改性Pd/GAC粒子电极吸附-电催化去除2,4,6-三氯苯酚  

Adsorption and electrocatalytic degradation of 2,4,6-trichlorophenol by modified Pd/GAC particle electrode

作　　者：张金珂 梁玉涵 吴玉超 吴晨达 陈吕军[3] 刘宏远[1] 颉亚玮 ZHANG Jinke;LIANG Yuhan;WU Yuchao;WU Chenda;CHEN Lvjun;LIU Hongyuan;XIE Yawei(School of Civil Engineering,Zhejiang University of Technology,Hangzhou 310023,China;Kaiyuan Environmental Technology Group Co.Ltd.,Hangzhou 311200,China;School of Environment,Tsinghua University,Beijing 100084,China)

机构地区：[1]浙江工业大学土木工程学院,杭州310023 [2]开源环境科技集团有限公司,杭州311200 [3]清华大学环境学院,北京100084

出　　处：《环境工程学报》2024年第1期79-90,共12页Chinese Journal of Environmental Engineering

基　　金：国家自然科学基金面上资助项目(52070111;52170093);浙江省自然科学基金资助项目(LY22E080010)。

摘　　要：以6 mol·L^(-1)硝酸和450℃高温共同改性后的颗粒活性炭(granular activated carbon,GAC)为载体,采用硼氢化钠还原法制备了改性Pd/GAC粒子电极,研究了电极对2,4,6-三氯苯酚(2,4,6-trichlorophenol,2,4,6-TCP)的去除能力、动力学特征及脱氯机理。结果表明,通过改性,GAC的比表面积(560.791 m^(2)·g^(-1))提高了1.5倍,孔容提高了36.02%,对2,4,6-TCP的最大吸附容量为199.2 mg·g^(-1)。在优化条件下,改性粒子电极4 h内对30 mg·L^(-1)的2,4,6-TCP去除率达到94.7%,反应速率常数为0.014 min^(-1),钯的催化活性为0.3(min·mmol)^(-1)。通过对反应过程中有机氯和无机氯变化的分析,阐明了改性Pd/GAC粒子电极强化去除2,4,6-TCP的过程。从还原途径、直接和间接还原贡献等方面探究了改性粒子电极电催化脱氯机理。A modified Pd/granular activated carbon(GAC) particle electrode was prepared via sodium borohydride reduction using HNO3(6 mol·L^(-1)) and high-temperature(450 ℃) modified GAC as the carrier.The performance,kinetics and dechlorination mechanism of the electrode on 2,4,6-trichlorophenol(2,4,6-TCP)removal were studied.The results showed that after modification,the specific surface area and pore volume of GAC increased by 1.5 times(560.791 m^(2)·g^(-1)) and 36.02%,respectively,and the maximum adsorption capacity to 2,4,6-TCP correspondingly increased to 199.2 mg·g^(-1).Under the optimized conditions,the modified particle electrode removed about 94.7% of 2,4,6-trichloropropanol(30 mg·L^(-1)) at a rate constant of 0.014 min^(-1) in 4hours.The catalytic activity of Pd was determined as 0.3(min·mmol)^(-1).The 2,4,6-TCP removal process was elucidated via the analysis of the variation of organic chlorine and inorganic Cl^(-).The electrocatalytic dechlorination mechanism of the modified particle electrodes was explored from the reduction pathways,direct and indirect reduction contributions.

关 键 词：粒子电极 电催化脱氯 2 4 6-三氯苯酚 反应机理 

分 类 号：X703[环境科学与工程—环境工程]