缓冲期碳酸盐型尾矿重金属释放机制——柱淋滤实验研究
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摘要
碳酸盐型尾矿在缓冲期/中性矿山废水(NMD)释放期的重金属污染问题易被忽视。本文以广西大厂锡石-硫化物尾矿作为研究对象,采用柱淋滤实验方法,探讨碳酸盐型尾矿在缓冲期重金属的释放机制,为此类型尾矿重金属污染的防治提供依据。实验结果表明,大厂尾矿在缓冲期(约7年,pH值为6. 6～8. 0)存在Sb、Zn、Cd、As(Pb)释放污染问题。在尾矿堆放初期(0. 5年,pH值由7. 6降至7. 2),Zn、Sb、Cd快速、大量释出;中期(0. 5～2. 5年,pH值由7. 2波动升高至8. 0),Sb较平稳释出;后期(2. 5～7年,pH值变化范围为8. 0～6. 6,呈降低趋势),受气温及pH值影响,As、Sb(Pb)呈波动或间歇振荡释出,即在夏季高温、pH值较高时,释出元素浓度较高,反之,在冬季低温、pH值较低时,释出元素浓度较低。重金属的释放与尾矿中硫化物的氧化程度高低及氧化先后顺序有关。这些矿物的氧化顺序大致为:闪锌矿(Zn、Cd)、辉锑锡铅矿(Sb)→脆硫锑铅矿(Sb)→毒砂(As)、方铅矿(Pb)。因此,对于(广西大厂)碳酸盐型尾矿在缓冲期的重金属污染应分阶段、季节(夏季),采取有针对性的防治措施;在缓冲期(7年)后应注意尾矿酸性矿山废水(AMD)+重金属(如As、Sb)复合污染的防治。
Heavy metal pollution from carbonate-type tailings in buffering/neutral mine drainage(NMD) period tends to be ignored. With the tailings of cassiterite-sulfide deposits in the Dachang ore district of Guangxi as the study object, the author conducted column leaching test to investigate the mechanism of heavy metals release from carbonate-type tailings in buffering period, so as to provide the basis for prevention and control of the heavy metal pollution involving the tailings. The results show that there probably exists the pollution of Sb, Zn, Cd, As(Pb)release from Dachangs tailings in the buffer period(about 7 years, with pH value being 6. 6 ～ 8. 0). At the beginning stage of tailings stacking(0 to 0. 5 years, with pH value dropped from 7. 6 to 7. 2), Zn, Sb and Cd are quickly and heavily released; in the middle stage(0. 5 to 2. 5 years, with pH value fluctuating from 7. 2 to 8. 0), Sb is more smoothly released; in the late stage(2. 5 to 7 years, with pH value changing between 8. 0 and 6. 6, showinga decreasing trend), As, Sb(Pb) fluctuate periodically or intermittently following air temperature and pH value,implying that when temperature and pH value are high in summer, element concentrations are higher; on the contrary, element concentrations are lower with the lowering temperature and pH value in winter. The heavy metals release is related to the oxidation degree/oxidation sequence of sulfide minerals that the metals are hosted in. The oxidation sequence of these minerals are sphalerite(Zn, Cd), franckeite(Sb) →jamesonite(Sb) →arsenopyrite(As), galena(Pb). Therefore, the measures to prevent and control the heavy metal pollution of the carbonate-type tailings(Dachang, Guangxi) in the buffering period should be carried out targetedly on the basis of tailings stocking stage and season(summer). After the buffer period(7 years), researchers should pay attention to the pollution combining the acid mine drainage(AMD) with heavy metals(As, Sb).
Heavy metal pollution from carbonate-type tailings in buffering/neutral mine drainage(NMD) period tends to be ignored. With the tailings of cassiterite-sulfide deposits in the Dachang ore district of Guangxi as the study object, the author conducted column leaching test to investigate the mechanism of heavy metals release from carbonate-type tailings in buffering period, so as to provide the basis for prevention and control of the heavy metal pollution involving the tailings. The results show that there probably exists the pollution of Sb, Zn, Cd, As(Pb)release from Dachangs tailings in the buffer period(about 7 years, with pH value being 6. 6 ～ 8. 0). At the beginning stage of tailings stacking(0 to 0. 5 years, with pH value dropped from 7. 6 to 7. 2), Zn, Sb and Cd are quickly and heavily released; in the middle stage(0. 5 to 2. 5 years, with pH value fluctuating from 7. 2 to 8. 0), Sb is more smoothly released; in the late stage(2. 5 to 7 years, with pH value changing between 8. 0 and 6. 6, showinga decreasing trend), As, Sb(Pb) fluctuate periodically or intermittently following air temperature and pH value,implying that when temperature and pH value are high in summer, element concentrations are higher; on the contrary, element concentrations are lower with the lowering temperature and pH value in winter. The heavy metals release is related to the oxidation degree/oxidation sequence of sulfide minerals that the metals are hosted in. The oxidation sequence of these minerals are sphalerite(Zn, Cd), franckeite(Sb) →jamesonite(Sb) →arsenopyrite(As), galena(Pb). Therefore, the measures to prevent and control the heavy metal pollution of the carbonate-type tailings(Dachang, Guangxi) in the buffering period should be carried out targetedly on the basis of tailings stocking stage and season(summer). After the buffer period(7 years), researchers should pay attention to the pollution combining the acid mine drainage(AMD) with heavy metals(As, Sb).
引文
Anju M and Banerjee D K.2010.Comparison of two sequential extraction procedures for heavy metal partitioning in mine tailings[J].Chemosphere,78:1 393~1 402.
Ashley P M,Lottermoser B G,Collins J,et al.2004.Environmental geochemistry of the derelict Webbs Consols mine,New South Wales,Australia[J].Environmental Geology,46(5):591~604.
Blowes D W,Jambor J L,Hanton-Fong C J,et al.1998.Geochemical,mineralogical and microbiological characterization of a sulphide-bearing carbonate-rich gold-mine tailings impoundment,Joutel,Québec[J].Applied Geochemistry,6:687~705.
Bodénan F,Baranger P,Piantone P,et al.2004.Arsenic behaviour in gold-ore mill tailings,Massif Central,France:hydrogeochemical study and investigation of in situ redox signatures[J].Applied Geochemistry,19:1 785~1 800.
Chen Binghui,Wan Moli,Wang Zhimei,et al.2010.A study of the biooxidation of pyrite by Acidithiobacillus ferrooxidans from the acid mine drainage in the Dabaoshan polymetallic ore deposit,northern Guangdong[J].Acta Petrologica et Mineralogica,29(5):562~568(in Chinese with English abstract).
Chen Zhiqiang,Su Liang and Yang Baojiang.2005.Geological characteristics and mineral resources of artificial ore deposits in tailing dams of nonferrous metal mines in Nandan area,Guangxi[J].Contributions to Geology and Mineral Resources,20(suppl.):139~144(in Chinese).
Courtin-Nomade A,Waltzing T,Evrard C,et al.2016.Arsenic and lead mobility:From tailing materials to the aqueous compartment[J].Applied Geochemistry,64:10~21.
Cravotta III C A.2008.Laboratory and field evaluation of a flushable oxic limestone drain for treatment of net-acidic drainage from a flooded anthracite mine,Pennsylvania,USA[J].Applied Geochemistry,12:3 404~3 422.
Holmstrom H,Ljungberg J and Ohlander B.1999.Role of carbonates in mitigation metal release from mining waste:Evidence from humidity cells tests[J].Environmental Geology,37:267~280.
Huminicki D M C and Rimstidt J D.2008.Neutralization of sulfuric acid solutions by calcite dissolution and the application to anoxic limestone drain design[J].Applied Geochemistry,23:148~165.
Johnson R H,Blowes D W,Robertson W D,et al.2000.The hydrogeochemistry of the Nickel Rim mine tailings impoundment,Sudbury,Ontario[J].Journal of Contaminant Hydrology,41:49~80.
Lei Liangqi,Lin Zheqiong,Mo Binji,et al.2016.Armoring effect of limestone in acid mine drainage:Static immersion experiments[J].Acta Petrologica et Mineralogica,35(3):553~562(in Chinese with English abstract).
Lei Liangqi,Shi Zhenghuan,Mo Jia,et al.2015.Characteristics of oxidation profile and acidification mechanism of a carbonate type tailings,Huangshaping Pb-Zn mine(Hunan Province,China)[J].Earth and Environment,43(2):173~182(in Chinese with English abstract).
Lei Liangqi,Song Ci’an,Xie Xiangli,et al.2011.Acidification characteristics and mechanism of carbonate-type tailings of Bali tailings storage,the Dachang tin-polymetallic orefield,Guangxi[J].Acta Petrologica et Mineralogica,30(1):141~149(in Chinese with English abstract).
Li Ling,Zhang Guoping,Liu Hong,et al.2009.Antimony and arsenic migration and environmental impacts on river draining in the Dachang multi-metalliferous mine area in Guangxi,China[J].Research of Environmental Sciences,22(6):682~687(in Chinese).
Li Xilin and Zhang Zhengen.1980.A restudy on sulfosalt mineral in an ore field in Guangxi province[J].Geochimica,2:172~185(in Chinese).
Liang Yali.2000.“10.18”event of Nandan tailings collapse[J].Coastal Environment,12:7(in Chinese).
Lindsay M B J,Condon P D,Jambor J L,et al.2009.Mineralogical,geochemical,and microbial investigation of a sulfide-rich tailings deposit characterized by neutral drainage[J].Applied Geochemistry,24:2 212~2 221.
Liu H Y,Probst A and Liao B H.2005.Metal contamination of soils and crops affected by the Chenzhou lead/zinc mine spill(Hunan,China)[J].Science of the Total Environment,339:153~166.
Lottermoser B G and Ashley P M.2006.Mobility and retention of trace elements in hardpan-cemented cassiterite tailings,north Queensland,Australia[J].Environmental Geology,50:835~846.
Mc Gregor R G,Blowes D W,Jambor J,et al.1998.Mobilization and attenuation of heavy metals within a nickel mine tailings impoundment near Sudbury,Ontario,Canada[J].Environmental Geology,36(3~4):305~319.
Moncur M C,Ptacek C J,Blowes D W,et al.2005.Release,transport and attenuation of metals from an old tailings impoundment[J].Applied Geochemistry,3:639~659.
Plante B,Bussière B and Benzaazoua M.2014.Lab to field scale effects on contaminated neutral drainage prediction from the Tio mine waste rocks[J].J.Geochem.Explor.,137:37~47.
Pope J and Trumm D.2015.Controls on Zn concentrations in acidic and neutral mine drainage from New Zealand’s bituminous coal and epithermal mineral deposits[J].Mine Water and the Environment,34:455~463.
Sherlockr E J,Lawrence R W,Poulin P,et al.1995.On the neutralization of acid rock drainage by carbonate and silicate minerals[J].Environment Geology,25:43~54.
Shu Wensheng,Zhang Zhiquan and Lan Chongyu.2001.Acid producing potential of a lead/zinc mine tailings at Lechang,Guangdong province[J].Environmental Science,22(3):113~117(in Chinese).
Soler J M,Boi M,Mogollón J L,et al.2008.The passivation of calcite by acid mine water.Column experiments with ferric sulfate and ferric chloride solutions at p H 2[J].Applied Geochemistry,12:3 579~3 588.
Souissi R,Souissi F,Chakroun H K,et al.2013.Mineralogical and geochemical characterization of mine tailings and Pb,Zn,and Cd mobility in a carbonate Setting(Northern Tunisia)[J].Mine Water and the Environment,32:16~27.
Tessier A,Campbell P G C and Bisson M.1979.Sequential extraction procedure for the speciation of particulate trace metals[J].Anal.Chem.,51:844~850.
Wisskirchen C,Dold B,Friese K,et al.2010.Geochemistry of highly acidic mine water following disposal into a natural lake with carbonate bedrock[J].Applied Geochemistry,8:1 107~1 119.
Zhai Limei,Chen Tongbin,Liao Xiaoyong,et al.2008.Pollution of agricultural soils resulting from a tailing spill at a Pb-Zn mine:A case study in Huanjiang,Guangxi Province[J].Acta Scientiae Circumstantiae,28(6):1 206~1 211(in Chinese with English abstract).
Zhang Xinying,Zhao Cailiu,Wu Haodong,et al.2008.Situation of heavy metal contamination in a typical mining town of Guangxi,south China[J].Environmental Monitoring in China,24(4):79~83(in Chinese).
Zhu Jibao,Chen Fanrong and Lu Long.2005.Heavy metal geochemistry behavior during the oxidation of the Fankou Pb-Zn mine tailings in Guangdong province and the implications for environmental remediation of the mines[J].Acta Scientiae Circumstantiae,25(3):414~422(in Chinese).
陈炳辉,万茉莉,王智美,等.2010.粤北大宝山多金属矿酸性矿山废水中氧化亚铁硫杆菌对黄铁矿的生物氧化作用研究[J].岩石矿物学杂志,29(5):562~568.
陈志强,苏亮,杨保疆.2005.广西南丹地区有色金属尾砂型人工矿床地质特征及其资源化[J].地质找矿论丛,20(增刊):139~144.
雷良奇,林哲琼,莫斌吉,等.2016.酸性矿山废水中石灰岩包壳作用研究[J].岩石矿物学杂志,35(3):553~562.
雷良奇,史振环,莫佳,等.2015.黄沙坪碳酸盐型尾矿氧化剖面组构及酸化机制[J].地球与环境,43(2):173~182.
雷良奇,宋慈安,谢襄漓,等.2011.广西大厂巴里碳酸盐型尾矿的酸化特征及机理[J].岩石矿物学杂志,30(1):141~149.
李玲,张国平,刘虹,等.2009.广西大厂多金属矿区河流中Sb和As的迁移及环境影响.环境科学研究[J].22(6):682~687.
李锡林,章振根.1980.广西某矿田中硫盐矿物的再研究[J].地球化学,2:172~185.
梁雅丽.2000.10.18南丹尾矿大坍塌[J].沿海环境,12:7.
束文圣,张志权,蓝崇钰.2001.广东乐昌铅锌尾矿的酸化潜力[J].环境科学,22(3):113~117.
翟丽梅,陈同斌,廖晓勇,等.2008.广西环江铅锌矿尾砂坝坍塌对农田土壤的污染及其特征[J].环境科学学报,28(6):1 206~1 211.
张新英,赵才流,吴浩东,等.2008.广西一个典型矿业镇环境中重金属污染分析[J].中国环境监测,24(4):79~83.
朱继保,陈繁荣,卢龙,等.2005.广东凡口Pb-Zn尾矿中重金属的表生地球化学行为及其对矿山环境修复的启示[J].环境科学学报,25(3):414~422.
Ashley P M,Lottermoser B G,Collins J,et al.2004.Environmental geochemistry of the derelict Webbs Consols mine,New South Wales,Australia[J].Environmental Geology,46(5):591~604.
Blowes D W,Jambor J L,Hanton-Fong C J,et al.1998.Geochemical,mineralogical and microbiological characterization of a sulphide-bearing carbonate-rich gold-mine tailings impoundment,Joutel,Québec[J].Applied Geochemistry,6:687~705.
Bodénan F,Baranger P,Piantone P,et al.2004.Arsenic behaviour in gold-ore mill tailings,Massif Central,France:hydrogeochemical study and investigation of in situ redox signatures[J].Applied Geochemistry,19:1 785~1 800.
Chen Binghui,Wan Moli,Wang Zhimei,et al.2010.A study of the biooxidation of pyrite by Acidithiobacillus ferrooxidans from the acid mine drainage in the Dabaoshan polymetallic ore deposit,northern Guangdong[J].Acta Petrologica et Mineralogica,29(5):562~568(in Chinese with English abstract).
Chen Zhiqiang,Su Liang and Yang Baojiang.2005.Geological characteristics and mineral resources of artificial ore deposits in tailing dams of nonferrous metal mines in Nandan area,Guangxi[J].Contributions to Geology and Mineral Resources,20(suppl.):139~144(in Chinese).
Courtin-Nomade A,Waltzing T,Evrard C,et al.2016.Arsenic and lead mobility:From tailing materials to the aqueous compartment[J].Applied Geochemistry,64:10~21.
Cravotta III C A.2008.Laboratory and field evaluation of a flushable oxic limestone drain for treatment of net-acidic drainage from a flooded anthracite mine,Pennsylvania,USA[J].Applied Geochemistry,12:3 404~3 422.
Holmstrom H,Ljungberg J and Ohlander B.1999.Role of carbonates in mitigation metal release from mining waste:Evidence from humidity cells tests[J].Environmental Geology,37:267~280.
Huminicki D M C and Rimstidt J D.2008.Neutralization of sulfuric acid solutions by calcite dissolution and the application to anoxic limestone drain design[J].Applied Geochemistry,23:148~165.
Johnson R H,Blowes D W,Robertson W D,et al.2000.The hydrogeochemistry of the Nickel Rim mine tailings impoundment,Sudbury,Ontario[J].Journal of Contaminant Hydrology,41:49~80.
Lei Liangqi,Lin Zheqiong,Mo Binji,et al.2016.Armoring effect of limestone in acid mine drainage:Static immersion experiments[J].Acta Petrologica et Mineralogica,35(3):553~562(in Chinese with English abstract).
Lei Liangqi,Shi Zhenghuan,Mo Jia,et al.2015.Characteristics of oxidation profile and acidification mechanism of a carbonate type tailings,Huangshaping Pb-Zn mine(Hunan Province,China)[J].Earth and Environment,43(2):173~182(in Chinese with English abstract).
Lei Liangqi,Song Ci’an,Xie Xiangli,et al.2011.Acidification characteristics and mechanism of carbonate-type tailings of Bali tailings storage,the Dachang tin-polymetallic orefield,Guangxi[J].Acta Petrologica et Mineralogica,30(1):141~149(in Chinese with English abstract).
Li Ling,Zhang Guoping,Liu Hong,et al.2009.Antimony and arsenic migration and environmental impacts on river draining in the Dachang multi-metalliferous mine area in Guangxi,China[J].Research of Environmental Sciences,22(6):682~687(in Chinese).
Li Xilin and Zhang Zhengen.1980.A restudy on sulfosalt mineral in an ore field in Guangxi province[J].Geochimica,2:172~185(in Chinese).
Liang Yali.2000.“10.18”event of Nandan tailings collapse[J].Coastal Environment,12:7(in Chinese).
Lindsay M B J,Condon P D,Jambor J L,et al.2009.Mineralogical,geochemical,and microbial investigation of a sulfide-rich tailings deposit characterized by neutral drainage[J].Applied Geochemistry,24:2 212~2 221.
Liu H Y,Probst A and Liao B H.2005.Metal contamination of soils and crops affected by the Chenzhou lead/zinc mine spill(Hunan,China)[J].Science of the Total Environment,339:153~166.
Lottermoser B G and Ashley P M.2006.Mobility and retention of trace elements in hardpan-cemented cassiterite tailings,north Queensland,Australia[J].Environmental Geology,50:835~846.
Mc Gregor R G,Blowes D W,Jambor J,et al.1998.Mobilization and attenuation of heavy metals within a nickel mine tailings impoundment near Sudbury,Ontario,Canada[J].Environmental Geology,36(3~4):305~319.
Moncur M C,Ptacek C J,Blowes D W,et al.2005.Release,transport and attenuation of metals from an old tailings impoundment[J].Applied Geochemistry,3:639~659.
Plante B,Bussière B and Benzaazoua M.2014.Lab to field scale effects on contaminated neutral drainage prediction from the Tio mine waste rocks[J].J.Geochem.Explor.,137:37~47.
Pope J and Trumm D.2015.Controls on Zn concentrations in acidic and neutral mine drainage from New Zealand’s bituminous coal and epithermal mineral deposits[J].Mine Water and the Environment,34:455~463.
Sherlockr E J,Lawrence R W,Poulin P,et al.1995.On the neutralization of acid rock drainage by carbonate and silicate minerals[J].Environment Geology,25:43~54.
Shu Wensheng,Zhang Zhiquan and Lan Chongyu.2001.Acid producing potential of a lead/zinc mine tailings at Lechang,Guangdong province[J].Environmental Science,22(3):113~117(in Chinese).
Soler J M,Boi M,Mogollón J L,et al.2008.The passivation of calcite by acid mine water.Column experiments with ferric sulfate and ferric chloride solutions at p H 2[J].Applied Geochemistry,12:3 579~3 588.
Souissi R,Souissi F,Chakroun H K,et al.2013.Mineralogical and geochemical characterization of mine tailings and Pb,Zn,and Cd mobility in a carbonate Setting(Northern Tunisia)[J].Mine Water and the Environment,32:16~27.
Tessier A,Campbell P G C and Bisson M.1979.Sequential extraction procedure for the speciation of particulate trace metals[J].Anal.Chem.,51:844~850.
Wisskirchen C,Dold B,Friese K,et al.2010.Geochemistry of highly acidic mine water following disposal into a natural lake with carbonate bedrock[J].Applied Geochemistry,8:1 107~1 119.
Zhai Limei,Chen Tongbin,Liao Xiaoyong,et al.2008.Pollution of agricultural soils resulting from a tailing spill at a Pb-Zn mine:A case study in Huanjiang,Guangxi Province[J].Acta Scientiae Circumstantiae,28(6):1 206~1 211(in Chinese with English abstract).
Zhang Xinying,Zhao Cailiu,Wu Haodong,et al.2008.Situation of heavy metal contamination in a typical mining town of Guangxi,south China[J].Environmental Monitoring in China,24(4):79~83(in Chinese).
Zhu Jibao,Chen Fanrong and Lu Long.2005.Heavy metal geochemistry behavior during the oxidation of the Fankou Pb-Zn mine tailings in Guangdong province and the implications for environmental remediation of the mines[J].Acta Scientiae Circumstantiae,25(3):414~422(in Chinese).
陈炳辉,万茉莉,王智美,等.2010.粤北大宝山多金属矿酸性矿山废水中氧化亚铁硫杆菌对黄铁矿的生物氧化作用研究[J].岩石矿物学杂志,29(5):562~568.
陈志强,苏亮,杨保疆.2005.广西南丹地区有色金属尾砂型人工矿床地质特征及其资源化[J].地质找矿论丛,20(增刊):139~144.
雷良奇,林哲琼,莫斌吉,等.2016.酸性矿山废水中石灰岩包壳作用研究[J].岩石矿物学杂志,35(3):553~562.
雷良奇,史振环,莫佳,等.2015.黄沙坪碳酸盐型尾矿氧化剖面组构及酸化机制[J].地球与环境,43(2):173~182.
雷良奇,宋慈安,谢襄漓,等.2011.广西大厂巴里碳酸盐型尾矿的酸化特征及机理[J].岩石矿物学杂志,30(1):141~149.
李玲,张国平,刘虹,等.2009.广西大厂多金属矿区河流中Sb和As的迁移及环境影响.环境科学研究[J].22(6):682~687.
李锡林,章振根.1980.广西某矿田中硫盐矿物的再研究[J].地球化学,2:172~185.
梁雅丽.2000.10.18南丹尾矿大坍塌[J].沿海环境,12:7.
束文圣,张志权,蓝崇钰.2001.广东乐昌铅锌尾矿的酸化潜力[J].环境科学,22(3):113~117.
翟丽梅,陈同斌,廖晓勇,等.2008.广西环江铅锌矿尾砂坝坍塌对农田土壤的污染及其特征[J].环境科学学报,28(6):1 206~1 211.
张新英,赵才流,吴浩东,等.2008.广西一个典型矿业镇环境中重金属污染分析[J].中国环境监测,24(4):79~83.
朱继保,陈繁荣,卢龙,等.2005.广东凡口Pb-Zn尾矿中重金属的表生地球化学行为及其对矿山环境修复的启示[J].环境科学学报,25(3):414~422.