大气中甲磺酸的含量分析及其对酸雨的贡献
摘要
本课题来源于“近海海洋综合调查与评价专项”,简称国家908专项与“近海海洋综合调查与评价专项”,简称山东省908专项。于2006年夏季(7月18日-8月7日)和冬季(06年12月31日- 07年1月17日)对我国北黄海近海进行调查,2006年夏季(8月14日-23日)和冬季(06年12月17日-25日)对山东近海(日照-威海)进行调查,采集了大气颗粒物样品和雨水样品(雨水仅在夏季的北黄海航次采集),测定了大气颗粒物中总悬浮颗粒物的浓度及阳离子Na+、NH4+、K+、Mg2+和Ca2+及阴离子甲磺酸(MSA)、NO2-、SO42-、NO3-、PO43-的浓度和雨水中MSA的浓度,分析并讨论了它们的分布及季节变化。
此外,还于2006年5月-12月对中国海洋大学(鱼山校区)八关山气象观测站采集了大气颗粒物样品,测定了MSA的浓度,分析并讨论了其时间分布特征。主要研究结论如下:
(1)在文献基础上改进并完善了MSA的分析方法与区域,进行了滤膜样品提取率的研究,发现在超声波振荡时长40min时,样品提取率非常理想(100%-102%)。并且确定了利用ICS-1000离子色谱仪对阳离子Na+、NH4+、K+、Mg2+和Ca2+及阴离子MSA、NO2-、SO42-、NO3-和PO43-分别同时测定的时间长度。
(2)经过分析比较,发现山东近海和北黄海大气颗粒物浓度,都符合国家标准环境空气质量一类地区的一级标准,海域空气质量优良。但是,实际上颗粒物仅仅是评价环境的重要指标之一(还有雨水的状况等参考指标)。无论是山东近海还是北黄海,冬季近海大气颗粒物浓度比夏季要高,这与夏季降水量和次数比冬季大或多有直接关系,还有风力因素影响。黄海近海(包括山东近海和北黄海近海)大气受陆地污染源程度的影响较大。
(3)从5月到12月,这六个月青岛大气颗粒物浓度一直是在增大,这是由于风力的作用,使得陆地的大气颗粒物搬运到青岛近海的量也是随月份增大。这个规律和山东近海以及北黄海相似(颗粒物浓度夏季低于冬季)。青岛的大气颗粒物量符合国家标准环境空气质量二类地区的二级标准,即居住区(文化区)的标准,非常适合居住。
(4)综合北黄海和山东近海分析结果,发现颗粒物中MSA浓度都是夏高冬低,非常符合温度和光强越大或强MSA也随着增大的规律,与文献相符合。这主要是由于夏季DMS浓度高(北黄海夏季DMS远远高于冬季),从而使得其被氧化的产物MSA也是夏季浓度高。利用MSA进行估算DMS对nss-SO42-的贡献量,发现北黄海夏季大气中的DMS对nss-SO42-的贡献量夏季远高于冬季。
(5)青岛大气MSA浓度的月变化情况是先高,7月份达到最大值,再低,12月份到达最低值。即夏季的7月份最高,而春秋的5、6和10月份较低,冬季的11月份和12月份最低。
(6)通过对青岛雨水进行采样测定分析,发现MSA对雨水的总离子贡献量较大,为0.89%。可能与DMS的海洋释放量很大有关(夏季黄海DMS的浓度约为300ng/m3,而冬季约为90ng/m3)。MSA和nss-SO42-对雨水的总贡献量也较大,为48.18%。青岛雨水MSA浓度为0.130μg/m3,北黄海雨水中MSA浓度为0.132mg/L。比较得到北黄海大气颗粒物对雨水贡献率比青岛的相应值低,绝对贡献量却是相差不大的结论。
(7)青岛酸雨仍然是一个很严峻的问题,需要相关部门引起高度重视,应该重视治理环境问题,加大降低环境污染的措施力度,以期青岛的环境能够更好更美。
(8)从青岛检测结果来比较,雨水中离子的海盐贡献率随时间有共同的规律性变化,都是夏季的7、8月份左右达到最大贡献率,前和后都是较低。这可能是由于风力作用,夏季海洋对沿海大气贡献较大量的海洋元素,从而使得降水中7、8月份的海盐贡献率较高。
综上所述,本论文对山东近海夏季和冬季以及北黄海夏季和冬季四个航次大气颗粒物MSA等多种离子浓度、青岛大气颗粒物及雨水中MSA等多种离子的分布进行了较为全面、客观的分析讨论;对所测环境进行了科学的评价;并结合温度、风力等气象因素对颗粒物及MSA的季节(时间)变化进行规律性总结。本论文为全球硫循环、酸雨监测及环境监测提供了初步的科学依据。
Two cruises were carried out in the North Yellow Sea during summer (July 18～August 7, 2006) and winter (December 31, 2006～January 17, 2007) and two cruises were carried out in Shandong coastal sea during summer (August 14～23, 2006) and winter (December 17～25, 2006) to determine the content of methanesulfonic acid (MSA) in the atmosphere and its contribution to acid rain. The main conclusions are obtained as follows:
1) Analysis method about MSA is improved on the basis of literature. Extraction percentage of MSA in the filters containing samples ranged from 100 % to 102 %.The time of measurements of positive ions (Na+, NH4+, K+, Mg2+ and Ca2+ ) and negative ions ( MSA, NO2-, SO42-, NO3- and PO43- ) are ascertained by ICS-1000.
2) Concentration of Total Suspended Particulate(TSP) conforms to the first area and the first order standard of the State Ambient Air Quality Standard. The air quality on the sea is good. The concentration of TSP is only one aspect of Environmental Assessments. Concentrations of TSP whether in atmosphere of Shandong coastal Sea or North Yellow Sea are higher in winter than in summer, because it has more rainfall in summer than in winter. The atmosphere on the Yellow Sea (including Shandong coastal sea and the North Yellow Sea) is largely dependent on the extent of the contamination source on the land.
3) Concentrations of TSP in the atmosphere increase gradually from May to December, which is due to the effect of wind. Wind makes the TSP move from the inland to Qingdao coastal sea, as well as its concentration increases by month. This law is similar to the north Yellow Sea and Shandong coastal sea. Concentration of TSP conforms to the State Ambient Air Quality Standard of the second-rate area and the second-class standard. Therefore, Qingdao is a place fit for human habitation.
4) The results about the North Yellow Sea and Shandong coastal sea indicate that concentrations of MSA in TSP are high in summer and low in winter, in correlation with the temperature and light intensity, in correspondence with the literature. This is mainly due to higher concentrations of DMS in summer (DMS of Yellow Sea is higher in summer than in winter) than in winter. MSA is one oxidation product of DMS. MSA is used to estimate the contribution of nss-SO42-. We find that the contribution of DMS in the atmosphere to the nss-SO42- on the North Yellow Sea is far higher in summer than in winter.
5) Concentrations of MSA in Qingdao atmosphere is the highest in summer ( July), lower in the Spring and Autumn (May, June and October), and the lowest in winter (November and December).
6) By sampling Qingdao rain water, we can find that MSA contributes to total ions in the rain can not be ignored, the contribution rate is about 0.89%. This is likely related to the release of ocean. The contribution of MSA and nss-SO42- to the rainwater are about 48.18%.The mean concentration of MSA in Qingdao rainwater is 0.130 mg/L. The concentration of MSA in the rainwater of North Yellow Sea is 0.132 mg/L. The contribution rate is obviously lower in Qingdao rainwater than in North Yellow Sea rainwater. Absolute contribution amount is in the same level in Qingdao as in North Yellow Sea.
7) Qingdao acid rain is still a serious problem which needs to cause great attention by the relevant administration departments. Focused on environmental issues, we expect a better and more beautiful environment in Qingdao.
8) From the results of Qingdao rainwater, we find that the contribution of sea salt to the ions of rainwater has the same law with the time. The contribution rate is the highest in July and August. It is likely duo to the wind force, the ocean contributes more marine elements to the atmosphere on the coastal sea in summer, so the sea salt contribution rate is high in rainwater.
In short, through four cruises in summer and winter in Shandong coastal sea and North Yellow Sea, TSP, rainwater and MSA concentrations are objectively analyzed. The environment is scientifically evaluated. The relation between MSA, temperature and weather is summarized. This paper offers fundamental evidence on scientific research of global sulfur cycle, acid rain monitoring and environmental monitoring.
此外,还于2006年5月-12月对中国海洋大学(鱼山校区)八关山气象观测站采集了大气颗粒物样品,测定了MSA的浓度,分析并讨论了其时间分布特征。主要研究结论如下:
(1)在文献基础上改进并完善了MSA的分析方法与区域,进行了滤膜样品提取率的研究,发现在超声波振荡时长40min时,样品提取率非常理想(100%-102%)。并且确定了利用ICS-1000离子色谱仪对阳离子Na+、NH4+、K+、Mg2+和Ca2+及阴离子MSA、NO2-、SO42-、NO3-和PO43-分别同时测定的时间长度。
(2)经过分析比较,发现山东近海和北黄海大气颗粒物浓度,都符合国家标准环境空气质量一类地区的一级标准,海域空气质量优良。但是,实际上颗粒物仅仅是评价环境的重要指标之一(还有雨水的状况等参考指标)。无论是山东近海还是北黄海,冬季近海大气颗粒物浓度比夏季要高,这与夏季降水量和次数比冬季大或多有直接关系,还有风力因素影响。黄海近海(包括山东近海和北黄海近海)大气受陆地污染源程度的影响较大。
(3)从5月到12月,这六个月青岛大气颗粒物浓度一直是在增大,这是由于风力的作用,使得陆地的大气颗粒物搬运到青岛近海的量也是随月份增大。这个规律和山东近海以及北黄海相似(颗粒物浓度夏季低于冬季)。青岛的大气颗粒物量符合国家标准环境空气质量二类地区的二级标准,即居住区(文化区)的标准,非常适合居住。
(4)综合北黄海和山东近海分析结果,发现颗粒物中MSA浓度都是夏高冬低,非常符合温度和光强越大或强MSA也随着增大的规律,与文献相符合。这主要是由于夏季DMS浓度高(北黄海夏季DMS远远高于冬季),从而使得其被氧化的产物MSA也是夏季浓度高。利用MSA进行估算DMS对nss-SO42-的贡献量,发现北黄海夏季大气中的DMS对nss-SO42-的贡献量夏季远高于冬季。
(5)青岛大气MSA浓度的月变化情况是先高,7月份达到最大值,再低,12月份到达最低值。即夏季的7月份最高,而春秋的5、6和10月份较低,冬季的11月份和12月份最低。
(6)通过对青岛雨水进行采样测定分析,发现MSA对雨水的总离子贡献量较大,为0.89%。可能与DMS的海洋释放量很大有关(夏季黄海DMS的浓度约为300ng/m3,而冬季约为90ng/m3)。MSA和nss-SO42-对雨水的总贡献量也较大,为48.18%。青岛雨水MSA浓度为0.130μg/m3,北黄海雨水中MSA浓度为0.132mg/L。比较得到北黄海大气颗粒物对雨水贡献率比青岛的相应值低,绝对贡献量却是相差不大的结论。
(7)青岛酸雨仍然是一个很严峻的问题,需要相关部门引起高度重视,应该重视治理环境问题,加大降低环境污染的措施力度,以期青岛的环境能够更好更美。
(8)从青岛检测结果来比较,雨水中离子的海盐贡献率随时间有共同的规律性变化,都是夏季的7、8月份左右达到最大贡献率,前和后都是较低。这可能是由于风力作用,夏季海洋对沿海大气贡献较大量的海洋元素,从而使得降水中7、8月份的海盐贡献率较高。
综上所述,本论文对山东近海夏季和冬季以及北黄海夏季和冬季四个航次大气颗粒物MSA等多种离子浓度、青岛大气颗粒物及雨水中MSA等多种离子的分布进行了较为全面、客观的分析讨论;对所测环境进行了科学的评价;并结合温度、风力等气象因素对颗粒物及MSA的季节(时间)变化进行规律性总结。本论文为全球硫循环、酸雨监测及环境监测提供了初步的科学依据。
Two cruises were carried out in the North Yellow Sea during summer (July 18～August 7, 2006) and winter (December 31, 2006～January 17, 2007) and two cruises were carried out in Shandong coastal sea during summer (August 14～23, 2006) and winter (December 17～25, 2006) to determine the content of methanesulfonic acid (MSA) in the atmosphere and its contribution to acid rain. The main conclusions are obtained as follows:
1) Analysis method about MSA is improved on the basis of literature. Extraction percentage of MSA in the filters containing samples ranged from 100 % to 102 %.The time of measurements of positive ions (Na+, NH4+, K+, Mg2+ and Ca2+ ) and negative ions ( MSA, NO2-, SO42-, NO3- and PO43- ) are ascertained by ICS-1000.
2) Concentration of Total Suspended Particulate(TSP) conforms to the first area and the first order standard of the State Ambient Air Quality Standard. The air quality on the sea is good. The concentration of TSP is only one aspect of Environmental Assessments. Concentrations of TSP whether in atmosphere of Shandong coastal Sea or North Yellow Sea are higher in winter than in summer, because it has more rainfall in summer than in winter. The atmosphere on the Yellow Sea (including Shandong coastal sea and the North Yellow Sea) is largely dependent on the extent of the contamination source on the land.
3) Concentrations of TSP in the atmosphere increase gradually from May to December, which is due to the effect of wind. Wind makes the TSP move from the inland to Qingdao coastal sea, as well as its concentration increases by month. This law is similar to the north Yellow Sea and Shandong coastal sea. Concentration of TSP conforms to the State Ambient Air Quality Standard of the second-rate area and the second-class standard. Therefore, Qingdao is a place fit for human habitation.
4) The results about the North Yellow Sea and Shandong coastal sea indicate that concentrations of MSA in TSP are high in summer and low in winter, in correlation with the temperature and light intensity, in correspondence with the literature. This is mainly due to higher concentrations of DMS in summer (DMS of Yellow Sea is higher in summer than in winter) than in winter. MSA is one oxidation product of DMS. MSA is used to estimate the contribution of nss-SO42-. We find that the contribution of DMS in the atmosphere to the nss-SO42- on the North Yellow Sea is far higher in summer than in winter.
5) Concentrations of MSA in Qingdao atmosphere is the highest in summer ( July), lower in the Spring and Autumn (May, June and October), and the lowest in winter (November and December).
6) By sampling Qingdao rain water, we can find that MSA contributes to total ions in the rain can not be ignored, the contribution rate is about 0.89%. This is likely related to the release of ocean. The contribution of MSA and nss-SO42- to the rainwater are about 48.18%.The mean concentration of MSA in Qingdao rainwater is 0.130 mg/L. The concentration of MSA in the rainwater of North Yellow Sea is 0.132 mg/L. The contribution rate is obviously lower in Qingdao rainwater than in North Yellow Sea rainwater. Absolute contribution amount is in the same level in Qingdao as in North Yellow Sea.
7) Qingdao acid rain is still a serious problem which needs to cause great attention by the relevant administration departments. Focused on environmental issues, we expect a better and more beautiful environment in Qingdao.
8) From the results of Qingdao rainwater, we find that the contribution of sea salt to the ions of rainwater has the same law with the time. The contribution rate is the highest in July and August. It is likely duo to the wind force, the ocean contributes more marine elements to the atmosphere on the coastal sea in summer, so the sea salt contribution rate is high in rainwater.
In short, through four cruises in summer and winter in Shandong coastal sea and North Yellow Sea, TSP, rainwater and MSA concentrations are objectively analyzed. The environment is scientifically evaluated. The relation between MSA, temperature and weather is summarized. This paper offers fundamental evidence on scientific research of global sulfur cycle, acid rain monitoring and environmental monitoring.
引文
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