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Partitioning of Metal Species during an Enriched Fuel Combustion Experiment Speciation in the Gaseous and Particulate Phases

机译:气相和颗粒相中富油燃烧实验形态中金属种类的划分

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摘要

Combustion processes are the most important source of metal in the atmosphere and need to be better understood to improve flue gas treatment and health impact studies. This combustion experiment was designed to study metal partitioning and metal speciation in the gaseous and particulate phases. A light fuel oil was enriched with 15 organometallic compounds of the following elements; Pb, Hg, As, Cu, Zn, Cd, Se, Sn, Mn, V, Tl, Ni, Co, Cr, and Sb. The resulting mixture was burnt in a pilot-scale fuel combustion boiler under controlled conditions. After filtration of the particles, the gaseous species were sampled in the stack through a heated sampling tube simultaneously by standardized washing bottles-based sampling techniques and cryogenically. The cryogenic samples were collected at -80℃ for further speciation analysis by LT/GC-ICPMS. Three species of selenium and two of mercury were evidenced as volatile species in the flue gas. Thermodynamic predictions and experiments suggest the following volatile metal species to be present in the flue gas: H{sub}2Se, CSSe, CSe{sub}2, SeCI{sub}2, Hg{sup}0, and HgCI{sub}2. Quantification of volatile metal species in comparison between cryogenic techniques and the washing bottles-based sampling method is also discussed. Concerning metal partitioning, the results indicated that under these conditions, at least 60% (by weight) of the elements Pb, Sn, Cu, Co, Ti, Mn, V, Cr, Ni, Zn, Cd, and Sb mixed to the fuel were found in the particulate matter. For As and Se, 37 and 17%, respectively, were detected in the particles, and no particuiate mercury was found. Direct metal speciation in particles was performed by XPS allowing the determination of the oxidation state of the following elements: Sb(V), Tl(III), Mn(IV), Cd(II), Zn(II), Cr(III), Ni(II), Co(II), V(V), and Cu(II). Water soluble species of inorganic Cr, As, and Se in particulate matter were determined by HPLC/ICP-MS and identified in the oxidation state Cr(III), As(V), and Se(IV).
机译:燃烧过程是大气中最重要的金属来源,需要更好地理解燃烧过程以改善烟道气处理和健康影响研究。该燃烧实验旨在研究气相和颗粒相中的金属分配和金属形态。轻质燃油富含以下元素的15种有机金属化合物; Pb,Hg,As,Cu,Zn,Cd,Se,Sn,Mn,V,Tl,Ni,Co,Cr和Sb将所得混合物在中试规模的燃料燃烧锅炉中在受控条件下燃烧。过滤颗粒后,通过基于加热瓶的标准化采样瓶技术,同时通过低温采样管,通过加热的采样管对气态样品进行采样。在-80℃下收集低温样品,以通过LT / GC-ICPMS进行进一步的形态分析。烟气中有3种硒和2种汞被证明是挥发性物质。热力学预测和实验表明,烟气中存在以下挥发性金属物质:H {sub} 2Se,CSSe,CSe {sub} 2,SeCl {sub} 2,Hg {sup} 0和HgCl {sub} 2 。还讨论了低温技术与基于洗瓶的采样方法之间的比较,对挥发性金属种类的定量。关于金属分配,结果表明在这些条件下,至少60%(按重量计)的元素Pb,Sn,Cu,Co,Ti,Mn,V,Cr,Ni,Zn,Cd和Sb混合到了金属中。在颗粒物中发现了燃料。对于砷和硒,在颗粒中分别检测到37%和17%,并且没有发现汞。通过XPS在颗粒中进行直接金属形态分析,从而可以确定以下元素的氧化态:Sb(V),Tl(III),Mn(IV),Cd(II),Zn(II),Cr(III) ,Ni(II),Co(II),V(V)和Cu(II)。通过HPLC / ICP-MS测定了颗粒状物质中无机Cr,As和Se的水溶性物质,并以氧化态Cr(III),As(V)和Se(IV)进行了鉴定。

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