中國東部陸架海大氣氣溶膠中主要化學(xué)組成與來源分析
發(fā)布時(shí)間：2018-09-18 15:00
【摘要】：受陸地和海洋地共同影響，中國東部陸架海大氣氣溶膠中主要化學(xué)組成及其來源非常復(fù)雜，不僅如此大氣氣溶膠還可通過直接和間接輻射等方式影響大氣輻射平衡，影響全球環(huán)境。本文以中國黃渤海和東海為研究對(duì)象，分別對(duì)2012年春季和秋季黃渤海，2011年冬季、2012年夏季和秋季東海海域進(jìn)行大氣樣品的采集，分析其主要水溶性離子、部分痕量金屬元素和低分子量有機(jī)酸的濃度水平，探討其分布和來源情況，主要研究結(jié)果如下： （1）在黃渤海海域春季和秋季調(diào)查航次采集的大氣總懸浮顆粒物（TotalSuspended Particulates，TSP）的質(zhì)量分別為（0.18±0.04）g和（0.05±0.03）g，其中主要水溶性離子的總濃度分別為（23.3±10.7）μg·m-3和（27.1±9.4）μg·m-3，二次離子濃度比例最大，分別為84.7%和63.7%。各離子平均濃度大小順序是NO3- nss-SO42- NH4+ Cl- Na+ nss-K+ nss-Ca2+ Mg2+；秋季為NO3-nss-SO42- NH4+ Cl- Na+ nss-K+ nss-Ca2+ Mg2+。秋季痕量金屬離子濃度整體略高于春季，在所有金屬離子中Al和Fe濃度水平最高，表現(xiàn)為：春季，F(xiàn)eAlZnPbV CuCd；秋季，F(xiàn)eAlZnPbCuVCd。黃渤海春季大氣氣溶膠中甲基磺酸（methanesulfonic acid，MSA）濃度平均值為（22.0±18.2）ng·m-3，秋季黃渤海平均值為（11.4±9.6）ng·m-3。CH3COOH和HCOOH秋季濃度水平較高，分別為（472.5±147.3）ng·m-3和（264.2±131.0）ng·m-3，春季CH3COOH和HCOOH平均濃度水平分別為（74.9±47.2）ng·m-3、（55.6±39.5）ng·m-3。 （2）在東海夏季航次采集的TSP質(zhì)量為（0.012±0.003）g，水溶性離子總濃度為（12.3±3.1）μg·m-3，，其中海鹽離子的濃度較大，各離子平均濃度由大到小為Cl- Na+ NO3- nss-SO42- NH4+ Mg2+ nss-K+ nss-Ca2+，二次離子在水溶性離子中的比例為49.2%；秋季TSP的質(zhì)量為（0.020±0.013）g，水溶性離子總濃度為（21.3±8.2）μg·m-3，各離子大小順序?yàn)镃l- Na+ nss-SO42- NO3-NH4+ Mg2+ nss-K+ nss-Ca2+，二次離子占離子濃度的40.3%。東海冬季采樣航次水溶性離子濃度水平最高，平均濃度為（40.9±13.2）μg·m-3，二次離子所占比例也最高，67%，各離子大小順序nss-SO42- Cl- NH4+ NO3- Na+ Mg2+nss-K+ nss-Ca2+。東海航次中痕量金屬元素濃度水平低于黃渤海，夏季各金屬元素平均濃度大小為FeAlZn Pb V CuCd，秋季為FeAl Zn Pb Cu VCd。東海航次有機(jī)酸的濃度低于黃渤海，其中MSA秋季濃度最高，夏季次之，冬季最低，平均濃度依次為（5.8±1.5）、（5.0±3.1）、（1.9±0.3）ng·m-3。夏季航次CH3COOH和HCOOH平均值為（43.6±37.0）、（16.0±9.1）ng·m-3；秋季濃度水平相當(dāng)，分別為（50.8±45.0）、（66.8±56.2）ng·m-3。 （3）總水溶性離子對(duì)TSP質(zhì)量的貢獻(xiàn)表現(xiàn)為夏季最高，秋季次之，春季最低。二次離子NH4+、nss-SO42-和NO3-相對(duì)于地殼源的富集因子非常大，且三者相關(guān)性顯著，主要來自人為源，Mg2+主要來自海洋源，K+和Ca2+主要受地殼源控制；在富集因子基礎(chǔ)上分別估算人為源和地殼源對(duì)痕量金屬元素的貢獻(xiàn)率，結(jié)果表明近岸黃渤海中人為源對(duì)金屬元素的貢獻(xiàn)要普遍高于東海，人為源對(duì)Cd、Zn和Pb的貢獻(xiàn)最大，而Fe和V源于自然和人為源的共同貢獻(xiàn)。 （4）依據(jù)nss-SO42-/MSA的質(zhì)量比值計(jì)算生源硫酸鹽（SO42-bio）對(duì)nss-SO42-的貢獻(xiàn)率，得到結(jié)果為：黃渤海春季和秋季SO42-bio對(duì)nss-SO42-的貢獻(xiàn)率比較接近，分別為5.5%和5.6%，東海夏季、秋季和冬季航次SO42-bio對(duì)nss-SO42-的貢獻(xiàn)率分別是2.2%、2.8%和0.8%。春季生源硫酸鹽比例較高，但整體來看中國東部近海海域大氣氣溶膠的組成和其濃度分布明顯受到人為活動(dòng)輸入的影響。
[Abstract]:The main chemical compositions and sources of atmospheric aerosols in the continental shelf sea of Eastern China are very complex due to the combined effects of land and ocean terrain. Not only can the atmospheric aerosols affect the atmospheric radiation balance through direct and indirect radiation, but also affect the global environment. Atmospheric samples were collected in the Yellow Sea and Bohai Sea in the autumn and autumn of 2011, winter, summer and autumn of 2012. Concentrations of major water-soluble ions, some trace metal elements and low molecular weight organic acids were analyzed, and their distribution and sources were discussed.
(1) Total Suspended Particulates (TSP) in the Yellow Sea and Bohai Sea in spring and autumn were (0.18.04) g and (0.05.03) g, respectively. The total concentrations of major water-soluble ions were (23.3 (10.7) UG The average concentrations of the ions were NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, and NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+. The concentrations of trace metal ions in autumn were slightly higher than those in spring, and the concentrations of Al and Fe were the highest among all the metal ions, namely, in spring, Fe Al-ZnPbV-Cud, and in autumn, F-ZnPbV-Cd. EAlZnPbCuVCd. The mean concentrations of methanesulfonic acid (MSA) in the atmospheric aerosols of the Yellow Sea and Bohai Sea in spring were (22.0 6550 The bisection is (74.9 + 47.2) ng? M-3, (55.6 + 39.5) ng? M-3.
(2) The mass of TSP collected during the East China Sea summer voyage was (0.012.003) g and the total concentration of water-soluble ions was (12.3 The total concentration of water-soluble ions was (21.3 6550 The concentrations of trace metals in the East China Sea voyages were lower than those in the Yellow and Bohai Seas. The average concentrations of metals in summer were FeAlZn Pb V CuCd and in autumn were FeAl Zn Pb Cu VCd. The concentrations of organic acids in the East China Sea voyages were lower than those in the Yellow and Bohai Seas, and the concentrations of MSA in autumn were the highest. The average concentrations of CH3COOH and HCOOH in summer voyages were (43.6+37.0), (16.0+9.1) ng.m-3 and (50.8+45.0), (66.8+56.2) ng.m-3, respectively.
(3) The contribution of total water-soluble ions to TSP quality is the highest in summer, the second in autumn, and the lowest in spring. The enrichment factors of secondary ions NH4 +, nss-SO42 - and NO3 - are very large relative to crustal sources, and their correlation is significant, mainly from human sources, Mg2+ mainly from marine sources, and K + and Ca2+ mainly from crustal sources. The contributions of anthropogenic sources and crustal sources to trace metal elements are estimated respectively. The results show that the contribution of anthropogenic sources to metal elements is generally higher in the Yellow Sea and Bohai Sea than in the East China Sea. The contribution of anthropogenic sources to Cd, Zn and Pb is the greatest, while that of Fe and V is the joint contribution of natural and human sources.
(4) According to the mass ratio of nss-SO42-/MSA, the contribution rates of SO42-bio to nss-SO42-were calculated. The results showed that the contribution rates of SO42-bio to nss-SO42-in spring and autumn were close to 5.5% and 5.6%, respectively. The contribution rates of SO42-bio to nss-SO42-in summer, autumn and winter were 2.2%, 2.8% and 0.8% respectively. Source sulphates are relatively high, but the composition and concentration distribution of atmospheric aerosols in the coastal waters of Eastern China are obviously affected by anthropogenic input.
【學(xué)位授予單位】：中國海洋大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2014
【分類號(hào)】：P732;X513
本文編號(hào)：2248280
[Abstract]:The main chemical compositions and sources of atmospheric aerosols in the continental shelf sea of Eastern China are very complex due to the combined effects of land and ocean terrain. Not only can the atmospheric aerosols affect the atmospheric radiation balance through direct and indirect radiation, but also affect the global environment. Atmospheric samples were collected in the Yellow Sea and Bohai Sea in the autumn and autumn of 2011, winter, summer and autumn of 2012. Concentrations of major water-soluble ions, some trace metal elements and low molecular weight organic acids were analyzed, and their distribution and sources were discussed.
(1) Total Suspended Particulates (TSP) in the Yellow Sea and Bohai Sea in spring and autumn were (0.18.04) g and (0.05.03) g, respectively. The total concentrations of major water-soluble ions were (23.3 (10.7) UG The average concentrations of the ions were NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+, and NO3-nss-SO42-NH4+Cl-Na+nss-K+nss-Ca2+Mg2+. The concentrations of trace metal ions in autumn were slightly higher than those in spring, and the concentrations of Al and Fe were the highest among all the metal ions, namely, in spring, Fe Al-ZnPbV-Cud, and in autumn, F-ZnPbV-Cd. EAlZnPbCuVCd. The mean concentrations of methanesulfonic acid (MSA) in the atmospheric aerosols of the Yellow Sea and Bohai Sea in spring were (22.0 6550 The bisection is (74.9 + 47.2) ng? M-3, (55.6 + 39.5) ng? M-3.
(2) The mass of TSP collected during the East China Sea summer voyage was (0.012.003) g and the total concentration of water-soluble ions was (12.3 The total concentration of water-soluble ions was (21.3 6550 The concentrations of trace metals in the East China Sea voyages were lower than those in the Yellow and Bohai Seas. The average concentrations of metals in summer were FeAlZn Pb V CuCd and in autumn were FeAl Zn Pb Cu VCd. The concentrations of organic acids in the East China Sea voyages were lower than those in the Yellow and Bohai Seas, and the concentrations of MSA in autumn were the highest. The average concentrations of CH3COOH and HCOOH in summer voyages were (43.6+37.0), (16.0+9.1) ng.m-3 and (50.8+45.0), (66.8+56.2) ng.m-3, respectively.
(3) The contribution of total water-soluble ions to TSP quality is the highest in summer, the second in autumn, and the lowest in spring. The enrichment factors of secondary ions NH4 +, nss-SO42 - and NO3 - are very large relative to crustal sources, and their correlation is significant, mainly from human sources, Mg2+ mainly from marine sources, and K + and Ca2+ mainly from crustal sources. The contributions of anthropogenic sources and crustal sources to trace metal elements are estimated respectively. The results show that the contribution of anthropogenic sources to metal elements is generally higher in the Yellow Sea and Bohai Sea than in the East China Sea. The contribution of anthropogenic sources to Cd, Zn and Pb is the greatest, while that of Fe and V is the joint contribution of natural and human sources.
(4) According to the mass ratio of nss-SO42-/MSA, the contribution rates of SO42-bio to nss-SO42-were calculated. The results showed that the contribution rates of SO42-bio to nss-SO42-in spring and autumn were close to 5.5% and 5.6%, respectively. The contribution rates of SO42-bio to nss-SO42-in summer, autumn and winter were 2.2%, 2.8% and 0.8% respectively. Source sulphates are relatively high, but the composition and concentration distribution of atmospheric aerosols in the coastal waters of Eastern China are obviously affected by anthropogenic input.
【學(xué)位授予單位】：中國海洋大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2014
【分類號(hào)】：P732;X513
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