改进BCR法测定公路两旁表层土壤中铂钯铑的化学形态
Determination of Chemical Species of Platinum, Palladium and Rhodium in Roadside Surface Soil with a Modified BCR Method
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摘要: 铂、钯、铑是汽车催化转换器中的主要成分,在有效治理汽车尾气污染的同时,不断排放并在环境中累积增加,随着元素的迁移、转化及地下水的循环,可能成为一种新的环境污染问题。本文将改进的BCR顺序提取法应用于铂族元素形态分析,结合铂族元素的性质,将公路两旁表层土壤样品中Pt、Pd、Rh分为酸溶态、可还原态、可氧化态和残渣态四种形态。实验优化了原始的BCR浸取条件,利用电感耦合等离子体质谱法测定Pt、Pd、Rh的各形态。各形态的精密度、检出限满足地质矿产实验室测试质量管理规范的监控要求,各形态浸取量之和与样品各元素的总量之比(回收率)在95.3%~110.0%,说明方法具有较好的准确性和重现性。通过实际样品分析,公路两旁表层土壤样品中铂族元素非残渣态含量顺序为Pd(57.23%~58.03%)>Rh(22.64%~25.80%)>Pt(17.91~20.57%),研究认为铂族元素进入生物圈的几率是Pd>Rh>Pt。Abstract: Pt, Pd and Rh as the main ingredients in automotive catalytic converters, effectively reduce automobile exhaust pollution, but continuously emit into the environment. The migration, conversion and circulation in groundwater of these elements potentially generate new environmental pollution problems. In this paper the improved BCR sequential extraction method was applied to the chemical species analysis of platinum group elements (PGEs). Combined with the nature of the PGEs, the chemical species of Pt, Pd and Rh in roadside surface soil were divided into four fractions: acid soluble, reducible, oxidisable and residual. The original BCR leaching conditions were optimized and Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) was used to measure various chemical species of Pt, Pd and Rh. The precisions and detection limits of all the chemical species all met the monitoring requirements of the testing quality management for geological laboratories (DZ/T 0130—2006). All the recoveries were from 95.3% to 110.0%, which indicated the established method had good accuracy and reproducibility. The analysis results for actual samples of the surface soil samples on both sides of the road demonstrated the contents of PGEs in non-residual fraction were in order as Pd(57.23%-58.03%)>Rh(22.64%-25.80%)>Pt(17.91%-20.57%) and the probabilities for PGEs entering the biosphere were Pd> Rh> Pt.
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朱若华,邹红,贺闰娟.贵金属元素铂、铑、钯的分析进展[J].分析试验室,2004,23(2): 82-92. Tessier A, Campbell P G C, Bisson M. Sequential extra-ction procedure for the speciation of particulate trace-metals [J].Analytical Chemistry,1979,51(7): 844-851. Tessier A, Campbell P G C, Bisson M. Sequential extra-ction procedure for the speciation of particulate trace-metals [J].Analytical Chemistry,1979,51(7): 844-851.
李宇庆,陈玲,仇雁翎,赵建夫,李金柱.上海化学工业区土壤重金属元素形态分析[J].生态环境,2004,13(2): 154-155. 邵孝侯,邢光熹,侯文华.连续提取法区分土壤重金属元素形态的研究及应用[J].土壤学进展,1994,22(3): 40-44. 王学锋,杨艳琴.土壤-植物系统重金属形态分析和生物有效性研究进展[J].化工环境,2004, 24(1): 24-27. 吕彩芬,何红蓼,周肇如,支辛辛,李冰,张勤.锍镍试金-等离子体质谱法测定地球化学勘探样品中的铂族元素和金[J].岩矿测试,2002,21(1): 7-11. 赵素利,张欣,李曼,温宏利,屈文俊,曹亚萍,李超.锍镍试金-电感耦合等离子体质谱法测定硫铁矿中铂族元素[J].岩矿测试,2011,30(4): 412-415. 赵素利,张欣,温宏利,李超,屈文俊.锍镍试金富集-电感耦合等离子体质谱法测定黑色页岩中的铂族元素[J].岩矿测试,2011,30(6): 723-726. 刘少轻,施燕支,朱若华.铂族元素及形态分析进展[J].光谱实验室,2007,24(2): 43-49. 王娟,朱若华,施燕支.北京市公路两旁尘土中铂族元素的化学形态[J].环境化学,2007,26(4): 528-530. Quevauviller P, Rauret G, Griepink B. Single and sequential extraction in sediments and soils [J]. International Journal of Environmental Analytical Chemistry, 1993, 51(1-4):231-235. Quevauviller P, Rauret G, Griepink B. Single and sequential extraction in sediments and soils [J]. International Journal of Environmental Analytical Chemistry, 1993, 51(1-4):231-235.
Rauret G, López-Sánchez J F, Sahuquillo A, Rubio R, Davidson C, Ure A, Quevauviller P. Improvement of the BCR three step sequential extraction procedure prior to the certification of new sediment and soil reference materials [J]. Journal of Environmental Monitoring, 1999, 1(1): 57-61. Rauret G, López-Sánchez J F, Sahuquillo A, Rubio R, Davidson C, Ure A, Quevauviller P. Improvement of the BCR three step sequential extraction procedure prior to the certification of new sediment and soil reference materials [J]. Journal of Environmental Monitoring, 1999, 1(1): 57-61.
刘甜田,何滨,王亚韩,江桂斌,林海.改进BCR法在活性污泥样品重金属形态分析中的应用[J].分析试验室,2007,26(Z1): 17-20. 樊瑛,黄云,孟昭宇,缪明明,高诚伟.电感耦合等离子体质谱法测定尘土样品中贵金属元素的研究[J].干旱环境监测,2007,21(2): 71-74. Nischwitz V, Michalke B, Kettrup A. Speciation of Pt(Ⅱ) and Pt(Ⅳ) in spiked extracts from road dust using on-line liquid chromatography-inductively coupled plasma mass spectrometry [J]. Journal of Chromato-graphy A,2003,1016: 223-234. Nischwitz V, Michalke B, Kettrup A. Speciation of Pt(Ⅱ) and Pt(Ⅳ) in spiked extracts from road dust using on-line liquid chromatography-inductively coupled plasma mass spectrometry [J]. Journal of Chromato-graphy A,2003,1016: 223-234.
Nachtigall D, Kock H, Artelt S, Levsen K, Wünsch G, Rühle T, Schlögl R. Platinum solubility of a substance designed as a model for emissions of automobile catalytic converters [J].Fresenius' Journal of Analytical Chemistry, 1996, 354(5-6): 742-746. Nachtigall D, Kock H, Artelt S, Levsen K, Wünsch G, Rühle T, Schlögl R. Platinum solubility of a substance designed as a model for emissions of automobile catalytic converters [J].Fresenius' Journal of Analytical Chemistry, 1996, 354(5-6): 742-746.
刘爱菊,王洪海,刘家弟,李梦红.孝妇河水体沉积物中重金属的污染及形态分布特征[J].环境化学, 2010, 29(5): 875-879. 袁倬斌,吕元琦,张裕平,尹明.电感耦合等离子体质谱在铂族元素分析中的应用[J].冶金分析,2003,23(2): 24-30. Helmers E, Norbert Mergel. Platinum and rhodium in the polluted environment: Studying the emissions of automobile catalysts with emphasis on the application of CSV rhodium analysis [J]. Fresenius' Journal of Analytical Chemistry,1998,362: 522-528. Helmers E, Norbert Mergel. Platinum and rhodium in the polluted environment: Studying the emissions of automobile catalysts with emphasis on the application of CSV rhodium analysis [J]. Fresenius' Journal of Analytical Chemistry,1998,362: 522-528.
Wedepohl K H. The composition of the continental crust [J]. Geochimica et Cosmochimica Acta, 1995,59: 1217-1232. Wedepohl K H. The composition of the continental crust [J]. Geochimica et Cosmochimica Acta, 1995,59: 1217-1232.
Hodge V F, Stallard M O. Platinum and palladium in roadside dust [J]. Environmental Science & Technology ,1986,20(10): 1058-1060. Hodge V F, Stallard M O. Platinum and palladium in roadside dust [J]. Environmental Science & Technology ,1986,20(10): 1058-1060.
Niemelä M, Perämäki P, Piispanen J, Poikolainen J. Determination of platinum and rhodium in dust and plant samples using microwave assisted sample digest ion and ICP-MS [J]. Analytica Chimica Acta, 2004, 521: 137-142. Niemelä M, Perämäki P, Piispanen J, Poikolainen J. Determination of platinum and rhodium in dust and plant samples using microwave assisted sample digest ion and ICP-MS [J]. Analytica Chimica Acta, 2004, 521: 137-142.
Jackson M T, Sampson J, Prichard H M. Platinum and palladium variations through the urban environment: Evidence from 11 sample types from Sheffield, UK [J]. Science of the Total Environment,2007,385(1-3): 117-131. Jackson M T, Sampson J, Prichard H M. Platinum and palladium variations through the urban environment: Evidence from 11 sample types from Sheffield, UK [J]. Science of the Total Environment,2007,385(1-3): 117-131.
Zereini F, Alt F, Rankenberg K, Beyer J M, Artelt S. The distribution of platinum group elements (PGE) in the environmental compartments of soil, mud, roadside dust, road sweeping and water: Emission of the platinum group elements (PGE) from motor vehicle catalytic converters [J]. UWSF- Z Umveltchem kotox, 1997,9(4): 193-200. Zereini F, Alt F, Rankenberg K, Beyer J M, Artelt S. The distribution of platinum group elements (PGE) in the environmental compartments of soil, mud, roadside dust, road sweeping and water: Emission of the platinum group elements (PGE) from motor vehicle catalytic converters [J]. UWSF- Z Umveltchem kotox, 1997,9(4): 193-200.
Rauch S, Morrison G M. Platinum uptake by the freshwater isopod Asellus aquaticus in urban rivers [J]. Science of the Total Environment,1999,235(1-3): 261-268. Rauch S, Morrison G M. Platinum uptake by the freshwater isopod Asellus aquaticus in urban rivers [J]. Science of the Total Environment,1999,235(1-3): 261-268.
Müller M, Heumann K G.Isotope dilution inductively coupled plasma quadrupole mass spectrometry in connection with a chromatographic separation for ultra trace determinations of platinum group elements (Pt, Pd, Ru, Ir) in environmental samples [J]. Fresenius' Journal of Analytical Chemistry,2000,368(1): 109-115. Müller M, Heumann K G.Isotope dilution inductively coupled plasma quadrupole mass spectrometry in connection with a chromatographic separation for ultra trace determinations of platinum group elements (Pt, Pd, Ru, Ir) in environmental samples [J]. Fresenius' Journal of Analytical Chemistry,2000,368(1): 109-115.
Motelica-Heino M R, Morrison S, Donard G M. Deter-mination of palladium and rhodium concentrations in urban road sediments by laser ablation-ICP-MS [J]. Analytica Chimica Acta,2001,436: 233-244. Motelica-Heino M R, Morrison S, Donard G M. Deter-mination of palladium and rhodium concentrations in urban road sediments by laser ablation-ICP-MS [J]. Analytica Chimica Acta,2001,436: 233-244.
Petrucci F, Bocca B, Alimonti A, Caroli S. Determin-ation of Pd, Pt and Rh in airborne particulate and road dust by high resolution ICP-MS: A preliminary investigation of the emission from automotive catalysts in the urban area of Rome [J]. Journal of Analytical Atomic Spectrometry,2000,15: 525-528. Petrucci F, Bocca B, Alimonti A, Caroli S. Determin-ation of Pd, Pt and Rh in airborne particulate and road dust by high resolution ICP-MS: A preliminary investigation of the emission from automotive catalysts in the urban area of Rome [J]. Journal of Analytical Atomic Spectrometry,2000,15: 525-528.
Schramel P, Zischka M, Muntau H, Stojanik B, Dams R, Gómez M G, Quevauviller P. Collaborative evaluation of the analytical state-of-the-art of platinum, palladium and rhodium determinations in road dust [J]. Journal of Environmental Monitoring,2000, 2(5): 443-446. Schramel P, Zischka M, Muntau H, Stojanik B, Dams R, Gómez M G, Quevauviller P. Collaborative evaluation of the analytical state-of-the-art of platinum, palladium and rhodium determinations in road dust [J]. Journal of Environmental Monitoring,2000, 2(5): 443-446.
Rauch S, Motelica-Heino M, Morrison G, Donard O F X. Critical assessment of platinum group element determination in road and urban river sediments using ultrasonic nebulization and high resolution ICP-MS [J]. Journal of Analytical Atomic Spectrometry,2000,15: 329-334. Rauch S, Motelica-Heino M, Morrison G, Donard O F X. Critical assessment of platinum group element determination in road and urban river sediments using ultrasonic nebulization and high resolution ICP-MS [J]. Journal of Analytical Atomic Spectrometry,2000,15: 329-334.
Zereini F, Wiseman C, Alt F, Messerschmidt J, Müller J, Urban H. Platinum and rhodium concentrations in airborne particulate matter in Germany from 1988 to 1998 [J]. Environmental Science & Technology,2001,35(10): 1996-2000. Zereini F, Wiseman C, Alt F, Messerschmidt J, Müller J, Urban H. Platinum and rhodium concentrations in airborne particulate matter in Germany from 1988 to 1998 [J]. Environmental Science & Technology,2001,35(10): 1996-2000.
刘玉燕,刘敏,程书波.道路灰尘铂族元素含量的短期变化过程分析[J].环境科学学报,2009,29(9): 1864-1870. 举晓霞,朱若华.铂族元素在环境和生物样品中的积累及毒性研究进展[J].化学通报,2009(10): 881-888. 朱若华,刘少轻,施燕支.北京市城区环境和生物样品中痕量铂族元素的分布[J].环境化学,2008,27(3): 391-395. 单孝全,王仲文.形态分析与生物可给性[J].分析试验室,2001, 20(6): 103-108.
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