本文關(guān)鍵詞： 有害藻華治理 改性粘土 營養(yǎng)元素 毒素 生態(tài)效應(yīng)　出處：《中國科學(xué)院研究生院（海洋研究所）》2014年博士論文　論文類型：學(xué)位論文

【摘要】：隨著人類活動增多、氣候變化等因素影響，近年近岸有害藻華的暴發(fā)頻率和規(guī)模不斷增加，，其引起的海洋生態(tài)問題日益凸顯。改性粘土治理有害藻華是國際上推薦的野外應(yīng)急治理方法之一。本論文通過室內(nèi)實驗，開展改性粘土治理不同藻華生物的長期環(huán)境化學(xué)效應(yīng)的研究，針對有害甲藻藻華、硅藻藻華自然消亡過程中營養(yǎng)鹽循環(huán)特性及改性粘土絮凝后所引起水質(zhì)營養(yǎng)環(huán)境的差異特征以及改性粘土治理有毒藻華過程中對水和沉積物環(huán)境因子、藻毒素的影響研究，結(jié)合分析大量粘土絮凝有害藻華機(jī)理、元素生物地球化學(xué)循環(huán)、粘土材料結(jié)構(gòu)特性等研究文獻(xiàn)，獲得以下幾方面的階段性成果： (1)改性粘土治理方法能夠高效絮凝去除高密度有害藻華生物P. micans、P.donghaiense、S. costatum、A. tamarense，由于硅藻細(xì)胞外殼含有大量硅元素，與粘土中鋁元素易發(fā)生離子置換，外加硅藻細(xì)胞的自沉降特性，所以改性粘土對硅藻去除效率更為顯著，改性粘土通過“互蔭”效應(yīng)、改變營養(yǎng)結(jié)構(gòu)和膠體緩沖體系等方式影響有害藻華生物的微生境，顯著影響其細(xì)胞代謝合成不同的熒光物質(zhì)，單位藻細(xì)胞有機(jī)氮和磷短期內(nèi)顯著升高，改性粘土治理方法有效抑制了有害藻華生物二次增殖。 (2)自然消亡過程中藻源有機(jī)物在降解過程中會釋放大量營養(yǎng)物質(zhì)，這些營養(yǎng)物質(zhì)可為二次藻華暴發(fā)提供物質(zhì)基礎(chǔ)，改性粘土治理方法在除藻的同時有效地改善了水質(zhì)環(huán)境，水體中TN、TP大幅降低，且未出現(xiàn)二次釋放。實驗?zāi)┢诤Ｑ笤自錚. micans改性粘土絮凝后TP約去除39.28%~42.47%，TN約去除26.22%~29.93%；東海原甲藻P. donghaiense改性粘土絮凝后TP約去除51.39%，TN約去除17.24%；中肋骨條藻S. costatum改性粘土絮凝后TP約去除93.36%%~93.60%，TN約去除53.75%~71.95%；塔瑪亞歷山大藻A. tamarense改性粘土絮凝后TP約去除42.86%~56.30%，TN約去除20.72%~35.53%。 (3)改性粘土改變了水體中營養(yǎng)元素的濃度、形態(tài)比例以及元素循環(huán)過程，磷酸鹽和硅酸鹽以直接吸附影響為主，而溶解態(tài)無機(jī)氮以時間累加的間接效應(yīng)為主，有效地降低了水體營養(yǎng)程度，由于不同營養(yǎng)元素的去除機(jī)理和速率有所不同（無機(jī)營養(yǎng)元素轉(zhuǎn)化速率依次為v(NO3--N)v(DIP)v(NO2--N)v(NH4+-N)），造成營養(yǎng)結(jié)構(gòu)發(fā)生改變，改性粘土促進(jìn)了藻華生物對無機(jī)態(tài)營養(yǎng)物質(zhì)的吸收，同時加快了顆粒態(tài)營養(yǎng)物質(zhì)的沉降速率，水體中TDN/TDP比值顯著增加（100），形成極度磷限制環(huán)境從而破壞了藻細(xì)胞二次增殖所需的適宜營養(yǎng)條件。 (4)改性土治理方法形成的藻土有機(jī)粘土復(fù)合體聚合富集沉降大量有機(jī)氮和有機(jī)磷物質(zhì)進(jìn)入沉積物表層，通過沉積物顆粒、改性粘土顆粒與上覆水環(huán)境的離子交換作用、金屬有機(jī)物螯合作用、沉積物壓實作用等機(jī)制促使?fàn)I養(yǎng)物質(zhì)在月尺度上無法快速解吸或釋放，同時改性粘土具有一定的抗微生物活性特征，減緩了有機(jī)氮、磷的降解，在月尺度上無機(jī)營養(yǎng)鹽濃度未發(fā)生改變，使得這部分有機(jī)物如化石埋賦一樣保存于沉積物中；另一方面，粘土顆粒表面為某些有機(jī)物質(zhì)的聚合反應(yīng)提供反應(yīng)位置和催化中心，改性粘土自身的表面富集和選擇催化特性促使葉綠素a和藻毒素PSTs等活性有機(jī)物質(zhì)轉(zhuǎn)化加速，沉積物中高毒性GTX1和GTX4向較低毒性GTX2和dcGTX3轉(zhuǎn)化，尤其是沉積物-海水環(huán)境中，pH值和氧化環(huán)境在PSTs降解轉(zhuǎn)化過程中起重要作用，毒素由高毒性向低毒性甚至無毒物質(zhì)轉(zhuǎn)化速率顯著加快。 改性粘土治理方法形成的絮體與“海洋雪”具有一定的相似性，但絮體來源、組成、形成狀態(tài)有所不同。由于改性粘土添加是人為突發(fā)過程，對于自然水體而言這一過程如海底火山噴發(fā)般能突然改變區(qū)域微生物活性和元素地球化學(xué)循環(huán)過程。所以，針對特定水體條件和藻種，在篩選改性粘土用量和去除時應(yīng)深入研究生態(tài)效應(yīng)信息，在大規(guī)模施行前需要進(jìn)行長時間尺度生態(tài)效應(yīng)研究以保證安全使用這一治理方法。盡管本課題組針對改性粘土治理方法野外應(yīng)用積累了大量經(jīng)驗，但是我們依然建議應(yīng)該對其造成的環(huán)境影響需要慎重評估。研究改性粘土治理有害藻華后期營養(yǎng)元素的生物地球化學(xué)規(guī)律，對于正確認(rèn)識海洋中的有害藻華消亡及有害藻華治理的后期生態(tài)效應(yīng)都有重要意義。
[Abstract]:With the increasing human activities, climate change and other factors, in recent years, the coastal harmful algal blooms outbreak frequency and increasing scale, marine ecological problems caused by the increasingly prominent. The modified clay treatment of harmful algal blooms is one of the internationally recommended field emergency treatment method. This paper through indoor experiments, research on long-term effects of environmental chemistry clay treatment of different algae organisms, the harmful dinoflagellate algae, differences in the characteristics of water quality and nutrition environment caused by modified clay flocculation nutrient cycling characteristics of diatom bloom in the process after the demise of the natural and modified clay treatment of toxic algal blooms in the process of water and sediment environmental factors, effects of microcystins combined with the analysis of a large amount of clay, the flocculation mechanism of harmful algal blooms, the biogeochemical cycling of elements, the study of clay material structure characteristic of literature, acquired the following form Fruit:
(1) modified clay treatment method can remove the high density of harmful algal bloom species P. micans, S. costatum, P.donghaiense, flocculation, A. tamarense, the diatom cells contain a large number of silicon shell elements, and the elements in the aluminum clay prone ion exchange, and the characteristics of diatom cell death, so the removal efficiency of modified clay on diatom more significantly, the modified clay by "shadow" effect, change the microhabitat of harmful algal blooms biological effects of nutrient structure and colloid buffer system etc., significantly affect the cell metabolism synthesis of different fluorescent materials, unit cell organic nitrogen and phosphorus increased significantly in the short term, the modified clay treatment method can effectively restrain the harmful two biological algae proliferation.
(2) algae source organic natural death process will release a large amount of nutrients during the degradation process, these nutrients can provide the material basis for the two time the outbreak of algal blooms, modified clay treatment method improves water environment effectively while removing algae in water, TN, TP significantly reduced, and did not appear two release. At the end of the experiment Prorocentrum P. micans modified clay flocculation after removal of 39.28%~42.47% TP about TN, about the removal of 26.22%~29.93%; dinoflagellate P. donghaiense modified clay flocculation TP after removal of about 51.39%, about 17.24% TN removal; Skeletonema costatum S. costatum modified clay flocculation TP after removal of about 93.36%%~93.60%, TN about the removal of 53.75%~71.95%; Alexander A. tamarense tajmar algae modified clay flocculation after removal of TP about 42.86%~56.30%, TN about the removal of 20.72%~35.53%.
(3) modified clay changed the concentration of nutrient elements in the water, the proportion of form and element cycle, mainly by direct adsorption effects of phosphate and silicate, and dissolved inorganic nitrogen in the indirect effect time accumulation, effectively reduce the water eutrophication degree, different from the removal mechanism and rate in different nutrient elements (inorganic nutrients conversion rate were V (NO3--N) V (DIP) V (NO2--N) V (NH4+-N)), the nutrition structure changed, modified clay can promote the absorption of algae biological inorganic nutrients, and accelerate the sedimentation rate of particulate nutrients in the water, the ratio of TDN/TDP significantly increase (100), a form of extreme environment to the destruction of phosphorus limited algae cell proliferation two times the optimal nutritional conditions.
(4) organic clay soil algae complex formation of modified soil treatment methods of polymerization enrichment of settlements of a large number of organic nitrogen and organic phosphorus substances into the surface sediments, the sediment particles, modified clay particles and ion exchange effect of overlying water environment, metal organic chelation, sediment compaction and other mechanisms that promote the nutrients in monthly scale not quick desorption or release of the modified clay has certain characteristics of anti microbial activity, slowing the degradation of organic nitrogen, phosphorus, in the month scale inorganic nutrient concentrations did not change, so this part of organic matter such as fossil buried sediments deposited in the same host; on the other hand, the clay particle surface the polymerization of organic materials to provide the location of the response and the catalytic center, modified clay's surface enrichment and selective catalytic properties to chlorophyll a and algal toxins such as PSTs activity of organic compounds The acceleration of the transformation of matter, the high toxicity of GTX1 and GTX4 in sediments from GTX2 to lower toxicity and dcGTX3 transformation, especially the sediment water environment, plays an important role in pH and oxidation environment transformation process in the degradation of PSTs, from high to low toxic poisonous toxins or non-toxic substance conversion rate significantly accelerated.
Floc formation of modified clay treatment method and the "marine snow" has a certain similarity, but the floc origin, composition, form different. Because the modified clay is added for emergency process, for the process of natural water such as a submarine volcano eruption can suddenly change regional geochemical and microbial activity cycle. Therefore, according to the specific conditions of water and algae, we should study the ecological effect of information in the screening of modified clay dosage and removal, before the implementation of the need for research in large scale ecological effect of long time using this method to ensure safety management. Although the research group for the modified clay treatment field accumulation a lot of experience, but we still suggest that environmental impact should be the need to carefully assess students. To study the modified clay treatment of harmful algal blooms late nutrition elements The geochemical law is of great significance to the correct understanding of the extinction of the harmful algal blooms in the ocean and the late ecological effects of harmful algal blooms.

【學(xué)位授予單位】：中國科學(xué)院研究生院（海洋研究所）
【學(xué)位級別】：博士
【學(xué)位授予年份】：2014
【分類號】：X55

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