Fe(II)催化水铁矿晶相转变过程中Pb的吸附与固定

doi:10.6023/A17030093

化学学报 ›› 2017, Vol. 75 ›› Issue (6): 621-628.DOI: 10.6023/A17030093 上一篇下一篇

所属专题：铁环境化学

研究论文

Fe(II)催化水铁矿晶相转变过程中Pb的吸附与固定

刘承帅^a,b, 李芳柏^a, 陈曼佳^a, 廖长忠^a, 童辉^b, 华健^a

a 广东省生态环境技术研究所广东省农业环境综合治理重点实验室广州 510650;
b 中国科学院地球化学研究所环境地球化学国家重点实验室贵阳 550081

投稿日期:2017-03-06 发布日期:2017-05-09
通讯作者: 李芳柏 E-mail:cefbli@soil.gd.cn
基金资助:
项目受国家自然科学基金（Nos.41673135，41420104007，41671240）、广东省科技项目（Nos.S2013050014266，2015A030313752，2016A030313780，2016B020242006）和中国科学院“百人计划”资助.

Adsorption and Stabilization of Lead during Fe(II)-catalyzed Phase Transformation of Ferrihydrite

Liu Chengshuai^a,b, Li Fangbai^a, Chen Manjia^a, Liao Changzhong^a, Tong Hui^b, Hua Jian^a

a Guangdong Key Laboratory of Integrated Agro-Environmental Pollution Control and Management, Guangdong Institute of Eco-Environmental Science & Technology, Guangzhou 510650, China;
b State Key Laboratory of Environmental Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang 550081, China

Received:2017-03-06 Published:2017-05-09
Contact: 10.6023/A17030093 E-mail:cefbli@soil.gd.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Nos. 41673135, 41420104007, 41671240), the Science and Technology Project of Guangdong Province (Nos. S2013050014266, 2015A030313752, 2016A030313780; 2016B020242006), and One Hundred Talents Programme of the Chinese Academy of Sciences.

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摘要/Abstract

厌氧状态下，游离态Fe（Ⅱ）（Fe（Ⅱ）_aq）催化氧化铁晶相重组是重要的铁循环化学过程，其本质是Fe（Ⅱ）_aq与结构态Fe（Ⅲ）间的Fe原子交换，这一过程对稻田土壤和沉积物中重金属的环境行为产生重要影响，其影响机制有待于深入研究.本研究结果显示，Fe（Ⅱ）_aq催化水铁矿晶相转变过程中，重金属离子Pb（Ⅱ）通过与Fe（Ⅱ）的竞争性吸附，降低了水铁矿表面吸附态Fe（Ⅱ）浓度，抑制了Fe（Ⅱ）_aq与水铁矿中结构态Fe（Ⅲ）之间的Fe原子交换，最终降低水铁矿晶相转变速率并改变水铁矿晶相转变途径.无Pb（Ⅱ）时，水铁矿最终转变为针铁矿和磁铁矿；Pb（Ⅱ）影响下，转变产物主要为纤铁矿，部分为针铁矿和磁铁矿.在水铁矿晶相转变过程中，部分吸附到氧化铁表面的Pb（Ⅱ）通过晶体包裹或Fe结构位取代，被形成的氧化铁结构化固定，从而降低了重金属Pb（Ⅱ）的活性.

关键词: 氧化铁, Fe原子交换, 重金属, 稳定同位素示踪, 同晶置换

Aqueous Fe(Ⅱ) (Fe(Ⅱ)_aq)-catalyzed recrystallization of iron (hydr)oxides is the important chemical reaction of iron cycle in anaerobic environments, which poses significant effects on the environmental behavior of heavy metals in soils and sediments. Ferrihydrite is the initial iron mineral phase during the ferrous mineralization and has relatively unstable crystal structure. The structure transformation behavior of ferrihydrite is active and also poses important effects on environmental behavior of soil heavy metals. However, the Fe(Ⅱ)_aq-catalyzed phase transformation of ferrihydrite has been rarely reported, especially with the coexisting metal ions. In the present study, the effects of coexisting heavy metal of Pb(Ⅱ) on the Fe(Ⅱ)_aq-catalyzed phase transformation of ferrihydrite coupling the environmental behavior of Pb(Ⅱ) were systematically studied. The results show that ferrihydrite underwent efficient phase transformation rates when catalyzed by Fe(Ⅱ)_aq whenever with or without the effect of Pb(Ⅱ). Compared with the reaction system that without Pb(Ⅱ), the adsorption of Fe(Ⅱ) on the surface of ferrihydrite was inhibited due to the competition of Pb(Ⅱ) when with the coexistence of Pb(Ⅱ), which further decreased the rates of Fe atom exchange between Fe(Ⅱ)_aq and structural Fe(Ⅲ) of ferrihydrite. With the inhibited Fe atom exchange reaction, the phase transformation rates were relatively decreased and transformation products were changed during the Fe(Ⅱ)_aq-catalyzed phase transformation of ferrihydrite. Goethite and magnetite were found to be the final transformed products of iron (hydr)oxides when without Pb(Ⅱ), while lepidocrocite was determined to be the main transformed product with little goethite and magnetite as the other transformed products when with Pb(Ⅱ). During the Fe(Ⅱ)_aq-catalyzed phase transformation of ferrihydrite with the coexistence of Pb(Ⅱ), some Pb were stabilized through being incorporated into the structure of ferrihydrite transformed products with the possible mechanisms of occlusion by the crystal lattice and structural incorporation, so as to decrease the activity of the polluted heavy metal of Pb. The obtained results in the present study are expected to provide further insights for understanding the iron cycle coupling with the environmental behavior of heavy metals in soils and sediments.

Key words: iron oxide, Fe atom exchange, heavy metal, stable isotope tracing, isomorphous replacement

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刘承帅, 李芳柏, 陈曼佳, 廖长忠, 童辉, 华健. Fe(II)催化水铁矿晶相转变过程中Pb的吸附与固定[J]. 化学学报, 2017, 75(6): 621-628.

Liu Chengshuai, Li Fangbai, Chen Manjia, Liao Changzhong, Tong Hui, Hua Jian. Adsorption and Stabilization of Lead during Fe(II)-catalyzed Phase Transformation of Ferrihydrite[J]. Acta Chim. Sinica, 2017, 75(6): 621-628.

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[1] Latta, D. E.; Bachman, J. E.; Scherer, M. M. Environ. Sci. Technol. 2012, 46, 10614.
[2] (a) Suter, D.; Siffert, C.; Sulzberger, B.; Stumm, W. Nturwissenschaften 1988, 75, 571. (b) Suter, D.; Banwart, S.; Stumm, W. Langmuir 1991, 7, 809.
[3] (a) Williams, A. G.; Scherer, M. M. Environ. Sci. Technol. 2004, 38, 4782. (b) Pedersen, H. D.; Postma, D.; Jakobsen, R.; Larsen, O. Geochim. Cosmochim. Acta 2005, 69, 3967.
[4] (a) Yanina, S. V.; Rosso, K. M. Science 2008, 320, 218. (b) Rosso, K. M.; Yanina, S. V.; Gorski, C. A.; Larese-Casanova, P.; Scherer, M. M. Environ. Sci. Technol. 2010, 44, 61.
[5] Frierdich, A. J.; Helgeson, M.; Liu, C.; Wang, C.; Rosso, K. M.; Scherer, M. M. Environ. Sci. Technol. 2015, 49, 8479.
[6] (a) Frierdich, A. J.; Catalano, J. G. Environ. Sci. Technol. 2012, 46, 11070. (b) Frierdich, A. J.; Scherer, M. M.; Bachman, J. E.; Engelhard, M. H.; Rapponotti, B. W.; Catalano, J. G. Environ. Sci. Technol. 2012, 46, 10031.
[7] Liu, C. S.; Zhu, Z. K.; Li, F. B.; Liu, T. X.; Liao, C. Z.; Lee, J. J.; Shih, K. M.; Tao, L.; Wu, Y. D. Chem. Geol. 2016, 444, 110.
[8] (a) Jambor, J. L.; Dutrizac, J. E. Chem. Rev. 1998, 98, 2549. (b) Wang, X. M.; Li, W.; Harrington, R.; Liu, F.; Parise, J. B.; Feng, X. H.; Sparks, D. L. Environ. Sci. Technol. 2013, 47, 10322. (c) Liu, J.; Yang, J.; Zeng, X.; Wang, J.; Sparks, D. Acta Chim. Sinica 2017, DOI:10.6023/A17030082. (刘瑾, 杨建军, 曾希柏, Jian Wang, Donald Sparks, 化学学报, 2017, DOI:10.6023/A17030082.); (d) Wang, X.; Peng, J.; Xu, H.; Tan, W.; Liu, F.; Huang, Q.; Feng, X. Acta Chim. Sinica 2017, DOI:10.6023/A17020046. (王小明, 彭晶, 徐欢欢, 谭文峰, 刘凡, 黄巧云, 冯雄汉, 化学学报, 2017, DOI:10.6023/A17020046.)
[9] (a) Cornell, R. M.; Schwertmann, U. The Iron Oxides:Structure, Properties, Reactions, Occurences and Uses, 2nd ed., Wiley-VCH, Weinheim, 2003. (b) Wang, X.; Liu, H.; Wei, Y.; Li, Y.; Zhao, X.; Wang, Y. Acta Chim. Sinica 2008, 66, 685. (王欣, 刘辉, 魏雨, 李彦涛, 赵新强, 王延吉, 化学学报, 2008, 66, 685.); (c) Das, S.; Hendry, M. J.; Essilfie-Dughan, J. Environ. Sci. Technol. 2011, 45, 5557. (d) Wang, X. M.; Zhu, M. Q.; Lan, S.; Ginder-Vogel, M.; Liu, F.; Feng, X. H. Chem. Geol. 2015, 415, 37.
[10] (a) Tronc, E.; Belleville, P.; Jolivet, J. P.; Livage, J. Langmuir 1992, 8(1), 313. (b) Hansel, C. M.; Benner, S. G.; Fendorf, S. Environ. Sci. Technol. 2005, 39(18), 7147.
[11] (a) Stewart, B. D.; Nico, P. S.; Fendorf, S. Environ. Sci. Technol. 2009, 43(13), 4922. (b) Amstaetter, K.; Borch, T.; Larese-Casanova, P.; Kappler, A. Environ. Sci. Technol. 2010, 44(1), 102. (c) Felmy, A. R.; Moore, D. A.; Rosso, K. M.; Qafoku, O.; Rai, D.; Buck, E. C.; Ilton, E. S. Environ. Sci. Technol. 2011, 45(9), 3952.
[12] (a) Schwertmann, U.; Taylor, R. M. Clays Clay Miner. 1972, 20(3), 151. (b) Yang, L.; Steefel, C. I.; Marcus, M. A.; Bargar, J. R. Environ. Sci. Technol. 2010, 44(14), 5469.
[13] Frierdich, A. J.; Catalano, J. G. Environ. Sci. Technol. 2012, 46, 1519.
[14] (a) Wu, Z.; Zhang, W.; Sun, Z. Acta Chim. Sinica 2010, 68, 769. (吴震生, 张卫民, 孙中溪, 化学学报, 2010, 68, 769.); (b) Cao, F.; Wu, Y.; Liu, H.; Wei, Y. Acta Chim. Sinica 2008, 66, 1405. (曹付玲, 吴育飞, 刘辉, 魏雨, 化学学报, 2008, 66, 1405.)
[15] (a) Alvarez, M.; Rueda, E. H.; Sileo, E. E. Geochim. Cosmochim. Acta 2007, 71, 1009. (b) Kaur, N.; Gräfe, M.; Singh, B.; Kennedy, B. Clays Clay Miner. 2009, 57(2), 234.
[16] Jang, J. H.; Dempsey, B. A.; Catchen, G. L.; Burgos, W. D. Colloids Surf., A 2003, 221(1), 55.
[17] Boland, D. D.; Collins, R. N.; Miller, C. J.; Glover, C. J.; Waite, T. D. Environ. Sci. Technol. 2014, 48(16), 9086.
[18] (a) Gorski, C. A.; Handler, R. M.; Beard, B.; Pasakarnis, T.; Johnson, C. M.; Scherer, M. M. Environ. Sci. Technol. 2012, 46, 12399. (b) Liu, C. S.; Wei, Z. Q.; Li, F. B.; Dong, J. Scientia Sinica Terrae 2016, 46, 1542. (刘承帅, 韦志琦, 李芳柏, 董军, 中国科学:地球科学, 2016, 46, 1542.)
[19] (a) Handler, R. M.; Beard, B. L.; Johnson, C. M.; Scherer, M. M. Environ. Sci. Technol. 2009, 43, 1102. (b) Joshi, P.; Gorski, C. A. Environ. Sci. Technol. 2016, 50, 7315.
[20] Handler, R. M.; Frierdich, A. J.; Johnson, C. M.; Rosso, K. M.; Beard, B. L.; Wang, C.; Latta, D. E.; Neumann, A.; Pasakarnis, T.; Premaratne, W. A. P. J.; Scherer, M. M. Environ. Sci. Technol. 2014, 48, 11302.
[21] Reddy, T. R.; Frierdich, A. J.; Beard, B. L.; Johnson, C. M. Chem. Geol. 2015, 397, 118.
[22] Schilt, A. A. Applications of 1,10-Phenanthroline and Related Compounds, 1st ed., Pergamon Press, Oxford, 1969.
[23] Lu, X. W.; Shih, K. M.; Liu, C. S.; Wang, F. Environ. Sci. Technol. 2013, 47, 9972.
[24] Michel, F. M.; Ehm, L.; Antao, S. M.; Lee, P. L.; Chupas, P. J.; Liu, G.; Strongin, D. R.; Schoonen, M. A. A.; Phillips, B. L.; Parise, J. B.; Science 2007, 316, 1726.
[25] (a) De La Torre, A. G.; Bruque, S.; Aranda, M. A. G. J. Appl. Crystallogr. 2001, 34, 196. (b) Bernasconi, A.; Dapiaggi, M.; Gualtieri, A. F. J. Appl. Crystallogr. 2014, 47, 136.

Fe(II)催化水铁矿晶相转变过程中Pb的吸附与固定

Adsorption and Stabilization of Lead during Fe(II)-catalyzed Phase Transformation of Ferrihydrite

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