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Supervised by Ministry of Industry and Information Technology of The People's Republic of China Sponsored by Harbin Institute of Technology Editor-in-chief Yu Zhou ISSNISSN 1005-9113 CNCN 23-1378/T

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Related citation:Jie Ding,Dihui Song,Xianshu Liu,Zhao Song,Gaofeng Wu.Iron Species-Impregnated Granular Activated Carbon as Modified Particle Electrodes Applied in Benzothiazole Adsorption and Electrocatalytic Degradation[J].Journal of Harbin Institute Of Technology(New Series),2017,24(3):39-49.DOI:10.11916/j.issn.1005-9113.16053.
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Iron Species-Impregnated Granular Activated Carbon as Modified Particle Electrodes Applied in Benzothiazole Adsorption and Electrocatalytic Degradation
Author NameAffiliation
Jie Ding School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150001, China 
Dihui Song School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150001, China 
Xianshu Liu School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150001, China 
Zhao Song School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150001, China 
Gaofeng Wu School of Municipal and Environmental Engineering, Harbin Institute of Technology, Harbin 150001, China 
Abstract:
The object of this study is to prepare iron species-impregnated granular activated carbon as particle electrodes in order to improve their adsorption and electrocatalytic degradation capacity in Benzothiazole removal. The incorporation of Fe-containing catalysts was performed by Fe(NO3)3 impregnation. The obtained samples were characterized by BET, Fourier transform infrared spectroscopy, SEM-EDS, powder X-ray diffraction, X-ray photoelectron spectra and TG. Compared with pure activated carbon, this modified particle electrodes show higher static adsorption capacities and TOC removal, which have respectively increased by 25.9% and 54.4%. Both physisorption and chemisorption exist in the process of benzothiazole adsorption, where the latter plays a major role. In this way, the Fe-containing catalysts on modified particle electrodes are demonstrated to make a greater contribution to the improvement of electrocatalytic degradation by decreasing the activated energy by 32%.
Key words:  modified activated carbon  iron  particle electrodes  Benzothiazole  adsorption  electrocatalytic degreadation
DOI:10.11916/j.issn.1005-9113.16053
Clc Number:X522
Fund:
Descriptions in Chinese:
  

铁浸渍颗粒活性炭作为改性的粒子电极在苯并噻唑的吸附和电催化降解中的应用

丁 杰,宋迪慧,刘先树,宋 昭,吴高峰

(哈尔滨工业大学 市政环境工程学院)

创新点说明:

1)利用三维电催化氧化技术处理苯并噻唑类的废水;

2)制备含铁催化剂的活性炭粒子电极,获得成本较低并兼具良好吸附性能和催化性能的粒子电极。

研究目的:

利用三维电催化氧化技术处理难降解的复杂有机物。

研究方法:

1)孔道结构参数的测定:测定BET、BJH和HK,得到比表面积、总孔容、微孔孔径等参数,采用的设备为ASAP 2020.

2)傅里叶红外光谱的测定:为测得表面的官能团,采用的是溴化钾测定方法,使用的仪器为Spectrum One.

3)SEM-EDS测定:SEM为了测定粒子电极的表面形貌,所用仪器为EVO-18. EDS是该仪器设备的另一个附件,可测得粒子电极表面的元素含量比重,所用仪器为X-Max.

4)XRD的测定:为了测定粒子电极表面的晶型结构,从而判定表面含铁催化剂的物相。

5)XPS测定:为了测定粒子电极表面每种含铁催化剂的含量.

6)TG测定:热重分析法,得到TCD-DTG曲线,可以拟合燃烧热力学方程并计算得到粒子电极的活化能,使用的仪器为NETZSCH STA 499C.

7)苯并噻唑的测定:采用高相液相色谱仪,Waters Acquity Ultra Performance LC.

8)TOC和COD的测定:COD的测定采用国标法;TOC的测定仪器为TOC-V CPH/CPN Analyzer(Shimadzu)

9)中间产物的鉴定测定:利用LC-MS联用分析测定,采用的设备为Triple Quard Agilent 6430.

10)铁离子溶出浓度的检测:采用ICO-AES手段测定,仪器为Optima 5300DV analyzer(Perkin Elmer).

11)电化学工作站测定:采用的设备为上海华晨公司的CHI 700E。测定了开路电位、循环伏安曲线以及交流阻抗曲线等。

结果:

改性后的粒子电极相较于活性炭本身,吸附性能和电催化性能均有所提升。

结论:

1)获得了最佳的粒子电极制备条件:常温下,在硝酸铁溶液中浸渍活性炭18h,再在马弗炉里380 ℃下焙烧4 h。

2)改性后粒子电极的吸附性能提升包括物理吸附能力和化学吸附能力的提高,其中化学吸附起到主要的作用。

3)改性后粒子电极的电催化性能提升主要是表面镀上了含铁催化剂,分别为Fe、Fe2O3和Fe3O4,使得改性后粒子电极的活化能相较于活性炭降低了32%。

4)推断了苯并噻唑在三维电催化降解体系中的降解途径。

关键词:改性活性炭;铁;粒子电极;苯并噻唑;吸附;电催化

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