Partitioning of metal species during an enriched fuel combustion experiment. speciation in the gaseous and particulate phases.
Partitioning of metal species during an enriched fuel combustion experiment. speciation in the gaseous and particulate phases.
复制标题
富集燃料燃烧实验期间金属物质的分配。
DOI：
10.1021/es034408i
复制
发表时间：
2004
影响因子：
11.4
通讯作者：
O. Donard
中科院分区：
文献类型：
--
作者：
M. Pavageau;A. Morin;F. Séby;C. Guimon;E. Krupp;C. Pécheyran;J. Poulleau;O. Donard
燃烧过程是大气中最重要的金属来源，需要更好地了解燃烧过程，以改进烟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。轻质燃料油富含以下元素的 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。所得混合物在受控条件下在中试规模的燃料燃烧锅炉中燃烧。过滤颗粒后，通过加热的采样管同时采用标准化的基于洗瓶的采样技术和低温对烟囱中的气态物质进行采样。在 -80 摄氏度下收集低温样品，通过 LT/GC-ICPMS 进行进一步形态分析。三种硒和两种汞被证明是烟道气中的挥发性物质。热力学预测和实验表明烟气中存在以下挥发性金属物质：H2Se、CSSe、CSe2、SeCl2、Hg(0) 和 HgCl2。还讨论了低温技术和基于洗瓶的采样方法之间的挥发性金属物质的定量比较。关于金属分配，结果表明，在这些条件下，颗粒物中至少有 60%（按重量计）的元素 Pb、Sn、Cu、Co、Tl、Mn、V、Cr、Ni、Zn、Cd 和 Sb 混合到燃料中。对于颗粒中的 As 和 Se，分别检测到 37% 和 17%，并且未发现颗粒汞。通过 XPS 进行颗粒中的直接金属形态分析，可测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 测定颗粒物中无机 Cr、As 和 Se 的水溶性物质，并以氧化态 Cr(III)、As(V) 和 Se(IV) 进行鉴定。
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 degrees C 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: H2Se, CSSe, CSe2, SeCl2, Hg(0), and HgCl2. 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, Tl, 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 particulate 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).