下，反应0.5 h后ABTS-漆酶系统可将DES完全降解.本研究可为漆酶催化转化DES提供理论基础和实验方法.

• Abstract：Diethylstilbestrol (DES) is one of the most estrogenic active compounds in aquatic environment, and its harmful to organisms and environment has attracted people's attention. In this study, we firstly, analyzed the interaction between laccase and DES by molecular docking and molecular dynamics simulation. Secondly, the degradation kinetics model and the effects of different reaction conditions and medium on the catalytic conversion of DES by laccase were analyzed.Finally, the response surface analysis method was used to optimize the optimal conditions for the catalytic conversion of DES by the laccase-ABTS system. The results of calculations showed that the reaction of laccase with DES can occur spontaneously and there were mainly hydrogen bonds and hydrophobic interactions between them. The experimental results showed that the degradation rate of 50 mg·L^-1 DES can reach more than 93% in about 6 hours. According to the Michaelis-Menten model, the kinetic parameters K_m and V_max were 36.18 mg·L^-1 and 45.98 mg·L^-1·h^-1, respectively, The coefficient of determination (R²) of the model was 0.99. The optimum pH for laccase-catalyzed degradation of DES was 6, and the optimum temperature was 55 ℃. In the study of several mediators, ABTS was found to have the strongest effect on catalyzed degradation of DES by laccase. Response surface analysis revealed that the ABTS-laccase system completely degraded DES after half an hour of reaction at pH=5.5, 55.98 ℃, 1.52 mmol·L^-1 ABTS, and 31.52 mg·L^-1 DES. This study provides a theoretical basis and experimental method for the catalytic conversion of DES by laccase.

• Key words：diethylstilbestrol  laccase  molecular docking  molecular dynamics simulation  response surface analysis method

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