GSTDTAP  > 地球科学
DOI10.5194/acp-17-465-2017
In situ and denuder-based measurements of elemental and reactive gaseous mercury with analysis by laser-induced fluorescence results from the Reno Atmospheric Mercury Intercomparison Experiment
Hynes, Anthony J.1; Everhart, Stephanie1; Bauer, Dieter1; Remeika, James1; Ernest, Cheryl Tatum1,2
2017-01-10
发表期刊ATMOSPHERIC CHEMISTRY AND PHYSICS
ISSN1680-7316
EISSN1680-7324
出版年2017
卷号17期号:1
文章类型Article
语种英语
国家USA; Germany
英文摘要

The University of Miami (UM) deployed a sequential two-photon laser-induced fluorescence (2P-LIF) instrument for the in situ measurement of gaseous elemental mercury, Hg(0), during the Reno Atmospheric Mercury Intercomparison Experiment (RAMIX) campaign. A number of extended sampling experiments, typically lasting 6-8 h but on one occasion extending to similar to 24 h, were conducted, allowing the 2P-LIF measurements of Hg(0) concentrations to be compared with two independently operated instruments using gold amalgamation sampling coupled with cold vapor atomic fluorescence spectroscopic (CVAFS) analysis. At the highest temporal resolution, similar to 5 min samples, the three instruments measured concentrations that agreed to within 10-25 %. Measurements of total mercury (TM) were made by using pyrolysis to convert total oxidized mercury (TOM) to Hg(0). TOM was then obtained by difference. Variability in the ambient Hg(0) concentration limited our sensitivity for measurement of ambient TOM using this approach. In addition, manually sampled KCl-coated annular denuders were deployed and analyzed using thermal dissociation coupled with single-photon LIF detection of Hg(0). The TOM measurements obtained were normally consistent with KCl denuder measurements obtained with two Tekran speciation systems and with the manual KCl denuder measurements but with very large uncertainty. They were typically lower than measurements reported by the University of Washington (UW) Detector for Oxidized Hg Species (DOHGS) system. The ability of the 2P-LIF pyrolysis system to measure TM was demonstrated during one of the manifold HgBr2 spikes but the results did not agree well with those reported by the DOHGS system. The limitations of the RAMIX experiment and potential improvements that should be implemented in any future mercury instrument intercomparison are discussed. We suggest that instrumental artifacts make a substantial contribution to the discrepancies in the reported measurements over the course of the RAMIX campaign. This suggests that caution should be used in drawing significant implications for the atmospheric cycling of mercury from the RAMIX results.


领域地球科学
收录类别SCI-E
WOS记录号WOS:000393756100005
WOS关键词AIRBORNE INSTRUMENT INTERCOMPARISONS ; OXIDIZED MERCURY ; METHYLMERCURY EXPOSURE ; EXPERIMENT RAMIX ; HEALTH ; UNCERTAINTIES ; DEPLOYMENT ; DIOXIDE ; AIR
WOS类目Environmental Sciences ; Meteorology & Atmospheric Sciences
WOS研究方向Environmental Sciences & Ecology ; Meteorology & Atmospheric Sciences
引用统计
文献类型期刊论文
条目标识符http://119.78.100.173/C666/handle/2XK7JSWQ/24939
专题地球科学
作者单位1.Univ Miami, Rosenstiel Sch Marine & Atmospher Sci, Dept Marine & Atmospher Chem, 4600 Rickenbacker Causeway, Miami, FL 33149 USA;
2.Max Planck Inst Chem, Atmospher Chem Dept, Hahn Meitner Weg 1, D-55128 Mainz, Germany
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Hynes, Anthony J.,Everhart, Stephanie,Bauer, Dieter,et al. In situ and denuder-based measurements of elemental and reactive gaseous mercury with analysis by laser-induced fluorescence results from the Reno Atmospheric Mercury Intercomparison Experiment[J]. ATMOSPHERIC CHEMISTRY AND PHYSICS,2017,17(1).
APA Hynes, Anthony J.,Everhart, Stephanie,Bauer, Dieter,Remeika, James,&Ernest, Cheryl Tatum.(2017).In situ and denuder-based measurements of elemental and reactive gaseous mercury with analysis by laser-induced fluorescence results from the Reno Atmospheric Mercury Intercomparison Experiment.ATMOSPHERIC CHEMISTRY AND PHYSICS,17(1).
MLA Hynes, Anthony J.,et al."In situ and denuder-based measurements of elemental and reactive gaseous mercury with analysis by laser-induced fluorescence results from the Reno Atmospheric Mercury Intercomparison Experiment".ATMOSPHERIC CHEMISTRY AND PHYSICS 17.1(2017).
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