张国忠^{1, 2,},
黄威²,
潘月鹏²,
顾梦娜²,
吕雪梅²,
倪雪²,
何月欣²,
刘博文²,
王跃思^{1, 2,,},
田世丽^2,,
1.甘肃农业大学林学院 兰州 730070
2.中国科学院大气物理研究所/大气边界层物理和大气化学国家重点实验室 北京 100029
基金项目: 国家重点研发计划项目2016YFD0800302
国家重点研发计划项目2016YFC0201802

详细信息

作者简介:张国忠, 主要研究方向为大气沉降、生态与环境。E-mail:zhangguozhong@dq.cern.ac.cn

通讯作者:王跃思, 主要研究方向为大气化学与环境, E-mail:wys@dq.cern.ac.cn
田世丽, 主要研究方向为大气化学, E-mail:tianshili@mail.iap.ac.cn

中图分类号:X592

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出版历程

收稿日期:2019-02-01
录用日期:2019-03-27
刊出日期:2019-08-01

Dry deposition flux of atmospheric heavy metals and its source apportionment in a typical farmland of Hebei Province

ZHANG Guozhong^{1, 2,},
HUANG Wei²,
PAN Yuepeng²,
GU Mengna²,
LYU Xuemei²,
NI Xue²,
HE Yuexin²,
LIU Bowen²,
WANG Yuesi^{1, 2,,},
TIAN Shili^2,,
1. College of Forestry, Gansu Agricultural University, Lanzhou 730070, China
2. State Key Laboratory of Atmospheric Boundary Layer Physics and Atmospheric Chemistry/Institute of Atmospheric Physics, Chinese Academy of Sciences, Beijing 100029, China
Funds: the National Key Research and Development Program of China2016YFD0800302
the National Key Research and Development Program of China2016YFC0201802

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Corresponding author:WANG Yuesi, E-mail: wys@dq.cern.ac.cn;TIAN Shili, E-mail: tianshili@mail.iap.ac.cn

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摘要
摘要:重金属是影响农田土壤环境质量和农产品品质的主要污染物，大气沉降是农田重金属的来源之一。长期以来，由于观测资料缺乏，对于我国农业区大气重金属的沉降量和来源认识一直不清楚。本研究基于河北典型农田连续1年的外场观测，测试分析了大气气溶胶9个粒径段中25种金属元素的含量，结合干沉降阻抗模型估算了这些金属的干沉降量，并利用PMF模型对其来源进行了解析。结果表明，该区域25种金属元素在细粒子（D_P ≤ 2.1 μm，D_P为空气动力学直径，下同）、粗粒子（2.1 < D_P ≤ 9 μm）和巨粒子（D_P>9 μm）中的质量浓度存在较大差异。重金属（如：Zn、Cd和Pb等）主要富集在细粒子，而地壳源的金属（如：Al、Fe和Th等）主要富集在粗粒子。大多数金属元素的浓度呈现冬春季高于夏秋季的变化特征。Cr是细粒子和粗粒子中质量浓度最高的重金属，其次为As、Zn、Pb、V和Sb。重金属中，Cr的大气干沉降量最高，达350.7 mg·m^-2·a^-1，其次是As、Sb和V，分别为153.4 mg·m^-2·a^-1、103.1 mg·m^-2·a^-1和102.3 mg·m^-2·a^-1。研究区域大气中金属元素的主要来源为道路扬尘、工业、矿尘、燃煤和机动车排放。巨粒子中的金属主要来自矿尘源（62.0%），细粒子中的金属主要来自燃煤、机动车和工业源（67.7%）。颗粒物的粒径越小，人为排放源的贡献越大，重金属的污染风险（富集因子）也越高。农田重金属污染防治需要充分考虑大气沉降的输入及来源的变化。
关键词:农田/
大气干沉降/
重金属/
源解析/
污染控制
Abstract:Atmospheric deposition is a major contributor of heavy metals contaminating the farmland, which endangers the quality of soil as well as agricultural products. Because of the paucity of relevant observational data, the dry deposition flux and sources of atmospheric heavy metals in agricultural areas have for long remained unclear. Based on a year of field observation in a typical farmland in Hebei Province, we measured the content of 25 elements in nine size-segregated particles. The dry deposition flux of atmospheric metal elements was estimated by employing resistance modeling. In addition, the sources of atmospheric metal elements were apportioned using the PMF model. The results indicated that there were large differences in the concentrations of 25 metals between the fine particles (D_P ≤ 2.1 μm, aerodynamic diameter, the same below), coarse particles (2.1 < D_P ≤ 9 μm), and giant particles (D_P>9 μm). Heavy metals (such as Zn, Cd, and Pb) were primarily concentrated in fine particles, whereas the crustal elements (such as Al, Fe, and Th) were primarily concentrated in coarse particles. The concentrations of most metals were higher in spring and in winter rather than in summer and autumn. Annual mean concentration of Cr was the highest among the heavy metals both in fine and coarse particles, followed by As, Zn, Pb, V, and Sb. Regarding the dry deposition flux, Cr also had the highest value of 350.7 mg·m^-2·a^-1, followed by As, Sb, and V, which were 153.4, 103.1, and 102.3 mg·m^-2·a^-1, respectively. The primary sources of atmospheric metal elements confined to the study area were road dust, industrial pollution, mineral dust, coal combustion and vehicle emission. The metals in the giant particles were primarily from dust source (62.0%), whereas the metals in the fine particles were primarily from coal, motor vehicles and industrial sources (totally 67.7%). With decrease in particle size, the contribution of anthropogenic pollution increased, thereby increasing the pollution risk (enrichment factor) of heavy metals. In conclusion, the study was critical in considering the input and sources of atmospheric deposition regarding regulation of farmland involving heavy metals.
Key words:Farmland/
Atmospheric dry deposition/
Heavy metals/
Source apportionment/
Pollution control

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图1研究区大气颗粒物中金属元素质量浓度的粒径分布
Figure1.Size distributions of metal elements in atmospheric particles of the study area


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图2研究区大气细、粗和巨粒子中金属元素年平均浓度
Figure2.Annual mean concentrations of metal elements in fine, coarse and giant atmospheric particles in the study area


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图3研究区大气细、粗和巨粒子颗粒物中金属元素在其总质量浓度中的占比
Figure3.Relative proportions of concentrations of metal elements in fine, coarse and giant atmospheric particles in the study area


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图4研究区大气细、粗和巨粒子中金属元素浓度季节变化
Figure4.Seasonal variations of concentrations of metal elements in fine, coarse and giant atmospheric particles in the study area


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图5研究区大气细、粗和巨粒子中金属元素年平均干沉降通量
Figure5.Annual mean dry deposition fluxes of metal metals in fine, coarse and giant atmospheric particles in the study area


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图6研究区大气细、粗和巨粒子中金属通量在其总通量中的占比
Figure6.Relative proportions of metal elements fluxes in fine, coarse and giant atmospheric particles in the study area


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图7本文计算的干沉降通量值与其他地区通量值范围的比较
观测值来源于文献, 其中: a代表文献[31]; b代表文献[33]; c代表文献[34]; d代表文献[28]; e代表文献[27]; f代表文献[32]; g代表文献[35]; h代表文献[36]; i代表文献[37]; j代表文献[38]。
Figure7.Comparison of dry deposition fluxes between the modeled values in this study and observed values in other areas
Observed values are derived from literatures, where: "a" stands for the literature [31]; "b" stands for the literature [33]; "c" stands for the literature [34]; "d" stands for the literature [28]; "e" stands for the literature [27]; "f" stands for the literature [32]; "g" stands for the literature [35]; "h" stands for the literature [36]; "i" stands for the literature [37]; "j" stands for the literature [38].


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图8研究区大气细、粗、巨粒子中金属元素富集因子
Figure8.Enrichment factors of various metal elements in fine, coarse and giant atmospheric particles in the study area


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图9研究区大气颗粒物中不同金属元素PMF源解析结果
Figure9.Profiles of sources of metal elements in atmospheric particles identified by PMF model in the study area


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图10研究区不同源在大气细、粗、巨粒子中金属元素的相对贡献
Figure10.Relative contributions of each identified source to metal elements in fine, coarse and giant atmospheric particles in the study area


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