Interaction of reactive mercury with surfaces and implications for atmospheric mercury speciation measurements

Interaction of reactive mercury with surfaces and implications for atmospheric mercury speciation measurements
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活性汞与表面的相互作用及其对大气汞形态测量的影响

DOI:
10.1016/j.atmosenv.2023.120240
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发表时间:
2024
影响因子:
5
通讯作者:
Gustin, Mae Sexauer
Gustin, Mae Sexauer
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Allen, Natalie;Gačnik, Jan;Dunham-Cheatham, Sarrah M.;Gustin, Mae Sexauer

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由于大气中活性汞(RM)的反应性和超痕量浓度,其准确测量提出了分析挑战。在过去的十年中,内华达州大学里诺分校-反应性汞活性系统(RMAS)用于RM测量的使用有所增加,因为它已被证明比行业标准Tekran 2537/1130/1135系统更准确。然而,RMAS测量也有局限性,包括与用于RM采样的膜相关的长时间分辨率和采样偏差。因此,我们研究了使用更高的采样流速,以减少采样时间和测试替代膜材料使用环境空气采样和受控实验室实验与气态氧化汞(GOM)校准器。结果表明,增加RMAS采样流量对确定的RM浓度有负面影响。在春季/夏季和冬季,2 L min− 1时的RM浓度分别比1 L min− 1时低10%和30-50%。然而,膜上捕获的RM的化学组成不受流速增加的影响。RMAS中目前使用的膜比许多具有类似成分的替代品表现更好,更有效地保留了汞。环境空气采样和实验室实验都表明,设计用于仅保留颗粒结合汞(PBM)的膜也保留了大量的GOM。基于硼硅酸盐玻璃设计的PBM膜保留超过70%的GOM。
Accurate measurement of atmospheric reactive mercury (RM) presents analytical challenges due to its reactivity and ultra-trace concentrations. In the last decade, use of the University of Nevada, Reno – Reactive Mercury Active System (RMAS) for RM measurements has increased, since it has been shown to be more accurate than the industry standard, the Tekran 2537/1130/1135 system. However, RMAS measurements also have limitations, including long time resolution and sampling biases associated with membranes used for RM sampling. We therefore investigated the use of higher sampling flow rates to reduce sampling time and tested alternative membrane materials using both ambient air sampling and controlled laboratory experiments with a gaseous oxidized mercury (GOM) calibrator. Results indicated that increasing the RMAS sampling flow had a negative impact on determined RM concentrations. RM concentrations at 2 L min−1were 10% and 30–50% lower than at 1 L min−1in spring/summer and winter, respectively. However, the chemical composition of RM captured on membranes was not impacted by the increased flow rate. Membranes currently used in the RMAS performed better than numerous alternatives with similar composition, retaining Hg more efficiently. Both ambient air sampling and laboratory experiments revealed that membranes designed to retain only particulate-bound mercury (PBM) also retained significant amounts of GOM. PBM membranes based on borosilicate glass designs retained more than 70% of GOM.
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