Institutional Repository of Key Laboratory of Marine Ecology & Environmental Sciences, CAS
|Place of Conferral||中国科学院海洋研究所|
|Keyword||药物活性化合物 分布特征 源解析 生态风险 胶州湾|
不同海洋环境中PhACs的组成由于药物本身的性质、用途和用量而差异较大。胶州湾沉积物中PhACs浓度为3.62-21.4 ng/g，降雪、海水中PhACs浓度分别为52.8-1616 ng/L和23.6-217 ng/L。海水中主要为为金刚烷胺（24.7 ng/L）、林可霉素（8.55 ng/L）、酮基布洛芬（8.30 ng/L）和四环素（7.48 ng/L）；降雪融水中主要为四环素（125.8 ng/L）、3-去乙酰基头孢噻肟（17.7 ng/L）、罗硝唑（8.79 ng/L）和醋酸曲安西龙双（2.84 ng/L）；沉积物中主要为酮基布洛芬（2.49 ng/g）、土霉素（1.00 ng/g）和罗红霉素（0.97 ng/g）。虽然不同环境中PhACs的组成差异明显，但抗生素均为占比最大的种类，且这些抗生素类药物都是我国临床医疗和畜禽养殖常用药物，与我国的PhACs的生产和使用特点基本一致。
胶州湾PhACs海水及沉积物水平分布总体呈现湾内从东向西逐渐减少，湾内高于湾外的特征，且PhACs的总浓度的等值线均几乎与海岸线平行。胶州湾西部PhACs含量（平均值：38.4 ng/L；5.06 ng/g）明显低于受人为活动影响严重的东部（平均值：116 ng/L；14.2 ng/g）。
In recent years, a variety of novel zoonotic diseases, such as SARS, avian influenza and HFMD (hand-foot-and-mouth disease), have emerged, and the aging of the global population undergoes constant exacerbation. To face this situation, an increasing number of novel pharmaceutically active compounds (PhACs) are involved in accelerating research and development, production and application. As the types and consumption of PhACs increase each year, most drugs inevitably enter the environment. Their strong bioactivity, persistence and bioaccumulation characterize the drugs to be significantly influential on human health and the ecological environment. The impact of PhACs entering oceans on marine ecosystems is immeasurable, and the different impacts of PhACs on marine environments are also increasingly highlighted. For this reason, PhACs are recognized as an important new type of marine organic pollutant. In the meantime, the potential ecological risks in marine environments, especially offshore environments, and the prevention and control of PhAC pollution have been popular topics that have been increasingly investigated by scholars abroad and at home. Therefore, systematic studies on PhACs in marine environments are of great scientific significance and application value. In this study, the seawater, sediment and atmospheric sedimentation (snow) of Jiaozhou Bay (JZB), a model bay that is influenced by both human activities and natural factors, were selected as the primary study objects. By high throughput screening and the combination of the relationships between PhACs and the relevant environmental factors, a systematic exploration was applied to study the occurrence, biogeochemical distribution characteristics, sources, pollution trends, environmental control factors and potential ecological risks of PhACs in the environment of JZB. A series of new results and understandings have been obtained as follows:
1. In these three media—seawater, sediments and atmospheric sedimentation (snow) of JZB—PhAC contamination was found to different extents, suggesting a wide presence of PhACs in the environment of JZB. The PhAC distribution in the seawater of JZB is mainly guided by a means of “sources and channels—the hydrodynamic process of seawater”, in addition to the self-degradation factors of the compounds. Namely, the distribution of the compounds is formed by a passive diffusion mode. In contrast, in the sediments, the PhAC distribution is regulated and controlled by the path of “sources and channels—hydrodynamic process of seawater-composition of sediments”; that is, the distribution is shaped by a “passive diffusion-active adsorption” composite pattern.
Using high-throughput screening and advanced mass spectrum analysis technology, a total of thirty-six PhACs were detected in seawater, of which seventeen were first reported in seawater; thirty-eight targeted compounds were found in snow, and all of them were disclosed in a scientific journal for the first time, while the study was the first report concerning PhAC contamination in snow; moreover, twenty-five target PhACs were verified in the sediments of JZB, of which ten were discovered for the first time in marine sediments.
Among the three environmental media above, the sediments were found to contain the highest PhAC occurrence concentration, with a value of 3.62-21.4 ng/g, followed by snow and seawater, whose PhAC concentrations were 52.8-1616 ng/L and 23.6-217 ng/L, respectively. The occurrence of different types of PhACs in the marine environment varies greatly depending on the application range, utilization purpose and physicochemical properties of the drug itself. Of the PhACs remaining in the seawater, the preponderant kinds include tetracycline (7.48 ng/L), carprofen (8.30 ng/L), lincomycin (8.55 ng/L) and amantadine (24.7 ng/L). In the snow, the primary kinds were triamcinolone diacetate (2.84 ng/L), ronidazole (8.79 ng/L), desacetylcefotaxime (17.7 ng/L) and tetracycline (125 ng/L). In the sediments, the major PhACs included roxithromycin (0.97 ng/g), oxytetracycline (1.00 ng/g) and ketoprofen (2.49 ng/g). Despite a significant difference in the composition of PhACs in distinct environmental media, antibiotics and hormones generally dominate in environments because they are frequently used in clinical medical care and livestock and poultry farming in China. This result is overall consistent with the characteristics of PhAC production and utilization in China.
The PhAC distribution presents a gradual decrease in density from east to west, where the areas inside the bay have a higher concentration than the areas outside the bay. Meanwhile, the isopleth of the total PhAC concentration appears to be practically parallel to the coastline. In addition, it was noted that the PhAC concentration in western JZB (38.4 ng/L; 5.06 ng/g) was obviously lower than that in eastern JZB (116 ng/L; 14.2 ng/g), where the impact of human activities is severe.
Regarding the seawater environment, PhACs are positively correlated with nutrients, and both display a distribution pattern highly similar to each other (the correlation factors r being larger than 0.9). Of the nutrients, phosphates were proven to exhibit a significantly positive correlation with 16 PhACs (P<0.01). This finding indicates that phosphates may harbor similar sources. The content of PhACs is negatively correlated with salinity. Low salinity signifies a high input volume of fresh water, but the PhAC concentration in seawater increases when the fresh water input increases. The correlation indicates the “single-diffusion” passive mode of the PhAC distribution in seawater, which is managed by the “hydrodynamic process”.
Regarding the sediments, the PhACs here are significantly positively correlated with TOC (P<0.01, r=0.932). Organic matter plays a vital role in adsorbing PhAC contaminants. Similarly, a significantly positive correlation was noted between PhACs and clay (P<0.01, r=0.896). The smaller the diameter of sediment grains is, the larger the total surface area, and the stronger the adsorption action, which is also more favorable for the enrichment of PhACs. The PhAC distribution in sediments shows an active mode of “diffusion-adsorption”, where it is jointly regulated by the “hydrodynamic process” and “sediment adsorption”.
2. Land-based input was identified as the main source of PhACs in the JZB. River input was found to be the major land-based input of the PhACs in this area, which was mainly derived from eastern rivers (the sewage discharge of the Licun River, in particular). Atmospheric sedimentation may also be a non-negligible, important source of the PhACs in JZB. The PhACs were found to harbor potential toxicity risks for some biological groups in JZB.
According to the systematic analyses on the relationship between the PhACs in the JZB seawater and key environmental factors, phosphate was considered a potential indicator to prompt the distribution characteristics of PhAC concentrations in JZB seawaters, while coprostanol was considered a possible indicator of the distribution of the concentration of PhACs in the JZB sediments. The input of rivers in the eastern part of the bay, especially the waste discharge from the Licun River, forms the prime source of PhACs in this region. As the bay has been severely contaminated by human excreta, domestic sewage and medical wastewater from the eastern coastal region are likely to be the main sources of the PhACs in JZB.
The investigation of the PhAC transmission route suggested that in atmospheric sedimentation, in addition to the PhACs of salbutamol, ronidazole, oxolinic acid and a few other kinds that are from remote transmission, most of the PhACs come from local pollutant emissions. In short, for PhACs, the discharge of local contaminants contributes more than remote transmission. Of the PhACs in snow, drugs for humans only, animals only and both humans and animals account for 40.1%, 46.0% and 13.8%, respectively. The high amount of veterinary drugs in the atmosphere may be associated with the persistent landfill deposition of animal droppings.
The impacts of PhACs on aquatic organisms such as invertebrates, algae, fishes and plants in JZB were noted to vary greatly. Though unlikely to bring potential risks to fishes and plants (RQ<0.01), the PhACs in seawater, sediments and atmospheric sedimentation present a much less optimistic picture for invertebrates and algae. Tetracycline, ofloxacin, lincomycin, roxithromycin, clindamycin, oxytetracycline, and sulfamethoxazole posed high or medium risks to invertebrates and algae.
|MOST Discipline Catalogue||理学::海洋科学|
|Table of Contents|
第1章 绪论. 1
1.1 药物活性化合物（PhACs）概况. 1
1.1.1 研究背景. 1
1.1.2 环境中 PhACs的来源. 2
1.1.3 环境中 PhACs的分析方法比较. 5
1.1.4 PhACs在海洋环境中的研究进展和存在的问题. 7
1.2 论文的选题意义及主要研究内容. 9
1.3 研究区域概况及研究方法. 11
1.3.1 研究区域概况. 11
1.3.2 站位设置及采样. 12
1.3.3 分析方法. 15
1.3.4 质量控制（QA/QC）. 25
2.1 胶州湾海水中PhACs的组成与分布. 28
2.1.1 胶州湾海水中PhACs的构成与浓度水平. 28
2.1.2 胶州湾海水中PhACs的分布特征. 33
2.2.1 PhACs与海水环境因子的耦合关系. 37
2.2.2 海水中PhACs的生态风险评估. 43
2.3 胶州湾沉积物中PhACs的组成与分布. 45
2.3.2 胶州湾沉积物中PhACs的分布特征. 49
2.4 沉积物中PhACs环境生物地球化学特征. 52
3.1 降雪中PhACs的组成特征. 67
3.1.2 非甾体抗炎药（NSAIDs）. 71
3.1.3 激素. 72
3.1.4. 其它药物. 72
3.2 来源解析. 73
3.2.1 路径来源分析. 73
3.2.2 组成来源解析. 78
3.4 本章小结. 80
第4章 结论与创新. 82
4.1 结论. 82
4.2 创新点. 85
致 谢. 99
|彭全材. 胶州湾典型药物活性化合物(PhACs)的环境生物地球化学特征解析[D]. 中国科学院海洋研究所. 中国科学院大学,2020.|
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