三峽庫區(qū)典型農(nóng)業(yè)小流域溶解性有機質(zhì)（DOM）的地球化學(xué)特征分析
發(fā)布時間：2019-05-18 21:43
【摘要】：三峽庫區(qū)消落帶作為敏感的生態(tài)環(huán)境系統(tǒng),自蓄水以來,以其獨特的“干濕交替”特征一直受到廣泛關(guān)注。它是庫區(qū)水體和周邊陸地生態(tài)系統(tǒng)物質(zhì)和能量轉(zhuǎn)移與轉(zhuǎn)化的活躍地帶,具有緩沖帶和植物護岸功能,對外界變化的響應(yīng)相當(dāng)敏感。以坡耕地為主的農(nóng)業(yè)小流域系統(tǒng),對庫區(qū)消落帶生態(tài)環(huán)境質(zhì)量起著重要作用。DOM作為全球碳循環(huán)的重要組成部分,它對全球氣候變化有重要影響,也是生態(tài)系統(tǒng)中物質(zhì)與能量循環(huán)的重要活性組分,與生態(tài)系統(tǒng)中諸多重要環(huán)節(jié)密切相關(guān)。由于DOM活躍的環(huán)境角色,農(nóng)業(yè)小流域中DOM對臨近水環(huán)境產(chǎn)生的重要影響,無疑會進一步影響該區(qū)域內(nèi)營養(yǎng)元素、重金屬、有機污染物及溫室氣體等的環(huán)境行為�；诖�,本研究選取了三峽庫區(qū)消落帶典型農(nóng)業(yè)小流域——重慶涪陵區(qū)王家溝小流域為對象,結(jié)合紫外可見及熒光光譜手段對該流域內(nèi)不同利用類型土壤DOM和不同類型水體DOM以及兩條小流域出口水DOM的季節(jié)變化進行監(jiān)測分析,以期闡明典型農(nóng)業(yè)小流域土壤和水體中DOM地球化學(xué)特征的異質(zhì)性,結(jié)果表明:(1)不同土地利用條件下DOM性質(zhì)差異明顯,以林地土壤DOM的芳香性程度較高,腐殖化特征最強,其次為田地;盡管居民用地和菜地溶解性有機碳(DOC)含量高(均值分別為80.69 mg·L-1和89.20 mg·L-1),但是芳香化程度低,DOM中非生色組分對高DOC含量的貢獻明顯。所有樣本熒光指數(shù)(FI)介于自生源特征(FI=1.9)和陸源特征(FI=1.4)之間,自生(類蛋白組分)和異生源(類腐殖組分)對DOM均有貢獻。大部分土壤樣本類蛋白/類腐殖熒光組分(r(T/C))都大于2.0,說明該農(nóng)業(yè)小流域土壤DOM受外來因素尤其是人類活動影響較大,尤以菜地為代表。另外,不同紫外可見和熒光光譜參數(shù)對不同土地利用條件下DOM結(jié)構(gòu)和性質(zhì)差異性的靈敏程度不同,光譜斜率比值(SR)和腐殖化指數(shù)(HIX)不能反映DOM地化特征的差異性,因此單一的紫外可見或者熒光光譜指標(biāo)并不能全面提供DOM的特征信息,建議兩種光譜分析方法聯(lián)用。(2)溶解性有機質(zhì)(DOM)作為重要的地球化學(xué)因子,在流域水體環(huán)境中扮演著重要的作用。該農(nóng)業(yè)小流域水體dom空間差異較大,其組成和來源均存在明顯不同。有色溶解性有機質(zhì)(cdom)在dom中所占比例(ag*(355))大小順序為:稻田水溝渠水池塘水井水出口水,其中稻田水和溝渠水的suva254較井水和出口水大,芳香性更明顯。三維熒光光譜中存在2類4個熒光峰(a、c和b、t),dom來源都是內(nèi)部(微生物、藻類)以及外源(腐殖質(zhì))的雙重貢獻。除自生源微生物活動的影響外,外源生活污水和農(nóng)業(yè)生產(chǎn)用水的影響也是導(dǎo)致dom組分中類蛋白組分增多的重要原因。對比了不同種植季時相同位置水樣dom光譜特征,類蛋白組分是控制兩個種植季水體dom特征波動的重要因素。土地使用方式變化后水體doc、cdom和dom當(dāng)中的r(t/c)存在明顯差異,而fi、自生源指數(shù)(bix)和短波處/長波處類腐殖熒光組分(r(a/c))差異不顯著。(3)不同土地利用類型土壤doc庫容量差異較大,呈現(xiàn)出不同地化特征。其中以菜地doc庫容量最大為0.798mg·g-1,結(jié)構(gòu)較為復(fù)雜;田地最低為0.237mg·g-1。dom中非生色組分對高doc含量具有重要貢獻。不同提取比例的cdom與doc不存在顯著性相關(guān)性(p0.05)。主成分分析結(jié)果表明doc庫容量變化受到自生源微生物活動及外來人為因素等共同的影響。由于受到外部光降解及人為因素等的綜合影響,四種類型土壤doc庫容量與dom各光譜參數(shù)的相關(guān)性不盡相同,單一的光譜指標(biāo)并不能準確的反映出doc庫容量變化情況,建議紫外和熒光光譜兩種指標(biāo)聯(lián)合分析。吸附平衡常數(shù)ks與溶解性有機碳庫容量[doc]具有極顯著性正相關(guān),吸附常數(shù)大的土壤具有較高的doc庫容量。(4)小流域全年出口水樣dom的熒光有機物(fdom)、cdom分別與doc表現(xiàn)出極顯著的相關(guān)性(p0.05),不同采樣時間doc濃度大小順序為:4月11月7月1月。doc濃度全年變化范圍在1.22~165.00mg·l-1之間,cdom濃度[a(355)]變化范圍在0.08~24.47m-1,fdom濃度[fn(355)]變化范圍為2063.80~102811.99m-1。不同采樣時間類蛋白物質(zhì)(peakb和peakt)熒光強度的順序為4月11月7月1月。fi值年季變化范圍為1.55~1.75,介于陸源特征值1.40和內(nèi)源貢獻值1.90之間,dom受內(nèi)源貢獻和外源輸入的綜合影響。兩條小流域sub-1和sub-2的自生源貢獻、芳香性、疏水性組分大小、分子量均存在顯著性差異。夏季農(nóng)業(yè)小流域水體dom腐殖化程度最高,自生源特征較明顯,類蛋白組分貢獻較大,生物可利用性較高;春、秋季水樣dom腐殖化程度居中,冬季最弱。農(nóng)業(yè)小流域水體thg和表征dom分子量大小的sr存在極顯著正相關(guān)性(p0.05),而與fi顯著負相關(guān)(p0.05)。dhg與a(355)、sr也存在極顯著性正相關(guān)(p0.05),而與fi顯著負相關(guān)(p0.05)。(5)溶解性有機質(zhì)(dom)是水體生態(tài)系統(tǒng)的重要組成部分,其性質(zhì)和結(jié)構(gòu)決定了其在污染物環(huán)境行為中扮演著重要角色(例如對汞的遷移轉(zhuǎn)化的影響)。另外,SUVA254和DOC與各形態(tài)Hg無明顯相關(guān)性,但水體生色組分和分子量大小是控制溶解態(tài)和活性汞的重要因素;甲基汞變化可能與水體初級生產(chǎn)力導(dǎo)致的有機質(zhì)富集和遷移關(guān)系密切。
[Abstract]:As the sensitive ecological environment system of the Three Gorges Reservoir, its unique "dry and wet alternation" characteristics have been widely concerned since the water storage. It is an active area of the physical and energy transfer and transformation of the water and surrounding land ecosystem in the reservoir area, and has the function of buffer zone and plant bank protection, and is quite sensitive to the response of the external change. The agricultural small watershed system, which is based on the slope land, plays an important role in the ecological environment quality of the reservoir in the reservoir area. As an important part of the global carbon cycle, DOM has an important influence on the global climate change, and it is also an important active component of the material and energy circulation in the ecosystem, which is closely related to many important links in the ecosystem. Because of the active role of the DOM, the important influence of the DOM on the water environment in the agricultural small watershed will undoubtedly further affect the environmental behavior of the nutrient elements, heavy metals, organic pollutants and greenhouse gases in the region. On the basis of this, the study has selected the small watershed of Wangjiagou, the typical agricultural small watershed in the Three Gorges Reservoir area, which is the object of the small watershed. in ord to clarify that heterogeneity of the DOM geochemical characteristics in the soil and the water body of the typical agricultural small watershed, The results show that: (1) The difference of DOM in different land-use conditions is obvious, and the soil DOM of the forest land has a high degree of aromaticity, and the humification is the strongest, and the second is the field; Although the content of soluble organic carbon (DOC) was high (80.69 mg 路 L-1 and 89.20 mg 路 L-1, respectively), the degree of aromatalization was low and the contribution of the non-chromophoric component in the DOM to the high DOC content was significant. The fluorescence index (FI) of all samples is between the self-source characteristics (FI = 1.9) and the land-source characteristics (FI = 1.4), and the self-generated (class-like component) and the isogenic (species-like humic components) contribute to the DOM. Most of the soil sample class protein/ humic fluorescent component (r (T/ C)) is greater than 2.0, indicating that the soil DOM of the agricultural small watershed is influenced by external factors, especially human activities, especially in the vegetable field. in addition, that sensitivity of the different UV-and fluorescence spectral parameters to the difference of the DOM structure and the property in different land-use conditions is different, and the ratio of the spectral slope (SR) and the humification index (HIX) cannot reflect the difference of the characteristic of the DOM, Therefore, the single ultraviolet-visible or fluorescent spectrum index can not provide the characteristic information of the DOM in a comprehensive way, and it is suggested that the two spectral analysis methods can be used in combination. (2) The soluble organic matter (DOM) plays an important role in the water environment of the basin as an important geochemical factor. There is a large difference in the dom space between the water bodies in the small watershed, and the composition and the source of the water are obviously different. The order of the size of the colored soluble organic matter (cdrom) in the dom (ag * (355)) is: the water outlet of the water in the water and the water in the paddy field of the rice field, wherein the suva254 of the rice field water and the ditch water is larger than the well water and the outlet water, and the aromatic property is more obvious. There are four fluorescence peaks (a, c and b, t) in the three-dimensional fluorescence spectrum, both of which are the dual contribution of the inside (micro-organisms, algae) and the foreign (humus). In addition to the influence of the microbial activity of the biogenic source, the influence of the exogenous domestic sewage and the water for agricultural production is also an important cause of the increase of the protein-like components in the dom component. The dom spectral characteristics of the water samples at the same location in different planting season are compared, and the component of the class protein is an important factor to control the fluctuation of the dom characteristics of the two planting seasons. There was a significant difference in r (t/ c) among the water body doc, cdrom and dom after the change of the land use method, and the difference of fi, the self-source index (bix) and the humification fluorescent component (r (a/ c)) at the short-wave and long-wave sites was not significant. (3) The different types of soil doc storage capacity of different land use types show different characteristics. The maximum capacity of doc is 0.798 mg 路 g-1, the structure is more complex, the lowest of the field is 0.237 mg 路 g-1.dom, the non-chromophoric component has an important contribution to the high doc content. There was no significant correlation between ccom and doc in different extraction ratios (p0.05). The results of principal component analysis show that the change of the capacity of doc library is influenced by the self-source microbial activity and the external human factors. Due to the comprehensive influence of external photodegradation and human factors, the correlation between the capacity of the four types of soil doc and the parameters of dom's spectral parameters is different, and the single spectral index can not accurately reflect the change of the capacity of the doc library, and it is suggested that the combination of the two indexes of the ultraviolet and the fluorescence spectrum can be combined. The adsorption equilibrium constant ks has a very significant positive correlation with the dissolved organic carbon library capacity[doc], and the soil with large adsorption constant has higher doc storage capacity. (4) The fluorescence organic matter (fdom) and cdrom of the water sample dom in the whole year of the small watershed were significantly correlated with the doc (p0.05). The order of the concentration of the different sampling time doc was: April, November, November. The variation range of the concentration of doc (a (355)] in the range of from 1.22 to 165.00 mg 路 l-1 and the concentration of fdom[a (355)] varied from 0.08 to 24.47 m-1, and the range of fdom concentration[fn (355)] ranged from 2063.80 to 102811.99 m-1. The order of the fluorescence intensity of a different sample time class of protein material (peakb and peakt) was April, November, November. The variation range of fi-value is 1.55-1.75, between the land-source characteristic value 1.40 and the intrinsic contribution value of 1.90, and dom is influenced by the endogenous contribution and the exogenous input. There was a significant difference in the self-source contribution, the aromaticity, the hydrophobic component size and the molecular weight of the sub-1 and sub-2 of the two small watersheds. In summer, the degree of water dom in the small watershed is the highest, the self-source is more obvious, the component of the class protein is relatively large, and the bioavailability is high; in the spring, the water sample of autumn is in the middle of the humification degree, and the winter is the weakest. There was a significant positive correlation between the water content (thg) and the sr (p0.05), and the significant negative correlation with fi (p0.05), and a significant negative correlation with fi (p0.05), while there was a significant negative correlation with fi (p0.05). (5) Dissolved organic matter (Dom) is an important part of the water body ecosystem, and its nature and structure decide that it plays an important role in the environmental behavior of the pollutants (for example, the effect on the migration and transformation of the mercury). In addition, there is no significant correlation between SUVA 254 and DOC, but the color and molecular weight of the water body are important factors for controlling the dissolved state and active mercury; the change of methylmercury may be closely related to the enrichment and migration of organic matter caused by primary productivity of the water body.
【學(xué)位授予單位】：西南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：X52
[Abstract]:As the sensitive ecological environment system of the Three Gorges Reservoir, its unique "dry and wet alternation" characteristics have been widely concerned since the water storage. It is an active area of the physical and energy transfer and transformation of the water and surrounding land ecosystem in the reservoir area, and has the function of buffer zone and plant bank protection, and is quite sensitive to the response of the external change. The agricultural small watershed system, which is based on the slope land, plays an important role in the ecological environment quality of the reservoir in the reservoir area. As an important part of the global carbon cycle, DOM has an important influence on the global climate change, and it is also an important active component of the material and energy circulation in the ecosystem, which is closely related to many important links in the ecosystem. Because of the active role of the DOM, the important influence of the DOM on the water environment in the agricultural small watershed will undoubtedly further affect the environmental behavior of the nutrient elements, heavy metals, organic pollutants and greenhouse gases in the region. On the basis of this, the study has selected the small watershed of Wangjiagou, the typical agricultural small watershed in the Three Gorges Reservoir area, which is the object of the small watershed. in ord to clarify that heterogeneity of the DOM geochemical characteristics in the soil and the water body of the typical agricultural small watershed, The results show that: (1) The difference of DOM in different land-use conditions is obvious, and the soil DOM of the forest land has a high degree of aromaticity, and the humification is the strongest, and the second is the field; Although the content of soluble organic carbon (DOC) was high (80.69 mg 路 L-1 and 89.20 mg 路 L-1, respectively), the degree of aromatalization was low and the contribution of the non-chromophoric component in the DOM to the high DOC content was significant. The fluorescence index (FI) of all samples is between the self-source characteristics (FI = 1.9) and the land-source characteristics (FI = 1.4), and the self-generated (class-like component) and the isogenic (species-like humic components) contribute to the DOM. Most of the soil sample class protein/ humic fluorescent component (r (T/ C)) is greater than 2.0, indicating that the soil DOM of the agricultural small watershed is influenced by external factors, especially human activities, especially in the vegetable field. in addition, that sensitivity of the different UV-and fluorescence spectral parameters to the difference of the DOM structure and the property in different land-use conditions is different, and the ratio of the spectral slope (SR) and the humification index (HIX) cannot reflect the difference of the characteristic of the DOM, Therefore, the single ultraviolet-visible or fluorescent spectrum index can not provide the characteristic information of the DOM in a comprehensive way, and it is suggested that the two spectral analysis methods can be used in combination. (2) The soluble organic matter (DOM) plays an important role in the water environment of the basin as an important geochemical factor. There is a large difference in the dom space between the water bodies in the small watershed, and the composition and the source of the water are obviously different. The order of the size of the colored soluble organic matter (cdrom) in the dom (ag * (355)) is: the water outlet of the water in the water and the water in the paddy field of the rice field, wherein the suva254 of the rice field water and the ditch water is larger than the well water and the outlet water, and the aromatic property is more obvious. There are four fluorescence peaks (a, c and b, t) in the three-dimensional fluorescence spectrum, both of which are the dual contribution of the inside (micro-organisms, algae) and the foreign (humus). In addition to the influence of the microbial activity of the biogenic source, the influence of the exogenous domestic sewage and the water for agricultural production is also an important cause of the increase of the protein-like components in the dom component. The dom spectral characteristics of the water samples at the same location in different planting season are compared, and the component of the class protein is an important factor to control the fluctuation of the dom characteristics of the two planting seasons. There was a significant difference in r (t/ c) among the water body doc, cdrom and dom after the change of the land use method, and the difference of fi, the self-source index (bix) and the humification fluorescent component (r (a/ c)) at the short-wave and long-wave sites was not significant. (3) The different types of soil doc storage capacity of different land use types show different characteristics. The maximum capacity of doc is 0.798 mg 路 g-1, the structure is more complex, the lowest of the field is 0.237 mg 路 g-1.dom, the non-chromophoric component has an important contribution to the high doc content. There was no significant correlation between ccom and doc in different extraction ratios (p0.05). The results of principal component analysis show that the change of the capacity of doc library is influenced by the self-source microbial activity and the external human factors. Due to the comprehensive influence of external photodegradation and human factors, the correlation between the capacity of the four types of soil doc and the parameters of dom's spectral parameters is different, and the single spectral index can not accurately reflect the change of the capacity of the doc library, and it is suggested that the combination of the two indexes of the ultraviolet and the fluorescence spectrum can be combined. The adsorption equilibrium constant ks has a very significant positive correlation with the dissolved organic carbon library capacity[doc], and the soil with large adsorption constant has higher doc storage capacity. (4) The fluorescence organic matter (fdom) and cdrom of the water sample dom in the whole year of the small watershed were significantly correlated with the doc (p0.05). The order of the concentration of the different sampling time doc was: April, November, November. The variation range of the concentration of doc (a (355)] in the range of from 1.22 to 165.00 mg 路 l-1 and the concentration of fdom[a (355)] varied from 0.08 to 24.47 m-1, and the range of fdom concentration[fn (355)] ranged from 2063.80 to 102811.99 m-1. The order of the fluorescence intensity of a different sample time class of protein material (peakb and peakt) was April, November, November. The variation range of fi-value is 1.55-1.75, between the land-source characteristic value 1.40 and the intrinsic contribution value of 1.90, and dom is influenced by the endogenous contribution and the exogenous input. There was a significant difference in the self-source contribution, the aromaticity, the hydrophobic component size and the molecular weight of the sub-1 and sub-2 of the two small watersheds. In summer, the degree of water dom in the small watershed is the highest, the self-source is more obvious, the component of the class protein is relatively large, and the bioavailability is high; in the spring, the water sample of autumn is in the middle of the humification degree, and the winter is the weakest. There was a significant positive correlation between the water content (thg) and the sr (p0.05), and the significant negative correlation with fi (p0.05), and a significant negative correlation with fi (p0.05), while there was a significant negative correlation with fi (p0.05). (5) Dissolved organic matter (Dom) is an important part of the water body ecosystem, and its nature and structure decide that it plays an important role in the environmental behavior of the pollutants (for example, the effect on the migration and transformation of the mercury). In addition, there is no significant correlation between SUVA 254 and DOC, but the color and molecular weight of the water body are important factors for controlling the dissolved state and active mercury; the change of methylmercury may be closely related to the enrichment and migration of organic matter caused by primary productivity of the water body.
【學(xué)位授予單位】：西南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2016
【分類號】：X52
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8 肖q轄，
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