Oxalate Formation Enhanced by Fe-Containing Particles and Environmental Implications

被引:47
作者
Zhang, Guohua [1 ,2 ]
Lin, Qinhao [1 ,2 ]
Peng, Long [1 ,2 ,3 ]
Yang, Yuxiang [1 ,2 ,3 ]
Jiang, Feng [1 ,2 ,3 ]
Liu, Fengxian [1 ,2 ,3 ]
Song, Wei [1 ,2 ]
Chen, Duohong [4 ]
Cai, Zhang [5 ]
Bi, Xinhui [1 ,2 ]
Miller, Mark [6 ]
Tang, Mingjin [1 ,2 ]
Huang, Weilin [6 ]
Wang, Xinming [1 ,2 ]
Peng, Ping'an [1 ,2 ]
Sheng, Guoying [1 ,2 ]
机构
[1] Chinese Acad Sci, Guangzhou Inst Geochem, State Key Lab Organ Geochem, Guangzhou 510640, Guangdong, Peoples R China
[2] Chinese Acad Sci, Guangzhou Inst Geochem, Guangdong Key Lab Environm Resources Utilizat & P, Guangzhou 510640, Guangdong, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100039, Peoples R China
[4] Guangdong Environm Monitoring Ctr, State Environm Protect Key Lab Reg Air Qual Monit, Guangzhou 510308, Guangdong, Peoples R China
[5] Penn State Univ, John & Willie Leone Family Dept Energy & Mineral, University Pk, PA 16802 USA
[6] Rutgers State Univ, Dept Environm Sci, New Brunswick, NJ 08901 USA
关键词
SECONDARY ORGANIC AEROSOL; BIOMASS-BURNING AEROSOLS; PEARL RIVER DELTA; OXALIC-ACID; DICARBOXYLIC-ACIDS; MIXING STATE; IRON SOLUBILITY; CHEMICAL-CHARACTERIZATION; MOLECULAR-DISTRIBUTIONS; KETOCARBOXYLIC ACIDS;
D O I
10.1021/acs.est.8b05280
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
We used a single particle mass spectrometry to online detect chemical compositions of individual particles over four seasons in Guangzhou. Number fractions (Nfs) of all the measured particles that contained oxalate were 1.9%, 5.2%, 25.1%, and 15.5%, whereas the Nfs of Fe-containing particles that were internally mixed with oxalate were 8.7%, 23.1%, 45.2%, and 31.2% from spring to winter, respectively. The results provided the first direct field measurements for the enhanced formation of oxalate associated with Fe-containing particles. Other oxidized organic compounds including formate, acetate, methylglyoxal, glyoxylate, purivate, malonate, and succinate were also detected in the Fe-containing particles. It is likely that reactive oxidant species (ROS) via Fenton reactions enhanced the formation of these organic compounds and their oxidation product oxalate. Gas-particle partitioning of oxalic acid followed by coordination with Fe might also partly contribute to the enhanced oxalate. Aerosol water content likely, played an important role in the enhanced oxalate formation when the relative humidity is >60%. Interactions with Fe drove the diurnal variation of oxalate in the Fe-containing particles. The study could provide a reference for model simulation to improve understanding on the formation and fate of oxalate, and the evolution and climate impacts of particulate Fe.
引用
收藏
页码:1269 / 1277
页数:9
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