汞在水旱轮作系统的释放特征及其影响因素
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摘要
由于汞具有多种形态、易挥发和长距离传输等独特的物理性质，因而被公认为“全球性污染物”而引起人们的高度重视。特别是近年来发现，随着化石燃料燃烧、金属冶炼等人为过程向大气释放的汞逐渐增加，全球大气汞浓度逐年升高。大气环境中汞的存在形式主要有单质汞、二价汞及其化合物、甲基汞和颗粒态结合汞，其中元素汞(Hg~0)是主要形态，占总气汞含量的90％以上。元素汞在大气中停留时间约为0.5～2年，可进行长距离传输，参与全球的汞循环，造成全球范围内的汞污染。为此，近年来对汞污染问题的研究热点，已从对局部区域环境的污染与危害问题转向全球大气汞循环演化规律方面。而对这一问题认识的关键，首先必须正确地找出向大气释放汞的源头并正确测算其释放量。
近年对火山排气作用、地热活动、森林火灾、土壤表面释放、自然水体的排放、植物表面蒸腾作用、城市地表等自然释汞过程作了一些研究，为从宏观尺度估算当今全球地表每年向大气释放汞的总量提供了借鉴。但从时间尺度与区域规模上看，还极其有限，从而造成目前对全球地表向大气释放汞总量的估算还存在很大误差和不确定性。因此，进一步开展具有代表性的地表自然体汞释放通量的研究，对正确估算全球自然释放源向大气的排汞量和认识全球大气汞循环演化规律具有重要意义。
水旱轮作是亚洲各国普遍采用的稻田耕作制度，也是我国南方主要的耕作制之一。我国有水旱轮作稻田超过1400万hm~2，占稻田面积的30％～40％。水旱轮作系统由于水热条件及氧化还原条件的强烈变化，直接影响到土壤中汞的转化、迁移和积累。但对这一过程的系统研究相对缺乏，为此，本项研究以我国最具特色的周期性干湿交替环境——水旱轮作稻田为研究对象，开展干湿交替环境条件下土壤汞的释放通量及其迁移形态的研究，对正确认识区域及全球大气汞的来源及强度无疑具有重要意义。
本研究采用野外实地监测、采样分析及模拟试验的方法进行。实地监测及采样地点位于重庆北碚西南大学国家紫色土肥力与肥料效益监测试验基地的水早轮作试验地。试验地土壤为侏罗纪沙溪庙组紫色泥、页岩发育而成的紫色土(普通紫色常湿雏形土，Purpli-Udic Cambosols)，试验区面积共1200m~2，共设12个不同施肥组合的稻-麦轮作小区处理(其中1个为稻-油轮作)和1个长期休闲处理。自2005年4月至2006年12月，按水稻生长期、休闲期和油／麦生长期划分监测周期，现场测定汞释放通量，每月监测次数不少于3次，每次连续测定0.5～8h不等，同时测定光照强度、气温、大气湿度、土温和水温等参数。每月进行一次采样分析(包括土样、水样)，分析项目包括土壤基本性质(有机质、机械组成、pH、COD)、汞含量、汞形态、土壤微生物类群等指标。土／水-气界面汞交换通量采用动力通量箱与Lumex~(?) RA-915~+测汞仪联用技术监测，土壤汞形态参照Tessier(1979)的方法测定。同时，参照水旱轮作土壤干湿交替的环境条件进行室内模拟试验，以进一步研究其动态变化特征。通过数据分析整理，确定稻田土壤在干湿交替环境下向大气释放汞的通量。并研究不同施肥状况、不同季节、轮作的不同时期及其作物(油菜、小麦／水稻)条件下环境界面(水／土-气)汞的释放通量变化特征，研究了气象因子、土壤性质以及微生物类群对汞释放通量的影响，在此基础上对重庆市水-旱轮作农田汞的自然源释放进行初步量化。研究结果如下：
水旱轮作稻田土壤汞含量及汞的形态分布均随轮作期水旱交替过程而呈现周期性变化，表现为旱地土壤总汞含量高于水田土壤，汞形态以王水溶态为主，活性较低；水田土壤以可溶态汞为主，活性较高。这一变化过程的根本原因是由水早轮作方式导致的农田土壤氧化还原条件的周期性变化，汞的形态及活性的变化，必然影响到其在体系内的循环与转化过程。模拟试验显示，土壤汞含量越高，上覆水的汞浓度越大。淹水期间上覆水的汞浓度有两个较高点，第一个峰值出现在第3天，第二个峰值出现在第12天左右。土壤经过淹水—落干交替过程后，部分汞被散发到大气中，这部分汞主要是酸溶态和碱溶态汞经生物或非生物还原过程，以Hg~0的形式释放。淹水期间上覆水DGM和Hg~(2+)含量的变化趋势相反，说明它们之间在一定条件下可以相互转化。模拟试验中对汞通量的监测表明，二价汞(Hg~(2+))比其它价态的汞更容易在土壤-水体-大气界面中转化和交换。
试验区汞释放通量数据高于世界背景区域1个数量级，表明水旱轮作系统也是大气汞的一个重要的自然释放源。在水旱轮作期内，水稻生长期稻田水．气界面汞交换通量最大(82.94±73.3ng m~(-2) h~(-1))，休闲期土-气界面汞交换通量次之(24.0±17.1ngm~(-2)h~(-1))，油／麦生长期土-气界面汞交换通量最小(11.04±3.5ng m~(-2) h~(-1))。年平均汞通量为39.34±53.2ng m~(-2) h~(-1)。
紫色土农田水／土-气界面间的汞通量表现出明显的日变化、期间变化和季节性变化。不同轮作期不同界面间的汞挥发通量存在较大差异，其大小顺序为，暖季稻田＞暖季空地＞暖季油麦田＞冷季油麦田。白天水／土-气界面汞通量都呈现早晚低，午间高的趋势，沉降多出现在傍晚和早晨。水旱轮作稻田基质总汞含量与其释放量之间存在正相关关系(水体，r=0.463~*，p＜0.05；土壤，r=0.322~*，p＜0.05)。土壤有机质含量与汞通量之间存在极显著的负相关关系(r=-0.688~(**)，p＜0.01)。气象因子对界面汞交换的影响极其显著，水-旱轮作期间旱地土壤和稻田水体表面的汞挥发通量与太阳辐射量表现出相同的变化趋势，两者之间呈极显著的正相关(r=0.730~(**)，p＜0.01)。旱地土壤表面(2～5cm)温度、水体表层温度与汞通量呈极显著(r=0.514~(**)，p＜0.01)和显著(r=0.171~*，p＜0.05)正相关。经Arrhenius方程计算得出，农田早地土壤产生气态单质汞的化学反应活化能为21.5kcal mol~(-1)(19.5～33.4℃)，水田土壤为27.7 kcal mol~(-1)(4.5～34.3℃)。其化学反应活化能高于单质汞的蒸发焓，说明汞在水／土表面释放不是单质汞的直接蒸发。相对于土-气界面来说水-气界面汞交换更为复杂，水面汞释放应该看作是水体和大气亚表层发生的各种物理化学反应由此产生的拮抗或协同作用下的最终结果。空气相对湿度在水稻生长期与汞通量的关系不明显，而在油／麦生长期和休闲期，相对湿度与汞通量存在极显著的负相关关系(r=-0.748~(**)，-0.730~(**)，p＜0.01)。土壤湿度与汞通量在一定程度上有一致的变化趋势，但在监测期内对水旱轮作条件下紫色土汞的释放影响甚微。
耕作方式对汞释放的影响也较显著。不同试验小区的汞通量受施肥条件和地表覆盖物的影响很大，施肥状况影响作物生长量和作物密度，也影响到土壤性质、性状和土壤中汞形态及其相互转化，从而影响汞的固定和释放。但施肥条件对水体汞挥发的影响并不明显。
在水稻生长期，稻田土壤中的厌氧细菌群落数量与汞释放通量呈相反趋势(r=-0.580~*，p＜0.05)，其中硫酸盐还原菌(SRB)和厌氧纤维素分解菌(ACDB)与汞通量有显著负相关关系(r=-0.630~*，-0.558~*，p＜0.05)，是影响汞形态转化和释放的主要类群。而在休闲期及油／麦生长期，微生物群落数与汞通量之间不存在明显的相关性。这说明旱地土壤汞的释放，主要由其他环境因素(如气象因子)决定，而在厌氧环境下，细菌对水田土壤汞的释放起着重要作用。
基于通量箱法实地测得的数据，并结合重庆市的气候特点，对该地区水旱轮作农田汞释放量进行初步估算，重庆市每年从水-旱轮作农田释放到大气中的总汞量为565kg。
As a global pollutant, mercury is receiving intensive scrutiny due to its special physical characteristics. It occurs in various physical and chemical forms, likely volatilization and long range transportation in the environment. In recent years, the concentration of mercury is increasing in the atmosphere due to the elevated emission of anthropogenic activities, such as combustion of fossil fuels, roasting and smelting of ores etc. Most of atmospheric Hg in ambient air, above 90%, is made up of elemental mercury (Hg~0), while the remainders are divalent Hg compounds, either in the gaseous phase or bound to particles, and methylmercury. The Hg~0 (g) has a relatively long residence time of 0.5～2 years in the atmosphere, and which can transportation for a long distance along the global atmosphere cycling and to pose a global pollution. Researches of mercury pollution associated with human health risk had been considerable concerned in past years. In recent years, the hotspot issues of mercury pollution were mostly turned to the aspect of understanding the laws of mercury cycling and transformation in the atmosphere on global scale. So, it is important to discern the resources of mercury emission and measure or estimate the amounts correctly of mercury exchange.
The atmospheric loading of mercury is come from natural and anthropogenic sources. Emission inventories indicate that the contribution of mercury emission from natural sources is about 50% within the total amount of emission from global surface. Many researches involve to mercury emission from environmental surface in recent years, which include evasion from active volcano, earth heat-radiating, forest-fire, soil/water surface, transpiration from foliage of vegetation and urban surface etc, have provided lots of references to assessment of annual inventories of atmospheric mercury budget on global scale. However, there are some drawbacks with error and uncertainty in these estimations due to the restriction of limited spatial-temporal scale. Average inventories of mercury emission from natural sources has been estimated ranges between 2500 and 19325 t yr~(-1), and the contribution from anthropogenic sources ranges between 910 and 110001 yr~(-1). Researches on biogeochemical cycle of mercury in recent years were mostly focused on assessment of mercury release flux on environment surface, and an average rate of Hg evasion, 1.5 ng m~(-2)h~(-1), was taken to be the normal standard rate. Nevertheless, the field studies lately exhibited that the foregoing rate would lead to lower estimate the contribution from natural sources of mercury emission. Therefore, it is important to distinguish and determine the characteristics of various natural surfaces, and that is for the purpose of improvement estimation of mercury budget exactly and fully understanding global biogeochemical cycling of mercury.
At present, for study mercury emission from natural sources, dynamic flux chamber (DFC) technique has been adopted widely, which was first used by Schroeder et al. (1989) and Xiao et al. (1991) for measurement mercury exchange flux over different environmental interfaces (e.g. soil/water-air). Through the studies for last decade, people have realized preliminarily many important aspects of mercury exchange flux from various natural surfaces, but there are scarcely reports that involved with the mercury exchange characteristics in the interfaces of periodicity dry-wet alternating environment (e.g. water level fluctuating zone of reservoir, paddy-upland rotation farm land). Especially, there are lack of informations about the aspect of the seasonal varies characteristics of mercury release and climatic influencing factors in the special environment.
Paddy-upland rotation is a farming tradition that wildly adopted by Asian countries and it also used as a main culture manner in south China. The area of paddy-upland rotation farmland covered above 1400 millions hm~2 in China and it consists of 30～40% of the rice-land resources. Paddy-upland rotation system has an intrinsic peculiar characteristic that the conditions of thermal energy and oxidation- deoxidization change heavily along the periodic varying of season, and this may lead to an evident influence in the course of mercury transformation, transport and accumulation in soil. Because of lack of systematic informations measured about this circumstance, the purpose of this paper is to study the characteristics of mercury release fluxes and its chemical forms transformation, in the paddy-upland (dry-wet) rotation system. This research would exhibit an important significance for improvement on farther understanding the regional or global mercury resource and its release intensity.
Here, the study was conducted by both in simulating experiment, laboratory analysis and field investigation in situ. The field investigation site was located at National Purple Soil Fertility and Fertilizer Efficiency Monitored Base (E:106°24'33.3'' N:29°48'36.2"), which situated at Southwest University, Beibei District in Chongqing, China. The research area belongs to the purple hilly land with an elevation of 239 m. The subtropical earth monsoon climate is presented in there. According to statistics, the mean annual temperature is 18.4°C, annual precipitation is 1105.5 mm, and annual duration of sunshine is 1276.7 h. The tested soil was the gray brown purple soil (Purpli-Udic Cambosols), which is a neutral purple soil subtype and developed from the purple mud stone and shale of Saximiao Association of Jurassic Period. It is the most purple soil types, and it occupies about 40% of the area of purple soils and most of the grain base in Chongqing distribute in it. So it is the typical representative of purple soils. The research area covered 1200 m~2 and was ploted out to 13 divisions.
Different chemical form of mercury has different transference activeness in soil, and it can dominate the release flux of theirs, ultimately. Wherefore, this study had analyzed the mercury existence forms and its variety in different farming seasons while in the flooding period (rice growth term), the intermission period and the upland period (wheat/rape growth term), respectively. Besides, the study had studied the characteristics of mercury exchange and distribution between the soil and water interface in rice growth period by means of simulating flooding experiment. The results revealed that, the mercury content and species distribution of paddy-upland rotation soil varying periodically along with the alternating change of farming period, namely dry-wet change by turn. Total mercury content in the upland soil is higher than that of flooding soil. Residual Hg is the predomination species in the upland soil, and it has a lower activity. Contrarily, soluble Hg is the predomination species in the flooding soil and it has a higher activity. The essential reason of this situation is caused by the periodic change of oxidation-deoxidization conditions in farmland. The results of simulating flooding experiment demonstrated that the mercury concentration of water column increased with the increasing content of soil Hg. Mercury concentration in water have two peak values after flooding, the first peak occurred earlier (3~(rd) d), the latter appeared relatively later (about 12~(th) d). After the wet-dry process, partly soil mercury evasion into the air presented as Hg~0, and which is mainly the production of acid-soluble and H_2O-soluble forms Hg deoxidized through biological or abiological transforming course. During flooding period, the concentration fluctuation trend between DGM and Hg~(2+) in water column is reverse, and it implies that they could transform to each other at suitable environmental condition. The data of mercury fluxes measured in the simulating flooding experiment course showed that, the divalent Hg is easier exchange, transformation and finally evaporation to atmosphere than other forms of mercury in the soil-water-air interface.
Mercury fluxes measurement were performed by dynamic flux chamber (DFC) cope with the Lumex~? Multifunctional mercury analyzer RA-915~+during different farming season while in the flooding period (rice growth term), the intermission period and the upland period (wheat/rape growth term) respectively, at all plots in the investigating field. The characteristics of mercury flux in different farming seasons and covered crops were discussed. Simultaneously, mercury flux influencing factors such as meteorological, soil properties, fertilizer management and microbial communities were also discussed. Finally, an annual emission of mercury to the atmosphere from paddy-upland rotation farmland in Chongqing was estimated. The results indicated that, the average value of mercury fluxes in investigated area was higher than that of global background by 1 magnitude. Therefore, the results imply that the paddy-upland rotation system may be an importance resource which is a potentially contributor to the atmospheric mercury content. During whole dry-wet rotation farming seasons, the mean mercury exchange flux at water-air interface in rice land is the highest with the value of 82.9±73.3 ng m~(-2) h~(-1), next to the soil-air interface in intermission period with the value of 24.0±17.1 ng m~(-2) h~(-1), the mean flux of soil-air interface in wheat/rape growth period was the lowest with the value of 11.0±3.5 ng m~(-2) h~(-1). The annual average mercury flux in whole fanning seasons is 39.3±53.2 ng m~(-2) h~(-1).
Mercury fluxes of water/soil-air interfaces from purple soil rotation farmland exhibit a significantly diurnal and seasonal variation. There was evidently difference of fluxes measured from different season and interface, the decreasing order is as follows warm season rice land (water/air), warm season intermission leisure land (soil/air), warm reason rice/wheat land (soil/air) and cold season rice/wheat land (soil/air). Mercury evasion exhibits a strong diurnal cycle variation, with the highest during midday, while lower in the morning and early evening. Mercury fluxes over air/surfaces had bi-directional exchange in the morning and early evening in cold season. Results of statistical analysis showed, there was positive correlation between mercury flux and total Hg content in paddy-upland rotation farmland (water: r=0.463~*, soil: r=0.322~*), on the contrary, there was significantly negative correlation between mercury flux and soil organic matter content (r=-0.688**). Climatic factors had effected evidently to mercury flux in the water/soil-air interfaces. Regression analysis of data measured over water/soil surface indicated that mercury flux appear to be most significantly positive relation to solar radiation (r=0.730~(**)) and soil/water temperature (soil: r= 0.514~(**); water: r = 0.171~*), and significantly negatively correlated with relative humidity over soil surface (r=-0.748~(**)), and weaker correlated with relative humidity over water surface and soil moistness. Analysis of data measured also suggested that exponential correlation of mercury flux with soil/water temperature in some plots (soil: R~2= 0.3047~(**); water: R~2=0.7044~(**)). Arrhenius equation could be applied to explain the link between the kinetics rate constant of this process and the soil/water temperature, so the activation energy (Ea) was then calculated to be 21.5 / 27.7 kcal mol~(-1) from the slope of best fit line. The values were higher than the mercury vaporization heat of 14.5 kcal mol~(-1), implying that the mercury emission from soil /water surface is not the vaporization of elemental mercury alone.
Likewise, results of this research suggested that, farming manner, include crop category, coverage density and fertilizer management, would be an important influencing factor that can effect evidently to mercury flux from the soil/water surface. Especially, the fertilizer management can cause the changes of soil property, microbeial communities and mercury existence form and its transformation. Sequentially, it dominates the course of mercury accumulation and emission in soil.
Moreover, data obtained from microorganism cultivation revealed that, a negatively correlation (r= -0.580~*) between the amount of anaerobic bacterial communities (cfu) in the flooding soil and mercury fluxes over water surface during the rice/rape growth term. Two categories of bacterial populations, sulfate-reducing bacteria (SRB) and anaerobic cellulose-decomposing bacteria (ACDB) , were the dominating populations for influencing mercury release flux during the flooding terms, the correlation coefficients were -0.630~*(SRB) and -0.558~* (ACDB), respectively. Nevertheless, the correlation between bacteria communities and mercury fluxes in upland was insignificant. This means that the mercury flux in upland was dominated by other environmental factors.
Associating with climate characteristics of Chongqing, a preliminary estimation of regional mercury budget was carried out based on the fluxes data of the experimental plots which measured by dynamic flux chamber. The total mercury emission to the atmosphere from dry-wet rotation farm fields was annually about 565 kg in Chongqing.
近年对火山排气作用、地热活动、森林火灾、土壤表面释放、自然水体的排放、植物表面蒸腾作用、城市地表等自然释汞过程作了一些研究，为从宏观尺度估算当今全球地表每年向大气释放汞的总量提供了借鉴。但从时间尺度与区域规模上看，还极其有限，从而造成目前对全球地表向大气释放汞总量的估算还存在很大误差和不确定性。因此，进一步开展具有代表性的地表自然体汞释放通量的研究，对正确估算全球自然释放源向大气的排汞量和认识全球大气汞循环演化规律具有重要意义。
水旱轮作是亚洲各国普遍采用的稻田耕作制度，也是我国南方主要的耕作制之一。我国有水旱轮作稻田超过1400万hm~2，占稻田面积的30％～40％。水旱轮作系统由于水热条件及氧化还原条件的强烈变化，直接影响到土壤中汞的转化、迁移和积累。但对这一过程的系统研究相对缺乏，为此，本项研究以我国最具特色的周期性干湿交替环境——水旱轮作稻田为研究对象，开展干湿交替环境条件下土壤汞的释放通量及其迁移形态的研究，对正确认识区域及全球大气汞的来源及强度无疑具有重要意义。
本研究采用野外实地监测、采样分析及模拟试验的方法进行。实地监测及采样地点位于重庆北碚西南大学国家紫色土肥力与肥料效益监测试验基地的水早轮作试验地。试验地土壤为侏罗纪沙溪庙组紫色泥、页岩发育而成的紫色土(普通紫色常湿雏形土，Purpli-Udic Cambosols)，试验区面积共1200m~2，共设12个不同施肥组合的稻-麦轮作小区处理(其中1个为稻-油轮作)和1个长期休闲处理。自2005年4月至2006年12月，按水稻生长期、休闲期和油／麦生长期划分监测周期，现场测定汞释放通量，每月监测次数不少于3次，每次连续测定0.5～8h不等，同时测定光照强度、气温、大气湿度、土温和水温等参数。每月进行一次采样分析(包括土样、水样)，分析项目包括土壤基本性质(有机质、机械组成、pH、COD)、汞含量、汞形态、土壤微生物类群等指标。土／水-气界面汞交换通量采用动力通量箱与Lumex~(?) RA-915~+测汞仪联用技术监测，土壤汞形态参照Tessier(1979)的方法测定。同时，参照水旱轮作土壤干湿交替的环境条件进行室内模拟试验，以进一步研究其动态变化特征。通过数据分析整理，确定稻田土壤在干湿交替环境下向大气释放汞的通量。并研究不同施肥状况、不同季节、轮作的不同时期及其作物(油菜、小麦／水稻)条件下环境界面(水／土-气)汞的释放通量变化特征，研究了气象因子、土壤性质以及微生物类群对汞释放通量的影响，在此基础上对重庆市水-旱轮作农田汞的自然源释放进行初步量化。研究结果如下：
水旱轮作稻田土壤汞含量及汞的形态分布均随轮作期水旱交替过程而呈现周期性变化，表现为旱地土壤总汞含量高于水田土壤，汞形态以王水溶态为主，活性较低；水田土壤以可溶态汞为主，活性较高。这一变化过程的根本原因是由水早轮作方式导致的农田土壤氧化还原条件的周期性变化，汞的形态及活性的变化，必然影响到其在体系内的循环与转化过程。模拟试验显示，土壤汞含量越高，上覆水的汞浓度越大。淹水期间上覆水的汞浓度有两个较高点，第一个峰值出现在第3天，第二个峰值出现在第12天左右。土壤经过淹水—落干交替过程后，部分汞被散发到大气中，这部分汞主要是酸溶态和碱溶态汞经生物或非生物还原过程，以Hg~0的形式释放。淹水期间上覆水DGM和Hg~(2+)含量的变化趋势相反，说明它们之间在一定条件下可以相互转化。模拟试验中对汞通量的监测表明，二价汞(Hg~(2+))比其它价态的汞更容易在土壤-水体-大气界面中转化和交换。
试验区汞释放通量数据高于世界背景区域1个数量级，表明水旱轮作系统也是大气汞的一个重要的自然释放源。在水旱轮作期内，水稻生长期稻田水．气界面汞交换通量最大(82.94±73.3ng m~(-2) h~(-1))，休闲期土-气界面汞交换通量次之(24.0±17.1ngm~(-2)h~(-1))，油／麦生长期土-气界面汞交换通量最小(11.04±3.5ng m~(-2) h~(-1))。年平均汞通量为39.34±53.2ng m~(-2) h~(-1)。
紫色土农田水／土-气界面间的汞通量表现出明显的日变化、期间变化和季节性变化。不同轮作期不同界面间的汞挥发通量存在较大差异，其大小顺序为，暖季稻田＞暖季空地＞暖季油麦田＞冷季油麦田。白天水／土-气界面汞通量都呈现早晚低，午间高的趋势，沉降多出现在傍晚和早晨。水旱轮作稻田基质总汞含量与其释放量之间存在正相关关系(水体，r=0.463~*，p＜0.05；土壤，r=0.322~*，p＜0.05)。土壤有机质含量与汞通量之间存在极显著的负相关关系(r=-0.688~(**)，p＜0.01)。气象因子对界面汞交换的影响极其显著，水-旱轮作期间旱地土壤和稻田水体表面的汞挥发通量与太阳辐射量表现出相同的变化趋势，两者之间呈极显著的正相关(r=0.730~(**)，p＜0.01)。旱地土壤表面(2～5cm)温度、水体表层温度与汞通量呈极显著(r=0.514~(**)，p＜0.01)和显著(r=0.171~*，p＜0.05)正相关。经Arrhenius方程计算得出，农田早地土壤产生气态单质汞的化学反应活化能为21.5kcal mol~(-1)(19.5～33.4℃)，水田土壤为27.7 kcal mol~(-1)(4.5～34.3℃)。其化学反应活化能高于单质汞的蒸发焓，说明汞在水／土表面释放不是单质汞的直接蒸发。相对于土-气界面来说水-气界面汞交换更为复杂，水面汞释放应该看作是水体和大气亚表层发生的各种物理化学反应由此产生的拮抗或协同作用下的最终结果。空气相对湿度在水稻生长期与汞通量的关系不明显，而在油／麦生长期和休闲期，相对湿度与汞通量存在极显著的负相关关系(r=-0.748~(**)，-0.730~(**)，p＜0.01)。土壤湿度与汞通量在一定程度上有一致的变化趋势，但在监测期内对水旱轮作条件下紫色土汞的释放影响甚微。
耕作方式对汞释放的影响也较显著。不同试验小区的汞通量受施肥条件和地表覆盖物的影响很大，施肥状况影响作物生长量和作物密度，也影响到土壤性质、性状和土壤中汞形态及其相互转化，从而影响汞的固定和释放。但施肥条件对水体汞挥发的影响并不明显。
在水稻生长期，稻田土壤中的厌氧细菌群落数量与汞释放通量呈相反趋势(r=-0.580~*，p＜0.05)，其中硫酸盐还原菌(SRB)和厌氧纤维素分解菌(ACDB)与汞通量有显著负相关关系(r=-0.630~*，-0.558~*，p＜0.05)，是影响汞形态转化和释放的主要类群。而在休闲期及油／麦生长期，微生物群落数与汞通量之间不存在明显的相关性。这说明旱地土壤汞的释放，主要由其他环境因素(如气象因子)决定，而在厌氧环境下，细菌对水田土壤汞的释放起着重要作用。
基于通量箱法实地测得的数据，并结合重庆市的气候特点，对该地区水旱轮作农田汞释放量进行初步估算，重庆市每年从水-旱轮作农田释放到大气中的总汞量为565kg。
As a global pollutant, mercury is receiving intensive scrutiny due to its special physical characteristics. It occurs in various physical and chemical forms, likely volatilization and long range transportation in the environment. In recent years, the concentration of mercury is increasing in the atmosphere due to the elevated emission of anthropogenic activities, such as combustion of fossil fuels, roasting and smelting of ores etc. Most of atmospheric Hg in ambient air, above 90%, is made up of elemental mercury (Hg~0), while the remainders are divalent Hg compounds, either in the gaseous phase or bound to particles, and methylmercury. The Hg~0 (g) has a relatively long residence time of 0.5～2 years in the atmosphere, and which can transportation for a long distance along the global atmosphere cycling and to pose a global pollution. Researches of mercury pollution associated with human health risk had been considerable concerned in past years. In recent years, the hotspot issues of mercury pollution were mostly turned to the aspect of understanding the laws of mercury cycling and transformation in the atmosphere on global scale. So, it is important to discern the resources of mercury emission and measure or estimate the amounts correctly of mercury exchange.
The atmospheric loading of mercury is come from natural and anthropogenic sources. Emission inventories indicate that the contribution of mercury emission from natural sources is about 50% within the total amount of emission from global surface. Many researches involve to mercury emission from environmental surface in recent years, which include evasion from active volcano, earth heat-radiating, forest-fire, soil/water surface, transpiration from foliage of vegetation and urban surface etc, have provided lots of references to assessment of annual inventories of atmospheric mercury budget on global scale. However, there are some drawbacks with error and uncertainty in these estimations due to the restriction of limited spatial-temporal scale. Average inventories of mercury emission from natural sources has been estimated ranges between 2500 and 19325 t yr~(-1), and the contribution from anthropogenic sources ranges between 910 and 110001 yr~(-1). Researches on biogeochemical cycle of mercury in recent years were mostly focused on assessment of mercury release flux on environment surface, and an average rate of Hg evasion, 1.5 ng m~(-2)h~(-1), was taken to be the normal standard rate. Nevertheless, the field studies lately exhibited that the foregoing rate would lead to lower estimate the contribution from natural sources of mercury emission. Therefore, it is important to distinguish and determine the characteristics of various natural surfaces, and that is for the purpose of improvement estimation of mercury budget exactly and fully understanding global biogeochemical cycling of mercury.
At present, for study mercury emission from natural sources, dynamic flux chamber (DFC) technique has been adopted widely, which was first used by Schroeder et al. (1989) and Xiao et al. (1991) for measurement mercury exchange flux over different environmental interfaces (e.g. soil/water-air). Through the studies for last decade, people have realized preliminarily many important aspects of mercury exchange flux from various natural surfaces, but there are scarcely reports that involved with the mercury exchange characteristics in the interfaces of periodicity dry-wet alternating environment (e.g. water level fluctuating zone of reservoir, paddy-upland rotation farm land). Especially, there are lack of informations about the aspect of the seasonal varies characteristics of mercury release and climatic influencing factors in the special environment.
Paddy-upland rotation is a farming tradition that wildly adopted by Asian countries and it also used as a main culture manner in south China. The area of paddy-upland rotation farmland covered above 1400 millions hm~2 in China and it consists of 30～40% of the rice-land resources. Paddy-upland rotation system has an intrinsic peculiar characteristic that the conditions of thermal energy and oxidation- deoxidization change heavily along the periodic varying of season, and this may lead to an evident influence in the course of mercury transformation, transport and accumulation in soil. Because of lack of systematic informations measured about this circumstance, the purpose of this paper is to study the characteristics of mercury release fluxes and its chemical forms transformation, in the paddy-upland (dry-wet) rotation system. This research would exhibit an important significance for improvement on farther understanding the regional or global mercury resource and its release intensity.
Here, the study was conducted by both in simulating experiment, laboratory analysis and field investigation in situ. The field investigation site was located at National Purple Soil Fertility and Fertilizer Efficiency Monitored Base (E:106°24'33.3'' N:29°48'36.2"), which situated at Southwest University, Beibei District in Chongqing, China. The research area belongs to the purple hilly land with an elevation of 239 m. The subtropical earth monsoon climate is presented in there. According to statistics, the mean annual temperature is 18.4°C, annual precipitation is 1105.5 mm, and annual duration of sunshine is 1276.7 h. The tested soil was the gray brown purple soil (Purpli-Udic Cambosols), which is a neutral purple soil subtype and developed from the purple mud stone and shale of Saximiao Association of Jurassic Period. It is the most purple soil types, and it occupies about 40% of the area of purple soils and most of the grain base in Chongqing distribute in it. So it is the typical representative of purple soils. The research area covered 1200 m~2 and was ploted out to 13 divisions.
Different chemical form of mercury has different transference activeness in soil, and it can dominate the release flux of theirs, ultimately. Wherefore, this study had analyzed the mercury existence forms and its variety in different farming seasons while in the flooding period (rice growth term), the intermission period and the upland period (wheat/rape growth term), respectively. Besides, the study had studied the characteristics of mercury exchange and distribution between the soil and water interface in rice growth period by means of simulating flooding experiment. The results revealed that, the mercury content and species distribution of paddy-upland rotation soil varying periodically along with the alternating change of farming period, namely dry-wet change by turn. Total mercury content in the upland soil is higher than that of flooding soil. Residual Hg is the predomination species in the upland soil, and it has a lower activity. Contrarily, soluble Hg is the predomination species in the flooding soil and it has a higher activity. The essential reason of this situation is caused by the periodic change of oxidation-deoxidization conditions in farmland. The results of simulating flooding experiment demonstrated that the mercury concentration of water column increased with the increasing content of soil Hg. Mercury concentration in water have two peak values after flooding, the first peak occurred earlier (3~(rd) d), the latter appeared relatively later (about 12~(th) d). After the wet-dry process, partly soil mercury evasion into the air presented as Hg~0, and which is mainly the production of acid-soluble and H_2O-soluble forms Hg deoxidized through biological or abiological transforming course. During flooding period, the concentration fluctuation trend between DGM and Hg~(2+) in water column is reverse, and it implies that they could transform to each other at suitable environmental condition. The data of mercury fluxes measured in the simulating flooding experiment course showed that, the divalent Hg is easier exchange, transformation and finally evaporation to atmosphere than other forms of mercury in the soil-water-air interface.
Mercury fluxes measurement were performed by dynamic flux chamber (DFC) cope with the Lumex~? Multifunctional mercury analyzer RA-915~+during different farming season while in the flooding period (rice growth term), the intermission period and the upland period (wheat/rape growth term) respectively, at all plots in the investigating field. The characteristics of mercury flux in different farming seasons and covered crops were discussed. Simultaneously, mercury flux influencing factors such as meteorological, soil properties, fertilizer management and microbial communities were also discussed. Finally, an annual emission of mercury to the atmosphere from paddy-upland rotation farmland in Chongqing was estimated. The results indicated that, the average value of mercury fluxes in investigated area was higher than that of global background by 1 magnitude. Therefore, the results imply that the paddy-upland rotation system may be an importance resource which is a potentially contributor to the atmospheric mercury content. During whole dry-wet rotation farming seasons, the mean mercury exchange flux at water-air interface in rice land is the highest with the value of 82.9±73.3 ng m~(-2) h~(-1), next to the soil-air interface in intermission period with the value of 24.0±17.1 ng m~(-2) h~(-1), the mean flux of soil-air interface in wheat/rape growth period was the lowest with the value of 11.0±3.5 ng m~(-2) h~(-1). The annual average mercury flux in whole fanning seasons is 39.3±53.2 ng m~(-2) h~(-1).
Mercury fluxes of water/soil-air interfaces from purple soil rotation farmland exhibit a significantly diurnal and seasonal variation. There was evidently difference of fluxes measured from different season and interface, the decreasing order is as follows warm season rice land (water/air), warm season intermission leisure land (soil/air), warm reason rice/wheat land (soil/air) and cold season rice/wheat land (soil/air). Mercury evasion exhibits a strong diurnal cycle variation, with the highest during midday, while lower in the morning and early evening. Mercury fluxes over air/surfaces had bi-directional exchange in the morning and early evening in cold season. Results of statistical analysis showed, there was positive correlation between mercury flux and total Hg content in paddy-upland rotation farmland (water: r=0.463~*, soil: r=0.322~*), on the contrary, there was significantly negative correlation between mercury flux and soil organic matter content (r=-0.688**). Climatic factors had effected evidently to mercury flux in the water/soil-air interfaces. Regression analysis of data measured over water/soil surface indicated that mercury flux appear to be most significantly positive relation to solar radiation (r=0.730~(**)) and soil/water temperature (soil: r= 0.514~(**); water: r = 0.171~*), and significantly negatively correlated with relative humidity over soil surface (r=-0.748~(**)), and weaker correlated with relative humidity over water surface and soil moistness. Analysis of data measured also suggested that exponential correlation of mercury flux with soil/water temperature in some plots (soil: R~2= 0.3047~(**); water: R~2=0.7044~(**)). Arrhenius equation could be applied to explain the link between the kinetics rate constant of this process and the soil/water temperature, so the activation energy (Ea) was then calculated to be 21.5 / 27.7 kcal mol~(-1) from the slope of best fit line. The values were higher than the mercury vaporization heat of 14.5 kcal mol~(-1), implying that the mercury emission from soil /water surface is not the vaporization of elemental mercury alone.
Likewise, results of this research suggested that, farming manner, include crop category, coverage density and fertilizer management, would be an important influencing factor that can effect evidently to mercury flux from the soil/water surface. Especially, the fertilizer management can cause the changes of soil property, microbeial communities and mercury existence form and its transformation. Sequentially, it dominates the course of mercury accumulation and emission in soil.
Moreover, data obtained from microorganism cultivation revealed that, a negatively correlation (r= -0.580~*) between the amount of anaerobic bacterial communities (cfu) in the flooding soil and mercury fluxes over water surface during the rice/rape growth term. Two categories of bacterial populations, sulfate-reducing bacteria (SRB) and anaerobic cellulose-decomposing bacteria (ACDB) , were the dominating populations for influencing mercury release flux during the flooding terms, the correlation coefficients were -0.630~*(SRB) and -0.558~* (ACDB), respectively. Nevertheless, the correlation between bacteria communities and mercury fluxes in upland was insignificant. This means that the mercury flux in upland was dominated by other environmental factors.
Associating with climate characteristics of Chongqing, a preliminary estimation of regional mercury budget was carried out based on the fluxes data of the experimental plots which measured by dynamic flux chamber. The total mercury emission to the atmosphere from dry-wet rotation farm fields was annually about 565 kg in Chongqing.
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