Cathodic Hydrogen as Electron Donor in Enhanced Reductive Dechlorination

doi:10.1016/S1004-9541(13)60639-4

Chinese Journal of Chemical Engineering ›› 2013, Vol. 21 ›› Issue (12): 1386-1390.DOI: 10.1016/S1004-9541(13)60639-4

• 能源、资源与环境技术 • 上一篇下一篇

Cathodic Hydrogen as Electron Donor in Enhanced Reductive Dechlorination

张瑞玲¹, 路晓霞², Danny D. Reible³, 焦刚珍¹, 秦松岩¹

1 School of Environmental Science and Safety Engineering, Tianjin University of Technology, Tianjin 300384, China;
2 Anchor Qea, LLC, Austin, TX 78746, USA;
3 Department of Civil & Environmental Engineering, Texas Tech University, Lubbock, TX 79409-1023, USA

收稿日期:2012-10-19 修回日期:2013-06-16 出版日期:2013-12-28 发布日期:2013-12-27
通讯作者: ZHANG Ruiling
基金资助:
Supported by the National Natural Science Foundation of China (51108317), and the Municipal Natural Science Foundation of Tianjin (12JCQNJC05400).

Cathodic Hydrogen as Electron Donor in Enhanced Reductive Dechlorination

ZHANG Ruiling¹, LU Xiaoxia², Danny D. Reible³, JIAO Gangzhen¹, QIN Songyan¹

1 School of Environmental Science and Safety Engineering, Tianjin University of Technology, Tianjin 300384, China;
2 Anchor Qea, LLC, Austin, TX 78746, USA;
3 Department of Civil & Environmental Engineering, Texas Tech University, Lubbock, TX 79409-1023, USA

Received:2012-10-19 Revised:2013-06-16 Online:2013-12-28 Published:2013-12-27
Contact: ZHANG Ruiling
Supported by:
Supported by the National Natural Science Foundation of China (51108317), and the Municipal Natural Science Foundation of Tianjin (12JCQNJC05400).

摘要/Abstract

摘要： In situ capping is an attractive and cost-effective method for remediation of contaminated sediments, but few studies on enhancing contaminant degradation in sediment caps have been reported, especially for chlorinated benzenes. Electrically enhanced bioactive barrier is a new process for in situ remediation for reducible compounds in soil or sediments. The primary objective of this study is to determine if electrodes in sediment could create a redox gradient and provide electron acceptor/donor to stimulate degradation of chlorinated contaminant. The results demonstrate that graphite electrodes lead to sustainable evolution of hydrogen, displaying zero-order kinetics in the initial stages with different voltages. The constant rates of hydrogen evolution at 3, 4, and 5 V are 1.05, 2.54, and 4.3 nmol·L^-¹·d^-¹, respectively. Even higher voltage can produce more hydrogen, but it could not keep long time because the over potentials on electrode surfaces prevent its function. The study shows that 4 V is more appropriate for hydrogen evolution. The measured and evaluated concentration of 1,2,3,5-tetrachlorobenzene in pore water of sediment and concentration of sulfate show that dechlorination is inhibited at higher concentration of sulfate.

关键词: hydrogen, electrode, reductive, dechlorination, capping

Abstract: In situ capping is an attractive and cost-effective method for remediation of contaminated sediments, but few studies on enhancing contaminant degradation in sediment caps have been reported, especially for chlorinated benzenes. Electrically enhanced bioactive barrier is a new process for in situ remediation for reducible compounds in soil or sediments. The primary objective of this study is to determine if electrodes in sediment could create a redox gradient and provide electron acceptor/donor to stimulate degradation of chlorinated contaminant. The results demonstrate that graphite electrodes lead to sustainable evolution of hydrogen, displaying zero-order kinetics in the initial stages with different voltages. The constant rates of hydrogen evolution at 3, 4, and 5 V are 1.05, 2.54, and 4.3 nmol·L^-¹·d^-¹, respectively. Even higher voltage can produce more hydrogen, but it could not keep long time because the over potentials on electrode surfaces prevent its function. The study shows that 4 V is more appropriate for hydrogen evolution. The measured and evaluated concentration of 1,2,3,5-tetrachlorobenzene in pore water of sediment and concentration of sulfate show that dechlorination is inhibited at higher concentration of sulfate.

Key words: hydrogen, electrode, reductive, dechlorination, capping

张瑞玲, 路晓霞, Danny D. Reible, 焦刚珍, 秦松岩. Cathodic Hydrogen as Electron Donor in Enhanced Reductive Dechlorination[J]. Chinese Journal of Chemical Engineering, 2013, 21(12): 1386-1390.

ZHANG Ruiling, LU Xiaoxia, Danny D. Reible, JIAO Gangzhen, QIN Songyan. Cathodic Hydrogen as Electron Donor in Enhanced Reductive Dechlorination[J]. Chin.J.Chem.Eng., 2013, 21(12): 1386-1390.

参考文献

1 Lampert, D.J., Reible, D.D., “An analytical modeling approach for evaluation of capping of contaminated sediments”, Soil and Sediment Contamination: An International Journal, 18 (4), 470-488 (2009).

2 Sun, M., Yan, F., Zhang, R.L., Reible, D.D., Lowry, G.V., Gregory, K.B., “Redox control and hydrogen production in sediment caps using carbon cloth electrodes”, Environ. Sci. Technol., 44 (21), 8209-8215 (2010).

3 Zhu, B.W., Lim, T.T., Feng, J., “Reductive dechlorination of 1,2,4-trichlorobenzene with palladized nanoscale Fe⁰ particles supported on chitosan and silica”, Chemosphere, 65 (7), 1137-1145 (2006).

4 Meharg, A.A., Wright, J., Osborn, D., “Chlorobenzenes in rivers draining industrial catchments”, The Science of the Total Environment, 251/252, 243-253 (2000).

5 Sokol, R.C., Kwon, O.S., Bethoney, C.M., Rhee, G.Y., “Reductive dechlorination of polychlorinated biphenyls in St. Lawrence River sediments and variations in dechlorination characteristics”, Environ. Sci. Technol., 28, 2054-2064 (1994).

6 Young, C.C., Kyoung, H.O., “Effects of sulfate concentration on the anaerobic dechlorination of polychlorinated biphenyls in estuarine sediments”, The Journal of Microbiology, 4, 166-171 (2005).

7 Mohn, W.W., Kennedy, K.J., “Limited degradation of chlorophenols by anaerobic sludge granules”, Appl. Environ. Microbiol., 58, 2131-2136 (1992).

8 Häggblom, M.M., Rivera, M.D., Young, L.Y., “Effects of auxiliary carbon sources and electron acceptors on methanogenic degradation of chlorinated phenols”, Environ. Toxicol. Chem., 12, 1395-1403 (1993).

9 Lin, C.J., Lo, S.L., Liou, Y.H., “Dechlorination of trichloroethylene in aqueous solution by noble metal-modified iron”, J. Hazard. Mater., 31, 219-228 (2004).

10 Shekar, S.C., Murthy, J.K., Rao, P.K., Rao, K.S.R., Kemnitz, E., “Selective hydrogenolysis of dichlorodifluoromethane (CCl₂F₂) over CCA supported palladium bimetallic catalysts”, Applied Catalysis A: General, 244, 39-48 (2003).

11 Adrian, L., Szewzyk, U., Wecke, J., Görisch, H., “Bacterial dehalorespiration with chlorinated benzenes”, Nature, 408 (6812), 580-583 (2000).

12 Skadberg, B., Geoly-Horn, S.L., Sangamalli, V., Flora, J.R.V., “Influence of pH, current and copper on the biological dechlorination of 2,6-dichlorophenol in an electrochemical cell”, Water Research, 33 (9), 1997-2010 (1999).

13 Gregory, K.B., Bond, D.R., “Graphite electrodes as electron donors for anaerobic respiration”, Environ. Microbiol., 6 (6), 596-604 (2004).

14 Strycharz, S.M., Woodard, T.L., “Graphite electrode as a sole electron donor for reductive dechlorination of tetrachlorethene by Geobacter lovleyi”, Appl. Environ. Microbiol., 74 (19), 5943-5947 (2008).

15 Thrash, J.C., Van Trump, J.I., “Electrochemical stimulation of microbial perchlorate reduction”, Environ. Sci. Technol., 41 (5), 1740-1746 (2007).

16 Laura, S., Johnsona, C.A., Annette, K., “Redox conditions and alkalinity generation in a seasonally anoxic lake (Lake Greifen)”, Marine Chemistry, 36 (11), 9-26 (1991).

17 Alter, M.D., Steiof, M., “Optimized method for dissolved hydrogen sampling in groundwater”, J. Contam. Hydrol., 78, 71-86 (2005).

18 Kelvin, B.G., Bond, D.R., Lovley, D.R., “Graphite electrodes as electron donors for anaerobic respiration”, Environ. Microbiol., 6 (6), 596-604 (2004).

19 Alison, E.S., “Demonstration and evaluation of solid-phase microextraction for assessment of contaminant mobility and bioavailability”, Master Thesis, The University of Texas at Austin (2008).

20 Lu, X.X., Reible, D.D., Fleeger, J.W., “Bioavailability of polycyclic aromatic hydrocarbons in field-contaminated Anacostia river (Washington, DC) sediment”, Environ. Toxicol. Chem., 25 (11), 2869-2874 (2006).

21 Dash, B.P., Chaudhari, S., “Electrochemical denitrificaton of simulated ground water”, Water Research, 39, 4065-4072 (2005).

22 Rozendal, R.A., Jeremiasse, A.W., “Hydrogen production with a microbial biocathode”, Environ. Sci. Technol., 42 (2), 629-634 (2008).

23 Sun, M., Sheng, G.P., “An MEC-MR-coupled system for biohydrogen production from acetate”, Environ. Sci. Technol., 42 (21), 8095-8100 (2008).

24 Rhee, G.Y., Bush, B., Bethoney, C.M., DeNucci, A., Oh, H.M., Sokol, R.C., “Anaerobic dechlorination of Aroclor 1242 as affected by some environmental conditions”, Environ. Toxicol. Chem., 12, 1033-1039 (1993).

[1]	Peipei Ai, Huiqing Jin, Jie Li, Xiaodong Wang, Wei Huang. Ultra-stable Cu-based catalyst for dimethyl oxalate hydrogenation to ethylene glycol[J]. 中国化学工程学报, 2023, 60(8): 186-193.
[2]	Xiaolin Guo, Zhaoyang Zhang, Pengfei Xing, Shuai Wang, Yibing Guo, Yanxin Zhuang. Kinetic mechanism of copper extraction from methylchlorosilane slurry residue using hydrogen peroxide as oxidant[J]. 中国化学工程学报, 2023, 60(8): 228-234.
[3]	Hae-Kyun Park, Dong-Hyuk Park, Bum-Jin Chung. Influence of the electrolyte conductivity on the critical current density and the breakdown voltage[J]. 中国化学工程学报, 2023, 59(7): 169-175.
[4]	Zhonghao Li, Yuanyuan Yang, Huanong Cheng, Yun Teng, Chao Li, Kangkang Li, Zhou Feng, Hongwei Jin, Xinshun Tan, Shiqing Zheng. Measurement and model of density, viscosity, and hydrogen sulfide solubility in ferric chloride/trioctylmethylammonium chloride ionic liquid[J]. 中国化学工程学报, 2023, 59(7): 210-221.
[5]	Qunfeng Zhang, Bingcheng Li, Yuan Zhou, Deshuo Zhang, Chunshan Lu, Feng Feng, Jinghui Lv, Qingtao Wang, Xiaonian Li. Regulation of the selective hydrogenation performance of sulfur-doped carbon-supported palladium on chloronitrobenzene[J]. 中国化学工程学报, 2023, 58(6): 69-75.
[6]	Bin Gao, Junwen Chen, Qi Zuo, Hongyan Wang, Wenlin Li. The critical role of Zr in controlling the activity of Pd/Beta on the hydrogenation of phenol to cyclohexanone[J]. 中国化学工程学报, 2023, 57(5): 79-87.
[7]	Yunchang Fan, Chunyan Zhu, Sheli Zhang, Lei Zhang, Qiang Wang, Feng Wang. Efficient and selective extraction of sinomenine by deep eutectic solvents[J]. 中国化学工程学报, 2023, 57(5): 109-117.
[8]	Qi Yang, Weikang Dai, Maoshuai Li, Jie Wei, Yi Feng, Cheng Yang, Wanxin Yang, Ying Zheng, Jie Ding, Mei-Yan Wang, Xinbin Ma. Enhanced selective hydrogenation of glycolaldehyde to ethylene glycol over Cu⁰-Cu⁺ sites[J]. 中国化学工程学报, 2023, 57(5): 141-150.
[9]	Shujun Peng, Song Lei, Sisi Wen, Jian Xue, Haihui Wang. A Ruddlesden–Popper oxide as a carbon dioxide tolerant cathode for solid oxide fuel cells that operate at intermediate temperatures[J]. 中国化学工程学报, 2023, 56(4): 25-32.
[10]	Chao Yang, Zhelin Su, Yeshuang Wang, Huiling Fan, Meisheng Liang, Zhaohui Chen. Insight into the effect of gel drying temperature on the structure and desulfurization performance of ZnO/SiO₂ adsorbents[J]. 中国化学工程学报, 2023, 56(4): 233-241.
[11]	Qiaoqiao Liu, Guihong Lin, Jian Zhou, Liangliang Huang, Chang Liu. Hydrogen-bond mediated and concentrate-dependent NaHCO₃ crystal morphology in NaHCO₃–Na₂CO₃ aqueous solution: Experiments and computer simulations[J]. 中国化学工程学报, 2023, 55(3): 49-58.
[12]	Peipei Ai, Li Zhang, Jinchi Niu, Huiqing Jin, Wei Huang. Boron-doped lamellar porous carbon supported copper catalyst for dimethyl oxalate hydrogenation[J]. 中国化学工程学报, 2023, 55(3): 222-229.
[13]	Yuandong Cui, Bin He, Yu Lei, Yu Liang, Wanting Zhao, Jian Sun, Xiaomin Liu. Lignin derived absorbent for efficient and sustainable CO₂ capture[J]. 中国化学工程学报, 2023, 54(2): 89-97.
[14]	Suhang Jiang, Lijuan Tan, Yujia Tong, Lijian Shi, Weixing Li. A heterogeneous double chamber electro-Fenton with high production of H₂O₂ using La–CeO₂ modified graphite felt as cathode[J]. 中国化学工程学报, 2023, 54(2): 98-105.
[15]	Xianglin Liu, Minjie Xu, Chenxi Cao, Zixu Yang, Jing Xu. Effects of zinc on χ-Fe₅C₂ for carbon dioxide hydrogenation to olefins: Insights from experimental and density function theory calculations[J]. 中国化学工程学报, 2023, 54(2): 206-214.

Cathodic Hydrogen as Electron Donor in Enhanced Reductive Dechlorination

Cathodic Hydrogen as Electron Donor in Enhanced Reductive Dechlorination

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价