本文選題：長江口-東海內(nèi)陸架　切入點：磷　出處：《中國海洋大學》2015年博士論文　論文類型：學位論文

【摘要】：大河河口及大河影響下的陸架邊緣海磷的生物地球化學過程是海洋磷循環(huán)的重要組成部分。本論文以長江口-東海內(nèi)陸架為主要研究海域,采用現(xiàn)場調(diào)查與實驗室模擬相結合的方法,借助顆粒物分級的手段,結合顆粒物粒度組成、比表面積(Specific surface area, SSA)、礦物組成、有機碳及其穩(wěn)定同位素和磷酸鹽中的氧同位素等多種參數(shù),對水體、顆粒物、沉積物及間隙水中磷的形態(tài)分布、混合行為和遷移轉化規(guī)律進行了較為系統(tǒng)的研究,以期加深對長江口-東海內(nèi)陸架磷的生物地球化學過程的理解,豐富對高渾濁河口生源要素的生物地球化學循環(huán)的認識。獲得的主要結果如下：1.沿長江口鹽度梯度采集了表層水和懸浮顆粒物樣品(2011年6月),對溶解磷和顆粒磷形態(tài)的分布、混合行為及遷移轉化進行了研究。用水淘選法將顆粒物分為5個粒級,用改進的SEDEX (sequential extraction method)方法對不同形態(tài)的顆粒磷進行分析測定,發(fā)現(xiàn)不同形態(tài)磷之間、尤其是溶解磷和活性顆粒磷形態(tài)即可交換態(tài)磷(Exchangeable-P, Ex-P)、有機磷(Organic-P, Or-P)和鐵結合態(tài)磷(Fe-bound P, Fe-P)之間存在強烈的相互轉化。碎屑磷(Detrital-P,De-P)和Or-P是懸浮顆粒物中含量最為豐富的兩種磷形態(tài),分別占了總顆粒磷的43.9%和26.1%。De-P的含量隨著顆粒物粒徑的增大而升高,而Or-P及其它形態(tài)磷的含量隨著顆粒物粒徑的增大而降低。8μm組分被認為是“真正懸浮”的顆粒物,本研究表明,“真正懸浮”的顆粒物所攜帶的生物可利用磷(Bioavailable-P, BAP;為Ex-P、Or-P和Fe-P之和)的通量為0.21×104tPyr-1,占總生物可利用磷輸送通量的29%。細粒徑顆粒物中P/SSA值很低,表明這些顆粒物中磷的保存效率較低。長江口分級懸浮顆粒物中的De-P/SSA和Fe-P/SSA與長江口表層沉積物基本基本相當,Au-P(自生磷灰石磷,Authigenic-P)/SSA和Re-P(難分解有機磷,Refractory-P)/SSA從懸浮顆粒物到表層沉積物略有降低,而表層沉積物中Ex-P/SSA和Or-P/SSA顯著低于懸浮顆粒物,進一步表明了不同形態(tài)的顆粒磷隨懸浮顆粒物在河口沉降的過程中具有不同的行為特征。2.測定了沉積物分級樣品的顆粒磷形態(tài)并用分級的沉積物樣品進行吸附動力學實驗、吸附特征受鹽度影響的實驗和等溫吸附實驗。結果表明,沉積物中De-P的含量最為豐富,其次為Or-P。細粒徑沉積物中生物可利用磷的含量遠高于砂質沉積物,表明細粒徑顆粒物對磷從沉積物向上覆水或周圍間隙水的釋放發(fā)揮著主導作用。對從來自同一采樣站位的分級沉積物獲得的吸附等溫線進行分析發(fā)現(xiàn),不同粒徑沉積物對應的零平衡磷酸鹽濃度值(zero equilibrium phosphate concentration,EPCo)非常接近(細粉砂、中粉砂、粗粉砂和砂分別為55.0、54.9、51.7和49.0μgL-1)。沉積物對磷酸鹽的吸附容量、吸附速率和本底吸附值(native adsorbed phosphorus, NAP)很大程度上受粒徑的控制,粒徑32μm沉積物的總吸附容量值是粒徑32μm的沉積物的6倍。由于細粒徑沉積物對磷酸鹽具有較高的吸附容量,東海內(nèi)陸架的泥質區(qū)對上覆水及間隙水中的磷酸鹽濃度起著重要的調(diào)控作用,同時對長江輸入的磷酸鹽是一個有效的捕集器,可降低東海外陸架遭受富營養(yǎng)化的風險。3.通過對長江口及鄰近的東海內(nèi)陸架表層沉積物中的磷形態(tài)和沉積物基本特征進行分析,研究了磷的分布、生物可利用性和保存。結果表明,表層沉積物中總磷(Total phosphorus, TP)的變化范圍為15.0-21.4 μmolg-1,最高值出現(xiàn)在口門附近。De-P、Re-P、Or-P、Au-P、Ex-P和Fe-P對TP的貢獻分別為55.6%、17.8%、16.1%、5.5%、2.5%和2.5%。De-P含量最高的區(qū)域出現(xiàn)在長江口口門和河口外陸架區(qū)域。Or-P在長江口和浙閩沿岸泥質區(qū)含量較高,并與粉砂、SSA和TOC有相似的分布特點。Re-P主要分布在近河口和浙閩沿岸區(qū)域。De-P/SSA和TOC/SSA的比值隨SSA的增大而逐漸減小,而Or-P/SSA的比值隨SSA的增大基本不發(fā)生改變,表明Or-P在礦物表面已經(jīng)達到吸附-解吸平衡。TOC與總有機磷(Total organic-P, TOP;為Re-P與Or-P之和)的比值(平均～84)低于Redfield比值,表明長江口及鄰近的東海內(nèi)陸架移動泥區(qū)的有機物已經(jīng)進行了充分的再礦化。而TOC/Or-P的比值(72～422,平均值為188)則相對較高,表明在有機物再礦化的過程中Or-P優(yōu)先于TOC發(fā)生分解。4.測定了采集于該研究海域泥質區(qū)和非泥質區(qū)的三根柱狀沉積物樣品中的磷的形態(tài),并結合粒度組成、21oPb活度、TOC及其穩(wěn)定同位素(813C)、間隙水中的Fe2+和Mn2+以及間隙水和上覆水中的PO43-和NH4+等參數(shù),探討了不同沉積環(huán)境下磷的遷移轉化、成巖過程和保存特點。研究表明,受長江陸源輸入的影響,處于長江口及東海內(nèi)陸架泥質區(qū)的12和31號柱沉積物中的TP以及一些陸源磷形態(tài)尤其是De-P的含量遠高于處于非泥質區(qū)的33號站位。由于移動泥層的混勻作用,31號柱沉積物中的210Pbexcess、中值粒徑(Median grain size, MGS)以及多種磷形態(tài)(Ex-P、Or-P、Au-P、Re-P和De-P)的含量在沉積柱上層一定深度范圍內(nèi)幾乎保持不變,而且與下層分布表現(xiàn)出明顯的不同；而12號柱沉積物中210Pbcxcess及非活性磷形態(tài)(如De-P、Au-P和Re-P)的含量在整個深度范圍內(nèi)均保持不變。該區(qū)域柱狀沉積物中的Or-P和Fe-P發(fā)生了向Au-P的轉化。研究還發(fā)現(xiàn),處于泥質區(qū)的31號柱的沉積物是間隙水中磷酸鹽的源,而處于非泥質區(qū)的33號柱的沉積物充當了間隙水中磷酸鹽的匯。5.通過對采集于東海內(nèi)陸架柱狀沉積物中的沉積物粒徑、SSA、TOC、C/N比值、碳穩(wěn)定同位素以及顆粒磷形態(tài)進行分析,探討了用碎屑磷作為長江流域洪水歷史重建指標的可行性。研究發(fā)現(xiàn),De-P峰值出現(xiàn)在1850s、1860s、1900s、 1920s、1950s、1980s和2000s,與長江流域200年來發(fā)生的大洪水記錄吻合。研究還發(fā)現(xiàn),De-P與長江口1981年和1998年發(fā)生的兩次由長江大洪水引發(fā)的極端缺氧事件有較好的對應關系,而這兩次極端缺氧事件也已被Mo/Al所證實。進一步分析表明,De-P與長江流域1950s、1980s和2000s年發(fā)生的極端洪水事件以及與洪水相關的氣候事件,如加強的厄爾尼諾-南方濤動(ENSO, El Nino-Southern Oscillation)、偏弱的東亞夏季風(EASM, East Asian summer Monsoon)以及太平洋十年際振蕩(PDO, Pacific Decadal Oscillation)的暖位相均有較好的對應關系,表明De-P也可能成為指示與極端洪水事件相關的氣候事件的替代指標。6.沿長江口鹽度梯度共采集了7個站位的表層水樣品(2013年7月),通過磷酸鹽的氧同位素分析示蹤長江口磷酸鹽的循環(huán)狀況。結果表明,長江口水團可以用長江淡水和東海海水兩個端元的混合模型進行較好地描述。在此基礎上,本研究建立了磷酸鹽的818Op兩端元混合線和混合平衡線,并對磷酸鹽的循環(huán)情況進行研究,發(fā)現(xiàn)在長江淡水端,磷酸鹽并未經(jīng)歷強烈的生物循環(huán)過程,主要受物理混合作用的影響；最大渾濁帶磷酸鹽的生物循環(huán)過程也較弱,較深水層其它來源的磷酸鹽改變了該區(qū)域δ18Op原本的特征值；而在羽狀前鋒,δ18Op的測定值幾乎等于其平衡值,表明磷酸鹽已經(jīng)進行了充分的生物循環(huán)過程。
[Abstract]:The biogeochemical process of the River Estuary and river under the influence of marginal sea phosphorus is an important component of the marine phosphorus cycle. This paper takes the Yangtze Estuary and inner shelf of the East China Sea as the main study area, using field investigation and laboratory simulation combined with particulate fractions, the means of combining particle size composition the specific surface area (Specific, surface, area, SSA), mineral composition, particulate organic carbon and its stable isotopes and phosphate oxygen isotopes in various parameters of water, sediment and interstitial water, distribution of phosphorus, the mixing behavior of migration and transformation rules are studied systematically, in order to deepen biogeochemistry the process of Changjiang estuary and inner shelf of the East China Sea of phosphorus rich understanding of biogeochemical cycling of biogenic elements on high turbidity estuary. The main results are as follows: 1. along the Yangtze River Estuary salt Gradient of collected surface water and suspended particulate matter samples (June 2011), the distribution of dissolved phosphorus and particulate phosphorus, mixing behavior and migration were studied. Water elutriation particles are divided into 5 grade, with improved SEDEX (sequential extraction method) analysis method was used to determine the different particulate phosphorus form, was found between different forms of phosphorus, especially dissolved phosphorus and phosphorus can be activated particles of exchangeable phosphorus (Exchangeable-P, Ex-P), organic phosphorus (Organic-P, Or-P) and iron bound phosphorus (Fe-bound, P, Fe-P) has strong mutual transformation between detrital phosphorus. (Detrital-P, De-P) and Or-P is the most two kinds of phosphorus forms in suspended particulate matter, the content of total particulate phosphorus accounted for 43.9% and 26.1%.De-P increases with the diameter of the particle, and the content of Or-P and other forms of phosphorus with the increasing of the size of particles .8 decreased M component is considered to be the "real particle suspension", this study shows that "carry real floating" particles of bioavailable phosphorus (Bioavailable-P, BAP; Ex-P, Or-P and Fe-P and the flux is 0.21 * 104tPyr-1), the total biomass flux can be accounted for P/SSA the use of 29%. fine particles of phosphorus in value is very low, indicating that these particles of phosphorus in the preservation of low efficiency. The surface sediments of Yangtze Estuary grading of suspended particulate matter in the De-P/SSA and Fe-P/SSA and the mouth of the Yangtze River basic, Au-P (authigenic apatite, Authigenic-P / SSA (Re-P) and refractory organic phosphorus, Refractory-P /SSA) from suspended particulate matter to the sediments decreased slightly, while Ex-P/SSA and Or-P/SSA in surface sediments was significantly lower than that of suspended particles, further show that the particles of different forms of phosphorus with suspended particles in estuarine sedimentation in the process is different .2. determination of particle behavior of phosphorus form in the sediment samples and sediment samples grading grading of adsorption kinetics and isothermal adsorption experiments, experimental adsorption characteristics affected by salinity. The results showed that the content of De-P in sediments is the most abundant content, followed by biological Or-P. fine particle size in the sediment phosphorus availability is much higher than that of Sandy that fine sediment, particles of phosphorus from the sediment to the overlying water or surrounding interstitial water release plays a leading role. The analysis found from adsorption isotherms from the same sampling stations of the graded sediments obtained, zero equilibrium phosphate concentration in different particle size of sediment corresponds to the value of (zero equilibrium phosphate concentration, EPCo) is close (fine sand, silt and coarse silt and sand were 55.0,54.9,51.7 and 49 gL-1). The adsorption capacity of sediments to phosphate, adsorption rate The adsorption rate and the value (native adsorbed phosphorus, NAP) are largely controlled by the particle size, the adsorption capacity of the total size of 32 mu m sediment value is 6 times the sediment grain size of 32 m. The adsorption capacity of fine-grained sediments with high phosphate, Inner Shelf mud areas of the East China Sea plays an important role in the regulation of phosphate concentration in the overlying water and interstitial water of the Yangtze River at the same time, the input of phosphate is an effective collector, can reduce the East China Sea continental shelf suffered eutrophication risk.3. through the analysis of precipitation of phosphorus and sediment characteristics of sediments in the Changjiang Estuary and its adjacent the inner shelf of the East China Sea surface, the distribution of phosphorus, bioavailability and preservation. The results showed that the total phosphorus in the surface sediments (Total, phosphorus, TP) in the range of 15.0-21.4 molg-1, the highest value appeared in.De-P, near the entrance of Re-P, Or-P, Au- P, Ex-P and Fe-P's contribution to TP were 55.6%, 17.8%, 16.1%, 5.5%, appeared in the Yangtze River Estuary and Yangtze Estuary shelf region.Or-P in the Yangtze River Estuary and Zhejiang Fujian coastal mud area with high content of area 2.5% and the highest content of 2.5%.De-P, and SSA and TOC silt, similar ratio increases. The distribution characteristics of.Re-P are mainly distributed in the near estuary and Zhejiang Fujian coastal areas.De-P/SSA and TOC/SSA with SSA decreases, and the ratio of Or-P/SSA was increased with the SSA basic does not change, show that Or-P has reached the adsorption desorption equilibrium of.TOC and total organic phosphorus on the mineral surface (Total organic-P, Re-P and TOP; Or-P) and the ratio (average ~ 84) lower than the ratio of Redfield, showed that the organic matter in the Changjiang Estuary and adjacent to the inner shelf of the East China Sea mobile mud area has been fully remineralization. And the ratio of TOC/Or-P (72~422, average value is 188) is relatively high, that in organic The process of remineralization of Or-P prior to the TOC sample three column sediments collected from the study area determination of mud area and non mud area decomposition.4. in the form of phosphorus, and combined with the grain size composition, activity of 21oPb, TOC and stable isotope (813C), Fe2+ and Mn2+, and interstitial water the overlying water in the PO43- and NH4+ parameters such as pore water, discusses the migration under different sedimentary environment of phosphorus transformation, diagenetic processes and preservation characteristics. The results show that the Yangtze River affected by terrestrial input, in the Yangtze River Estuary and East China Sea Mud Area on the inner shelf of the 12 and 31 columns in TP and terrigenous sediments phosphorus forms especially the content of De-P is much higher than in the non Mud Area No. 33 stations. Because the mixing effect of the mobile mud layer, column 31, 210Pbexcess in the sediment, the median diameter (Median grain, size, MGS) and various forms of phosphorus (Ex-P, Or-P, Au-P, Re-P and De-P) The content remained almost unchanged in the upper sediment column within a certain depth range, and lower distribution are obviously different; and 210Pbcxcess 12 column sediments and non active phosphorus forms (such as De-P, Au-P and Re-P) were kept constant throughout the depth range. The domain sediments in this area Or-P Fe-P and the transformation to Au-P. The study also found that the sediment in the mud area No. 31 cylinder is the gap of phosphate in water source, while in the non Mud Area No. 33 column sediments act as pore water phosphate sink.5. of the collected in the East China Sea shelf sediments sediments the particle size, SSA, TOC, C/N ratio, carbon isotope and particulate phosphorus analysis, discusses the feasibility of detrital phosphorus as Yangtze River flood historical reconstruction index. The study found that the peak value of De-P appeared in 1850s, 1860s, 1900s, 1920s, 1 950s, 1980s and 2000s, consistent with the flood recorded in Yangtze River Basin in 200 years. The study also found that there is a good corresponding relationship between the De-P and the mouth of the Yangtze River in 1981 and 1998 occurred in two caused by large floods of the Yangtze River and the two extreme anoxic events, extreme anoxic events also has been confirmed by Mo/Al further. The analysis shows that the 1950s De-P and the Yangtze River Basin, the extreme flood events occurred in 2000s and 1980s and flood related climatic events, such as the strengthening of the El Nino Southern Oscillation (ENSO El, Nino-Southern Oscillation), the weakness of the East Asian summer monsoon (EASM, East Asian summer Monsoon) and Pacific interannual oscillation (PDO, Pacific ten Decadal Oscillation) the warm phase has a better correlation, indicating that De-P might become an alternative index.6. indicator associated with extreme flood events and climate events along the long river estuary salinity gradient were collected The surface water samples at 7 stations (July 2013), the circulation status of oxygen isotope tracer analysis of phosphate phosphate in the Changjiang Estuary. The results show that the mouth of the Yangtze River water can be mixed with the model of two end of the Yangtze River water and the East China Sea were well described. On this basis, this study established phosphate across 818Op yuan mixed line and mixed equilibrium line, and circulation of phosphate was studied, found in the Yangtze River water end, phosphate cycling process has not experienced strong, mainly affected by physical mixing effect; biological cycle process with phosphate turbidity maximum is also weak, deep water from other sources of phosphate changed the region originally 18Op. The characteristic value; and in the feather striker, 5 18Op measured value is almost equal to its equilibrium value, has been showed that phosphate cycling process fully.

【學位授予單位】：中國海洋大學
【學位級別】：博士
【學位授予年份】：2015
【分類號】：P736.4

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