冯义平,沈梦瑶,张伊健,高士祥.典型金属离子对漆酶催化降解溴代阻燃剂四溴双酚A的影响研究[J].环境科学学报,2020,40(6):2082-2089
典型金属离子对漆酶催化降解溴代阻燃剂四溴双酚A的影响研究
- Effect of metal ions on laccase-catalyzed degradation of tetrabromobisphenol A
- 基金项目：国家自然科学基金（No.21707019）；广州市科技计划（No.201804010396，201903010080）；广东省教育厅特色创新项目（No.2017KTSCX058）
- 冯义平
- 1. 广东工业大学环境科学与工程学院, 环境健康与污染控制研究院, 广州 510006;2. 南京大学环境学院, 污染控制与资源化研究国家重点实验室, 南京 210023
- 沈梦瑶
- 广东工业大学环境科学与工程学院, 环境健康与污染控制研究院, 广州 510006
- 张伊健
- 广东工业大学环境科学与工程学院, 环境健康与污染控制研究院, 广州 510006
- 高士祥
- 南京大学环境学院, 污染控制与资源化研究国家重点实验室, 南京 210023
- 摘要：研究了自然环境、垃圾渗滤液及工业废水中广泛存在的金属离子对真菌漆酶（Trametes versicolor）酶活性以及对漆酶催化降解典型溴代阻燃剂四溴双酚A（TBBPA）的影响.金属离子包括Na+、K+、Zn2+、Cd2+、Cu2+、Hg2+、Fe2+、Fe3+、Pb2+、Al3+能抑制漆酶酶活性和降低TBBPA的降解转化率，抑制效应随着金属离子浓度的升高而增大；Ca2+、Mg2+、Mn2+则对漆酶活性和TBBPA去除率均没有显著影响.金属离子的抑制作用主要是通过干扰漆酶的电子传递过程产生的.其中，Fe2+和Hg2+的抑制效应尤为明显，而二者的抑制机制不同，Fe2+竞争消耗O2，Hg2+则通过与漆酶结构中氨基酸络合，改变其构型从而抑制其活性.此外，通过加入介体物质2，2-联氮-二（3-乙基-苯并噻唑-6-磺酸）二铵盐（ABTS）、2，2，6，6-四甲基哌啶-氮-氧化物（TEMPO）等物质能够显著提高金属离子存在下漆酶对TBBPA的去除率.
- Abstract：In this study, the influences of different metal ions that present in natural water, industrial wastewater and landfill leachates on laccase (from Trametes versicolor) activity and laccase-catalyzed degradation of tetrabromobisphenol A (TBBPA) were examined. Metal ions including Na+、K+、Zn2+、Cd2+、Cu2+、Hg2+、Fe2+、Fe3+、Pb2+、Al3+ inhibited laccase activity and TBBPA degradation, and the inhibitions depend on metal ion species and concentrations. These metal ions affect laccase-catalyzed conversion of TBBPA through interrupting the electron transport system of laccase. However, because most metal ions inhibit the catalytic activity of laccase only at high concentration (e.g., 10 mmol·L-1), they would not influence laccase performance in natural water or wastewater water matrix. In particular, Fe2+ and Hg2+ substantially reduced TBBPA removal even at lower concentration (e.g., 10 μmol·L-1). The inhibition of Fe2+ was attributed to oxygen consumption, while the inhibition of Hg2+ occurred by binding with amino acid residues on laccase. In addition, 2, 2'-azino-bis (3-ethylbenz-thiazoline-6-sulfonic acid) (ABTS) and 2, 2, 6, 6-tetramethyl-1-piperidinyloxy free radical (TEMPO) as mediators were able to improve laccase-catalyzed degradation of TBBPA in the presence of metal ions, and TEMPO was identified as the most effective one.
