电感耦合等离子体发射光谱-逐级化学提取法研究低硫煤矸石中微量元素的赋存状态及其环境效应

丁帅帅; 郑刘根; 程桦

doi:10.15898/j.cnki.11-2131/td.2015.06.005

电感耦合等离子体发射光谱-逐级化学提取法研究低硫煤矸石中微量元素的赋存状态及其环境效应

安徽大学资源与环境工程学院, 矿山环境修复与湿地生态安全协同创新中心, 安徽合肥 230601

基金项目: 国家自然科学基金资助项目(41373108);安徽省国土资源科技项目(2013-K-07);淮北矿业(集团)科技攻关项目(2014-HBKJ-01);煤矿生态环境保护国家工程实验室科技攻关项目(HNKY-JT-JS2013-41)

详细信息

作者简介: 丁帅帅，硕士研究生，环境科学专业。E-mail：ssding1992@163.com; 刘根，博士，副教授，主要从事矿区污染物环境地球化学研究。E-mail：lgzheng@ustc.edu.cn

中图分类号: O657.31;TQ533.6

收稿日期: 2015-07-09

修回日期: 2015-10-30

录用日期: 2015-11-10

刊出日期: 2015-06-25

Study on the Occurrence of Trace Elements in Low-sulfur Coal Gangue and Their Environmental Effect by Inductively Coupled Plasma-Optical Emission Spectrometry with Sequential Extraction Procedure

School of Resource and Environmental Engineering, Collaborative Innovation Center for Mines Environmental Remediation and Wetland Ecological Security, Anhui University, Hefei 230601, China

Received Date: 09 July 2015

Revised Date: 30 October 2015

Accepted Date: 10 November 2015

Publish Date: 25 June 2015

摘要

摘要:
煤矸石是我国堆存量最大的工业固体废物, 本文应用电感耦合等离子体发射光谱法、逐级化学提取法和相关性分析研究了淮北临涣矿区低硫煤矸石中10种微量元素的含量及赋存状态, 并运用风险评价指数法评价其环境效应。结果表明, 低硫煤矸石中Ba、Co、Cr、Mn、Ni、Pb、V含量均高于淮北煤和中国煤均值, Mn、V的富集系数大于1, 有一定迁移风险。微量元素主要以残渣态和铁锰氧化物结合态存在, 两者质量分数之和为68.87%~92.93%, 其中Cd、Co、Cr、Cu、Ni、Pb、Zn赋存于硫化物矿物中, V赋存于黏土矿物中, Mn赋存于碳酸盐矿物和硫化物矿物中。10种微量元素对环境的危害性大小为:Mn >Zn >Ni >Pb >Cd >Cu >Ba >V >Cr >Co, 表明低硫煤矸石堆存过程中活性态Mn对生态环境造成危害的可能性最大, 由Mn可能引起的煤矸石山周边地区土壤及水体污染应当重视。
- 低硫煤矸石 /
- 微量元素 /
- 电感耦合等离子体发射光谱法 /
- 逐级化学提取法 /
- 赋存状态 /
- 环境效应
Abstract:
Coal gangue is the largest industrial solid waste in China. Trace elements in low-sulfur coal gangue samples from the Linhuan coal mining area in the Huaibei coalfield were measured by Inductively Coupled Plasma-Optical Emission Spectrometry(ICP-OES). Sequential extraction procedure and correlation analysis were employed to analyze the occurrence of trace elements in coal gangue. Meanwhile, the environmental effect of trace elements was studied by Risk Assessment Code(RAC). The results showed that trace elements(Ba, Co, Cr, Mn, Ni, Pb and V) were enriched in coal gangue compared with Huaibei coals and Chinese coals, in which the enrichment factors of Mn and V were greater than 1, indicating a certain risk of migration. Trace elements predominantly occur in residual and Fe-Mn oxide bound, the total quality fractions of which range from 68.87% to 92.93%. Cd, Co, Cu, Ni, Pb and Zn are hosted in sulfide minerals, V is hosted in clay minerals, and Mn mainly in carbonate minerals. The environmental hazard of trace elements was in order of Mn >Zn >Ni >Pb >Cd >Cu >Ba >V >Cr >Co, indicating that active Mn most likely pollutes the environment during the outdoor storage of coal gangue and the soil and water pollution induced by Mn should be of concern.
- low-sulfur coal gangue /
- trace elements /
- Inductively Coupled Plasma-Optical Emission Spectrometry /
- sequential extraction procedure /
- occurrence status /
- environmental effects

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图 1 微量元素的逐级化学提取实验结果

Figure 1.

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表 1 煤矸石中微量元素的含量与文献数据的对比

Table 1. The concentration of trace elements in coal gangue sample and comparison of analytical results with relative references

微量元素	本研究的低硫煤矸石样品		淮北煤均值^a (mg/kg)	中国煤均值^b (mg/kg)	黑色页岩^c (mg/kg)	克拉克值^d (mg/kg)	富集系数 (EF)
微量元素	含量范围(mg/kg)	平均值(mg/kg)	淮北煤均值^a (mg/kg)	中国煤均值^b (mg/kg)	黑色页岩^c (mg/kg)	克拉克值^d (mg/kg)	富集系数 (EF)
Ba	330.97~439.43	404.54	184.0	243.37	270~800	425.0	0.95
Cd	0.09~0.19	0.14	-	0.24	2~12	0.2	0.69
Co	11.20~32.01	17.34	9.2	7.05	10~30	25.0	0.69
Cr	39.13~53.39	46.60	34.2	15.35	50~160	100.0	0.47
Cu	4.78~13.57	9.34	48.2	18.35	35~150	55.0	0.17
Mn	103.29~373.02	194.64	20.0	125.00	200~800	100.0	1.95
Ni	10.75~35.08	18.18	16.4	13.71	40~140	75.0	0.24
Pb	22.65~38.17	29.61	18.0	15.55	10~40	-	-
V	108.47~216.20	180.10	108.0	35.05	100~400	135.0	1.33
Zn	26.18~87.63	51.28	304.0	42.18	60~300	70.0	0.73
注：a引自Zheng等^[10]、杨萍玥等^[11]，b引自任德贻等^[12]，c引自Ketris等^[13]，d引自Taylor^[14]；EF为富集系数，即煤矸石中微量元素平均含量与克拉克值之比；“-”表示暂无数据。

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表 2 煤矸石中微量元素与灰分、Al、Ca、Fe和S之间的Pearson相关系数(p < 0.05)

Table 2. The Pearson's correlation coefficients (p < 0.05) of trace elements with Al, Ca, Fe, S and ash yield in coal gangue sample

相关系数	r>0.7	0.7>r>0.5	0.5>r>0.35
与灰分	-	Ba(0.521) V(0.594)	-
与Al	V(0.967)	-	-
与Ca	-	-	Mn(0.369)
与Fe	Cu(0.627), V(0.816)	Pb(0.541)	Cr(0.481)
与S	Cd(0.722), Co(0.703) Cu(0.864), Ni(0.752)	Cr(0.630) Zn(0.523)	Mn(0.397)
元素之间	Co-Ni=0.997，Co-Zn=0.876 Ni-Zn=0.863，Co-Mn=0.803 Mn-Ni=0.794，Cd-Zn=0.722	-	-
注：“-”表示没有在此相关性范围内的元素。

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表 3 煤矸石中微量元素的环境效应

Table 3. The environmental effect of trace elements in coal gangue sample

微量元素	ERL~ERM (mg/kg)	各效应范围的样品数(%)			本项研究样品的RAC值		RAC值对应的风险程度^a
微量元素	ERL~ERM (mg/kg)	< ERL	> ERL且 < ERM	> ERM	范围	平均值	RAC值	风险程度
Ba	-	-	-	-	7.43~10.04	8.41	< 1	无
Cd	1.2~9.6	100	0	0	8.69~14.53	11.7
Co	-	-	-	-	1.56~6.04	3.87	1~10	轻度
Cr	81~370	100	0	0	3.61~6.40	4.7
Cu	34~270	100	0	0	8.64~12.64	10.19	10~30	中度
Mn	-	-	-	-	23.87~27.93	26.02
Ni	20.9~51.6	86	14	0	14.43~16.13	15.27	30~50	重度
Pb	46.7~218	100	0	0	9.65~16.65	11.97
V	-	-	-	-	5.38~10.65	8	>50	极严重
Zn	150~410	100	0	0	14.49~17.49	15.76
注：a引自Jain^[29]、刘春华等^[30]；ERL为效应浓度低值，ERM为效应浓度中值，RAC为风险评价指数；“-”表示暂无数据。

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电感耦合等离子体发射光谱-逐级化学提取法研究低硫煤矸石中微量元素的赋存状态及其环境效应

安徽大学资源与环境工程学院, 矿山环境修复与湿地生态安全协同创新中心, 安徽 合肥 230601

作者简介: 丁帅帅，硕士研究生，环境科学专业。E-mail：ssding1992@163.com; 刘根，博士，副教授，主要从事矿区污染物环境地球化学研究。E-mail：lgzheng@ustc.edu.cn

Study on the Occurrence of Trace Elements in Low-sulfur Coal Gangue and Their Environmental Effect by Inductively Coupled Plasma-Optical Emission Spectrometry with Sequential Extraction Procedure

School of Resource and Environmental Engineering, Collaborative Innovation Center for Mines Environmental Remediation and Wetland Ecological Security, Anhui University, Hefei 230601, China

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安徽大学资源与环境工程学院, 矿山环境修复与湿地生态安全协同创新中心, 安徽合肥 230601