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类型 基础研究 预答辩日期 2018-03-09
开始(开题)日期 2015-06-24 论文结束日期 2017-11-13
地点 东南大学(四牌楼校区李文正楼北312) 论文选题来源 国家自然科学基金项目     论文字数 8 (万字)
题目 挥发性组分检测及在健康评测中的应用研究
主题词 挥发性标志物,孤独症儿童,纳米纤维固相萃取,分析应用
摘要 随着现代分析技术的进步,检测各型样品中微量、痕量挥发性组分的需求日益增加。尤其是在生命健康领域,样本的挥发性组分通常反映了更多的疾病和健康信息。由于无创伤样品(唾液、尿液、呼吸气体等)的收集容易被受试者尤其是儿童接受,近年来通过分析无创样品中挥发性组分进行多种癌症、糖尿病等早期诊断研究成为热点。然而,由于样本基质复杂,挥发性组分具有种类多、含量极低、沸点低、嗅阈值低(PPb级)、化学活性强、稳定性差等特点,对目标物的萃取面临诸多挑战,是国内外公认的难题。目前最常用的萃取方法是顶空固相微萃取法,但该方法存在诸多不足之处,如萃取头种类较少,并且由于吸附剂数量较少且不能调整,限制了检测范围。因此,如何萃取样品中挥发性组分、提高检测灵敏度仍然是分析工作中的重点和难点。 本论文的研究特点是以检测和评价与人体健康状况相关的无创样品中生物标志物为目标,采用纳米纤维固相萃取技术(Packed-fiber solid-phase extraction,PFSPE),着重对挥发性组分的浓缩进行研究,以应用为目的带动不同纳米纤维材料的制备、表征及对目标物的吸脱附性能研究。本文不仅研究了纳米纤维对挥发性气体萃取的性能,并用于无创生物样本中挥发性和非挥发性生物标志物的分析及人群样本检测,如首次证明了孤独症儿童尿液中挥发性脂肪酸的水平偏高;探讨了对挥发性精油的提取效果,同时也将PFSPE应用于食品分析领域。主要工作内容是针对挥发性组分含量低、难以萃取的问题,根据目标物的性质制备不同的纳米纤维并表征,将其作为固相萃取介质,进行目标物的分离和富集功能,主要进行了以下几方面的研究内容: 第一,进行纳米纤维对挥发性有机物(VOCs)吸脱附性能研究,发现纳米纤维在挥发性组分萃取中具有选择性、热解析性、吸附平衡性、温敏性及再生性等特点。 第二,初步建立纳米纤维辅助的顶空固相微萃取技术;利用新型纳米材料作为待测样品中挥发性组分的富集和传递媒介,结合已有的成熟的固相微萃取技术,巧妙地将NFSPE和SPME相结合,使目标物的检测信号几十上百倍的增加,创造了更高效的挥发性组分样品前处理体系。 第三,以挥发性的短链脂肪酸为目标物,建立了基于PFSPE技术结合GC-MS的检测方法,并用于分析孤独症儿童人群的尿液样本,首次证明了ASD儿童尿液中SCFA水平偏高;实现了PFSPE技术在检测生物无创样本挥发性成分的应用,使得新方法有可能被用于孤独症儿童尿液中短链脂肪酸浓度的临床监测和实验调查。 第四,使用PFSPE样品前处理技术及其可批量化处理的优势,利用新建立的方法检测了4-5岁超重儿童尿液中挥发性脂肪酸的水平;首次同时检测了超重儿童的唾液和尿液中的皮质醇和可的松水平,并分析了目标物与体重和家庭饮食等因素的相关性,为控制和干预儿童体重提供数据支持和理论参考。 第五,探讨了纳米纤维对洋葱中挥发性硫化物的吸附解析效果,与现有的吸附材料相比具有较好的吸附性和解析性等优点;接着进行了纳米纤维提取洋葱精油的研究,实验证明该洋葱精油具有较好的体外抗氧化效果。 第六,最后探讨了测试新技术在检测食品中其它目标物的应用。首先,建立了基于PFSPE技术的检测牛奶中氯霉素的分析方法,结果表明该技术具有成本较低、耗时较短、有机溶剂用量小等优点,在实验中还实现了小批量化处理(12个),为进一步更大批量化处理样品提供了依据。然后,探讨了蓝光光盘薄膜作为一种新型的通用生物芯片基底材料,具有无荧光背景、表面活化无需设备且高效易行等优点,可实现操作简单的检测分析试验。结合PFSPE技术和新的基底材料,这对制造一次性生物芯片检测低浓度的生物标志物的生物医学装置具有很大的潜在作用和参考价值。 挥发性组分的检测对在人体健康评测中具有重要意义,也可为营养饮食的干预效果提供生化指标。本研究结果表明,孤独症儿童和超重儿童无创样本中挥发性脂肪酸的检测在评价健康方面起着重要作用,是重要的生物标志物。在对挥发性目标物的检测中,PFSPE技术实现了对挥发性组分的高效萃取,仅用几毫克的纳米纤维和一百微升的洗脱剂,即可实现对多种实际样品中目标物质的高效提取,显著提高了目标物信号,该技术可广泛地应用于涉及分析测试的多个领域。纳米纤维的独特性能,在其作为挥发性组分的固相萃取介质方面对人体健康评测方面具有较高的研究价值和很大的应用及推广潜力。
英文题目 DETECTION OF VOLATILE COMPONENTS AND APPLICATION TO EVALUATION OF HEALTH
英文主题词 Volatile markers; children with Autism Spectrum Disorder; Nanofiber solid-phase extraction; Analysis and application
英文摘要 With the development of the modern analysis technology, the demand for the detection of trace amount of volatile components in various types of samples is increasing. Especially in the field of health, the volatile components from samples often reveal much more information on the disease and health. Due to the easy collection of non-invasive samples, such as saliva, urine, respiratory gases, it is recently becoming a hot issues to analysis the volatile components from non-invasive samples for the early diagnosis of cancer, diabetes and other disease. However, because of the complex sample matrix, volatile components own many characteristics, such as much variety, low content, low boiling point, low olfactory threshold (PPb level), strong chemical activity and poor stability. Therefore, the extraction of these targets is facing with many challenges and recognized as very hard problem in the world. At present, the most common extraction method is headspace solid-phase microextraction, while there are many shortcomings, such as fewer types of extraction needles, and limited detection range due to the small amount of adsorbent and unable to be adjusted. Therefore, how to extract the volatile components from complex samples and improve the method sensitivity is still a key and difficult task in the field of analysis. In this work, we focused on the detection and evaluation of biomarkers in noninvasive samples related to human health, utilizing the packed-fiber solid-phase extraction (PFSPE) method to concentrate volatile targets. So, the purpose of application promotes the preparation and characterization of different nanofibers, and the study on adsorption and desorption properties for different targets. Not only were the extraction performance of nanofibers for volatile compounds studied but also the analysis of volatile and non-volatile biomarkers in non-invasive biological samples, children’s saliva and urine samples, was conducted. It is the first time to reveal that the volatile fatty acids in the urine samples from children with Autism Spectrum Disorder (ASD) has higher level than that of normal children. Also, the extraction of volatile essential oils using nanofibers was explored and the PFSPE was applied to the field of food analysis. The main content of the work is to deal with the problem of low content and difficult extraction for the volatile components. According to the nature of these targets, different nanofibers were prepared and characterized, then used as solid-phase extraction medium to separate and enrich the targets. The details are as follows: Firstly, the adsorption and desorption properties of nanofibers for the volatile organic compounds (VOCs) were investigated. The results show that the nanofibers own the characteristic of selectivity, thermally desorption, adsorptive balance, temperature sensitivity and regeneration for the extraction of volatile components. Secondly, the nanofiber-assisted headspace solid-phase microextraction was initially established. The new nanomaterials prepared as the enrichment and transmission medium for the volatile targets was combined with the traditional solid-phase microextraction technology, which is SPME assisted with NFSPE. The results displayed the target signal detected increases hundreds of times and creates a more efficient system of sample pre-treatment for the volatile components. Thirdly, the method of NFSPE coupled with GC–MS for the determination of volatile short-chain fatty acids (SCFAs) in children’s urine was developed and used to analyze urine samples from children with ASD. The results first demonstrated that the children with ASD have higher SCFAs level. The application of new method to the detection of volatile components in biological non-invasive samples has the potential to clinical monitoring and experimental investigation for the concentrations of SCFAs in urine from children with ASD Fourthly, using PFSPE method and its advantage of batch processing, the level of volatile fatty acids in the urine samples from overweight children aged 4-5 years was determined by the new method established. It’s the first time that, the biomarkers of cortisol and cortisone in the saliva and urine samples from overweight children were simultaneously detected, and the correlation between the targets and body weight and family diet habit was analyzed, which provided the control and intervention of children’s weight with the data support and theoretical reference. Fifthly, the adsorption and desorption performance of nanofibers on the Volatile Sulfur Compounds (VSCs) in onion was studied, and then the research on the extraction of onion essential oil by nanofibers membrane was conducted. Compared with the existing adsorbents, the nanofibers own better adsorption and desorption properties on VSCs. Experimental result shows that the onion essential oil extracted by nanofibers has good antioxidant effect in vitro. Lastly, using the new testing technology to detect other targets in food samples is discussed. A new analytical method based on PFSPE for the determination of chloramphenicol in milk was established. Its results show that the method has the advantages of low cost, short time and small dosage of organic solvents, and the mass processing of 12 samples was realized in the experiment which suggested the potential of high-through pre-treatment. Additionally, Blu-ray discs (BD) was explored as a new universal biochip substrate, which has no fluorescence background, no equipment needed for the surface activation, and is easy and efficient to operate. Coupled PFSPE method with the new substrate materials, there is a great potential to the biomedical device for the detection of low concentrations of biomarkers with disposable biochips. The detection of volatile components for the evaluation of human health is of great significance, also suggests the biochemical indicators for the nutrition intakes and diet interventions. This study displays that the volatile fatty acids are important biomarkers. It plays an important role in the evaluation of health to detect these biomarkers in non-invasive samples from children with ASD and overweight children. When determining the volatile targets, PFSPE technology achieves the efficient extraction and improve the target signal of the volatile components just using a few milligrams of nanofibers and one hundred microliters of eluent. The technology can be widely used in many fields involving analysis and testing. As the medium of solid-phase extraction on volatile biomarkers, the electrospun nanofibers with unique properties offer preferable research value and great potential of the application and promotion in the evaluation of human health.
学术讨论
主办单位时间地点报告人报告主题
东南大学学习科学中心 2016年4月20日9:30 李文正楼北312会议室 崔兴然 面向转化医学的动态生医指标体系
Department of Chemistry, Simon Fraser University January 13, 2017, 3:30pm Shrum Science Centre, C9001 Dr. John Ripmeester Structure, dynamics and guest-host
Department of Chemistry, Simon Fraser University February 1, 2017, 3:30pm Shrum Science Centre, C9001 Dr. Zhenfeng Xi, Peking University Spiro metalla-aromatics: Synthesis and Characterization
Department of Chemistry, Simon Fraser University February 22, 2017, 3:30 pm Shrum Science Centre, C9001 Dr. Bo Zhang, University of Washington Electrochemistry of single nanoparticles and molecules
2017 100th Canadian Chemistry Conference and Exhibition May 29, 2017,PM 2:00 Renaissance Toronto Downtown Hotel, Room 205C Dr. Hogan Yu Quantitative Electrochemistry at Molecular Interfaces: Modulation of Monolayer Structure and Hostguest Chemistry
东南大学学习科学中心康学军教授科研组 2013年12月15日9:30 李文正楼北312会议室 褚兰玲 静电纺丝制备纳米纤维及在食品检测和精油提取中的应用
东南大学学习科学中心康学军教授科研组 2014年12月15日9:30 李文正楼北312会议室 褚兰玲 Tenax吸附材料与PS-AR纳米纤维对唾液中挥发性成分HS-SPME的对比
东南大学学习科学中心康学军教授科研组 2015年3月14日9:30 李文正楼北312会议室 褚兰玲 Overweight and obese children of cortisol
Dr Yu’s Group, Department of Chemistry, Simon Fraser University 2016年9月16日上午9:30 Room: C7080 褚兰玲 Application of electrospun nanofibers to solid phase extraction(SPE)
Dr Yu’s Group, Department of Chemistry, Simon Fraser University 2017年8月14日上午9:30 Room: C7080 褚兰玲 Blu-ray discs as universal biochip substrates: lithography-free surface activation and assay application (DNA hybridization)
东南大学学习科学中心 2014年5月18日 李文正楼北335报告厅 Prof. Hideaki Koisumi Research and Development toward Human Security and Well-Being
东南大学学习科学中心 2016年2月25日上午8:45 榴园宾馆新华厅 李德毅院士 脑认知形式化
     
学术会议
会议名称时间地点本人报告本人报告题目
2015全国现场检测仪器及技术暨全面应用技术解决方案研讨会 2015年1月22-24日 中国海口 一种可在线快速前处理技术——纳米纤维固相萃取
第三届全国静电纺丝技术与纳米纤维学术会议 2015年9月24-25日 中国青岛 电纺纳米纤维在食品分析和洋葱油提取中的应用研究
2016高效液相色谱和色谱技术国际研讨会 2016年3月14-15日 英国伦敦 聚乙烯吡咯烷酮 - 聚苯乙烯复合纳米纤维与高效液相色谱结合分析几种极性分子的应用
     
代表作
论文名称
Adsorption/desorption performance of volatile organic compounds on electrospun nanofibers
Extraction of onion (allium cepa) essential oil by polystyrene nanofibrous membranes
Detection of β-agonists in pork tissue with novel electrospun nanofibers-based solid-phase extractio
. Comparison of Adsorption/Desorption of Volatile Organic Compounds (VOCs) on Electrospun Nanofibers
 
答辩委员会组成信息
姓名职称导师类别工作单位是否主席备注
孙桂菊 正高 教授 博导 东南大学 营养与食品卫生学
卢青 正高 教授 博导 东南大学
葛卫红 正高 主任药师 硕导 南京鼓楼医院
苏二正 正高 教授 博导 南京林业大学
祁争健 正高 教授 博导 东南大学
      
答辩秘书信息
姓名职称工作单位备注
张亚贤 其他 讲师 东南大学