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总悬浮颗粒(TSP)是粒径<100 μm的气溶胶粒子的总称. 大气中的气溶胶能吸收和散射太阳辐射,直接影响地表辐射强度和温度,也可以作为云凝结核或冰核,间接影响全球气候[1 − 3]. 此外细颗粒气溶胶(粒径小于2.5 μm)还能进入人体肺部,影响人体呼吸道与心血管健康[4 − 5].
海洋覆盖了地球71%的表面,海洋气溶胶长距离传输和沉降在海洋生源要素的循环中扮演重要的角色[6]. 海洋气溶胶来源包括一次来源(例如海盐和矿物等)和二次生成的无机和有机组分[7]. 其中,海盐是海洋大气气溶胶中最主要的自然源,全球每年大约有 3300 Tg海盐颗粒物通过风和波浪的作用进入大气[8]. 矿物颗粒物主要来源陆地传输,且研究表明东亚地区每年向大气传输约31—96 Tg沙尘,其中近 50%传输至太平洋[9]. 二次气溶胶主要是人为及自然源释放到大气中的气体(NOx、SO2和NH3等)在大气中通过一系列大气化学反应生成二次气溶胶(SO42−、NO3−和NH4+等)[10]. 陆地和人为活动释放到大气中的物质通过季风输送至我国近海及开阔大洋的大气[11],并通过干湿沉降到上层海洋,引起了海水酸化[12]. 无机氮(NO3−和NH4+)沉降到上层海洋后直接改变表层海水的N和P的比值,进而影响海洋初级生产力与全球氮循环[13 − 15].
对于西太平洋地区气溶胶的研究主要集中在西北太平洋及其边缘海(南海、黄海、东海和日本海等)[16 − 20],对赤道西太平洋的研究较少. 本研究以热带西太平洋为研究区域,通过航次采集了TSP样本,分析了TSP中主要水溶性离子的浓度,探讨了各离子的潜在来源以及估算西太平洋无机氮干沉降通量.
冬季西太平洋TSP水溶性离子空间分布特征、来源和氮沉降
Spatial distribution and origin of TSP water-soluble ions, and nitrogen dry deposition in the Western Pacific Ocean in winter
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摘要: 2015年12月5日至2016年1月10日,通过航次在西太平洋(WPO)采集了29个大气总悬浮颗粒物(TSP)样本,分析了TSP样本中水溶性离子(Na+、K+、NH4+、Mg2+、Ca2+、NO3−、SO42−)的浓度. 结合气团后向轨迹、化学计量学关系和主成分分析,对TSP中水溶性离子来源进行了分析. 结果显示,水溶性离子的总浓度的顺序为:Na+ >SO42− >Mg2+ >NO3− >Ca2+ >K+ >NH4+,其中Na+质量浓度为 (6.76 ± 5.92) μg·m−3,占总离子的52.0%;SO42−质量浓度 (3.78 ± 3.81) μg·m−3,占总离子浓度29.1%. SO42−、NO3−、NH4+ 和Ca2+浓度从近海到开阔大洋呈现明显的下降趋势,表明人为排放源和地壳源对近海海洋气溶胶中NO3−、NH4+ 和Ca2+的影响较大. 无机氮沉降通量在近海 (3.47 ± 2.44) mg·m−2·d−1明显高于开阔大洋 (0.20 ± 0.07) mg·m−2·d−1.Abstract: A total of 29 total suspended particulates (TSP) were collected over the Western Pacific Ocean (WPO) from December 5, 2015 to January 10, 2016 by cruise. Concentrations of water-soluble inorganic ions (Na+、K+、NH4+、Mg2+、Ca2+、NO3−、SO42−) were analyzed. The sources of water-soluble inorganic ions were investigated by together with air masses backward trajectories, stoichiometric analysis and principal component analysis. Results showed that the order of concentrations of water-soluble inorganic ions are Na+ > SO42− > Mg2+ > NO3− > Ca2+ > K+ > NH4+. Na+ ((6.76 ± 5.92) μg·m−3) and SO42− ((3.78 ± 3.81) μg·m−3) were the main ions, accounted for 52.0% and 29.1% mass concentrations of water-soluble inorganic ions. Concentrations of SO42−、NO3−、NH4+ and Ca2+ displayed decreased patterns from the offshore to the open ocean, suggested that the contributions of anthropogenic emissions and crust to those ions. The dry deposition fluxes of NO3− and NH4+ in offshore ((3.47 ± 2.44) mg·m−2·d−1) were obviously higher than those in open ocean ((0.20 ± 0.07) mg·m−2·d−1).
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Key words:
- western pacific ocean /
- TSP /
- water-soluble ions /
- source apportionment /
- nitrogen deposition.
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表 1 西太平洋冬季大气气溶胶中水溶性离子的浓度(µg·m−3)
Table 1. Concentrations of water-soluble ions in the atmospheric aerosols of Western Pacific in winter (μg·m−3)
Na+/(μg·m−3) NH4+/(μg·m−3) K+/(μg·m−3) Mg2+/(μg·m−3) Ca2+/(μg·m−3) SO42−/(μg·m−3) NO3−/(μg·m−3) 最大值 26.1 2.58 0.94 3.84 1.37 13.9 7.64 最小值 0.95 0.01 0.04 0.08 0.06 0.46 0.07 均值±标准差 6.76±5.92 0.21±0.50 0.25±0.22 0.83±0.80 0.36±0.27 3.78±3.81 0.80±1.79 表 2 冬季西太平洋TSP中水溶性离子相关性分析
Table 2. Correlation analysis of spring TSP water-soluble ions
开阔大洋(n = 24)
The open seaNa+ NH4+ K+ Mg2+ Ca2+ SO42− NO3− Na+ 1 NH4+ −0.19 1 K+ 0.998** −0.158 1 Mg2+ 0.993** −0.264 0.991** 1 Ca2+ 0.909** 0.046 0.914** 0.893** 1 SO42− 0.286 0.834** 0.321 0.218 0.420* 1 NO3− 0.209 −0.074 0.219 0.239 0.135 0.058 1 近海海域(n = 5)
Offshore areasNa+ NH4+ K+ Mg2+ Ca2+ SO42− NO3− Na+ 1 NH4+ −0.496 1 K+ 0.987** −0.352 1 Mg2+ 0.984** −0.509 0.966** 1 Ca2+ 0.903* −0.205 0.933* 0.939* 1 SO42− 0.536 0.319 0.652 0.55 0.727 1 NO3− 0.039 0.762 0.188 −0.055 0.151 0.608 1 注:*和**表示相关性达到显著(P < 0.05)和极显著水平(P < 0.01).
Note: * and ** indicate significant (P<0.05) and extremely significant levels of correlation (P < 0.01).表 3 主成分旋转因子载荷矩阵
Table 3. Rotated component matrix of major components
开阔大洋(n = 24)
The open sea近海海域(n = 5)
Offshore areas离子Ions 因子1Factor 1 因子2Factor 2 因子1Factor 1 因子2Factor 2 Na+ 0.988 −0.102 0.976 −0.153 NH4+ −0.087 0.985 −0.35 0.91 K+ 0.992 −0.068 0.99 0.009 Mg2+ 0.98 −0.177 0.98 −0.194 Ca2+ 0.945 0.115 0.964 0.087 SO42− 0.38 0.904 0.691 0.632 NO3− 0.268 −0.097 0.137 0.936 方差贡献率 57.7% 26.5% 63.5% 31.0% 累计贡献率 57.7% 84.2% 63.5% 94.5% 可能来源 海洋源 二次源 海洋源 二次源 表 4 冬季各地及本研究的无机氮沉降通量比较
Table 4. Comparison of inorganic nitrogen deposition fluxes in different regions with this study during winter
DDF NO3−-N/(mg·m−2·d−1) NH4+-N/(mg·m−2·d−1) Inorganic N/(mg·m−2·d−1) 开阔大洋(本研究) 0.14±0.60 0.05±0.05 0.20±0.07 近海海域(本研究) 2.78±2.61 0.71±0.71 3.47±2.44 太平洋西边界航线[29] 0.95±2.93 0.36±0.35 1.29±2.97 彭佳屿[28] 3.38±2.31 1.38±1.03 4.75±3.26 冲绳岛[30] 1.31±0.58 0.54±0.27 1.84±0.85 南海[27] 0.83±0.84 0.64±0.42 1.47±1.26 东海[27] 3.78±3.06 0.97±0.62 4.75±3.67 黄渤海[27] 5.24±2.95 2.02±0.88 7.26±3.83 -
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