钯/泡沫镍电化学还原降解四溴二苯醚  

Electrochemical reductive degradation of tetrabromodiphenyl ether on Pd/foam-nickel

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作  者:王楠[1] 姜子叶 张桂花 朱丽华[1] WANG Nan;JIANG Ziye;ZHANG Guihua;ZHU Lihua(School of Chemistry and Chemical Engineering,Huazhong University of Science and Technology,Wuhan 430074,China)

机构地区:[1]华中科技大学化学与化工学院,湖北武汉430074

出  处:《华中科技大学学报(自然科学版)》2022年第10期10-17,共8页Journal of Huazhong University of Science and Technology(Natural Science Edition)

基  金:国家自然科学基金资助项目(21976063,22076052);湖北省自然科学基金资助项目(2019CFB432).

摘  要:以NaCl/PdCl_(2)(3:1)为沉积液,采用置换沉积法在泡沫镍基材上均匀沉积细小钯颗粒,制备了钯/泡沫镍电极,并利用此电极建立了典型溴代污染物2,2’,4,4’-四溴二苯醚(BDE47)的电化学还原脱溴体系.在0.015 mol/L H_(2)SO_(4)的甲醇/水(体积比9:1)溶液、反应温度30℃,-1.5 V电位(相对于Ag/AgCl参比电极)的优化条件下,电化学还原降解初始质量浓度为10 mg/L的BDE47,3 h的去除率达98.5%,4 h后BDE47被完全降解和脱溴,且无含溴有机中间产物的累积.机理研究表明:BDE47的降解脱溴主要以活性氢进攻机理为主,而非单一的电子还原脱溴途径.With foam-nickel as the substrate and NaCl/PdCl_(2)(3:1)solution as the deposition solution,a displacement deposition method was used to prepare Pd/foam-nickel electrode,on which highly uniformly dispersed palladium particles were deposited on the nickel foam.By using this Pd/foam-Ni electrode,an electrochemical reductive system was established for the nearly complete debromination of 2,2’,4,4’-tetrabromodiphenyl ether(BDE47)as a typical brominated pollutant.The optimized conditions were as below:0.015 mol/L H_(2)SO_(4)in methanol/water(9:1)as the electrolyte,the reaction temperature of 30°C,and a constant applied potential of-1.5 V(vs Ag/AgCl as a reference electrode).Under such electrochemical conditions,the degradation removal of BDE47 with an initial concentration of 10 mg/Lreached up to 98.5%after 3 h,and BDE47 was completely degraded and debrominated after 4 h without the accumulation of brominated organic intermediates.Research on mechanism shows that the degradation and debromination of BDE47 mainly follows the active hydrogen attack mechanism,but not a simple electron reductive debromination pathway.

关 键 词:四溴二苯醚 泡沫镍 钯修饰电极 电化学还原降解 脱溴 

分 类 号:X13[环境科学与工程—环境科学]

 

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