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3种活性钛网阳极电化学降解水中阿特拉津

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阿特拉津(atrazine,ATZ)等有机杀虫剂的大量生产和使用对水生态安全造成威胁,其可被电化学阳极氧化技术有效降解和矿化.为探究水中ATZ电化学降解效率、能耗与反应路径,以多孔钛网为基板制备Ti/RuO2-IrO2、Ti/PbO2、Ti/Ti4O7钛网阳极,开展电化学降解和矿化水中ATZ研究,分析了 3种钛网阳极表面结构特征和电化学性能;比较和评估3种钛网阳极电化学降解ATZ效率、溶液总有机碳(TOC)去除率、反应能耗;考察了电流密度、ATZ初始质量浓度、溶液初始pH等反应参数对ATZ降解效率的影响;探究了 ATZ电化学降解中间产物及反应路径.结果表明:Ti/RuO2-IrO2、Ti/PbO2、Ti/Ti4O7钛网阳极表面活性组分覆盖致密、均匀,其电析氧电位为Ti/Ti4O7(2.4 V)>Ti/PbO2(1.98 V)>Ti/RuO2-IrO2(1.48 V);3种钛网阳极电化学降解和矿化ATZ效率较高,ATZ的降解率和溶液TOC去除率分别为85.45%~96.3%和48.7%~69.8%,其中Ti/Ti4O7钛网阳极对ATZ和TOC去除率可达96.3%和69.8%;与Ti/RuO2-IrO2和Ti/PbO2相比,Ti/Ti4O7稳定性较好,反应能耗(221.4 kWh·kg-1)较低;ATZ电化学降解率随电流密度增大而升高、随ATZ初始质量浓度和溶液初始pH的增大而降低;水中ATZ电化学降解产生A(C8H15N5O,m/z=198.24),A 继续氧化生成 B(C8H15N5O2,m/z=214.22)、C(C7H13N5O3,m/z=216.20)、D(C6H10N4O3,m/z=187.20)、E(C3H3N3O4,m/z=146.07)、F(C3H3N3O5,m/z=162.07)等中间产物.
Electrochemical oxidation of atrazine in water using three active titanium mesh anodes
The mass production and use of organic pesticides such as atrazine(atrazine,ATZ),which threaten water ecological safety,can be effectively degraded and mineralized by electrochemical anodic oxidation(EAO)technology.To investigate the efficiency,energy consumption,and reaction path of electrochemical degradation of ATZ in water,Ti/RuO2-IrO2,Ti/PbO2,and Ti/Ti4O7 titanium mesh anodes were prepared using a porous titanium mesh substrate,and the tests on the electrochemical degradation and mineralization of ATZ in water were conducted.The surface structural characteristics and electrochemical properties of three titanium mesh anodes were analyzed.The degradation efficiency of ATZ,the total organic carbon(TOC)removal rate from the solution,and the reaction energy consumption were compared and evaluated in the electro-oxidation processes within these three types of titanium mesh anodes.The effects of various reaction parameters,including the current density,the initial concentration of ATZ,and the initial pH,on the degradation efficiency of ATZ were investigated.The degradation intermediates and reaction pathways of ATZ electro-oxidation were also explored.The results showed that the surfaces of the Ti/RuO2-IrO2,Ti/PbO2,and Ti/Ti4O7 titanium mesh anodes were densely and uniformly covered with active components,and their oxygen evolution potentials were Ti/Ti4O7(2.4 V)>Ti/PbO2(1.98 V)>Ti/RuO2-IrO2(1.48 V).The three types of titanium mesh anodes demonstrated high efficiency in the electrochemical degradation and mineralization of ATZ.The degradation efficiency of ATZ and the TOC removal rate from the solution ranged from 85.45%to 96.3%and 48.7%to 69.8%,respectively.Among these,the Ti/Ti4O7 titanium mesh anode could lead to an ATZ degradation efficiency of 96.3%and a TOC removal of 69.8%.Compared with the Ti/RuO2-IrO2 and Ti/PbO2 titanium mesh anodes,the Ti/Ti4O7 titanium mesh anode exhibited better stability and lower energy consumption(221.4 kWh·kg-1).The electrochemical degradation efficiency of ATZ increased with the increase of current density,while decreased with the increase of initial ATZ concentrations or pH.The ATZ in water was gradually degraded into intermediate A(C8H15N5O,m/z=198.24),which was further oxidized into intermediates B(C8H15N5O2,m/z=214.22),C(C7H13N5O3,m/z=216.20),D(C6H10N4O3,m/z=1 87.20),E(C3H3N3O4,m/z=146.07),and F(C3H3N3O5,m/z=1 62.07).

atrazineelectrochemical oxidationtitanium mesh anodedegradation efficiencyreaction pathway

伍梦琳、周舒、郑飞予、艾莎莉、智丹、周耀渝

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湖南农业大学环境与生态学院,长沙 410128

阿特拉津 电化学氧化 钛网阳极 降解效率 反应路径

2024

环境工程学报
中国科学院生态环境研究中心

环境工程学报

CSTPCD北大核心
影响因子:0.804
ISSN:1673-9108
年,卷(期):2024.18(11)