新型固相電致化學(xué)發(fā)光傳感器的構(gòu)建及其對環(huán)境污染物的檢測
發(fā)布時間：2018-09-05 10:19
【摘要】：電致化學(xué)發(fā)光檢測具有靈敏度高、線性范圍較寬、分析速度快、儀器操作簡單等突出優(yōu)點,因此利用電致化學(xué)發(fā)光檢測可以滿足于環(huán)境中微量乃至痕量污染物的檢測要求。但目前電致發(fā)光傳感器主要集中單一材料從而造成發(fā)光信號不高,難以達到污染物濃度的檢測范圍;傳感器不能夠循環(huán)使用,造成資源浪費等。如何構(gòu)建綠色、無污染、可循環(huán)使用、檢測性能良好的電致化學(xué)發(fā)光傳感器有著重要的意義。本論文以制備固定化的電致化學(xué)發(fā)光傳感器為基礎(chǔ),構(gòu)建了由納米材料所組成的三種電致化學(xué)發(fā)光傳感器,并利用這些固相傳感器來進行快速靈敏地檢測環(huán)境中的五氯苯酚以及重金屬離子的含量。固定化的傳感器可以重復(fù)利用,減少資源的浪費,并為檢測環(huán)境污染物提供了新的方法。具體的研究工作分為以下幾個方面:(1)構(gòu)建了一個石墨烯-金納米簇的新型固相電化學(xué)發(fā)光傳感器,在共反應(yīng)劑過硫酸根的存在下,基于五氯苯酚(PCP)與激發(fā)態(tài)的金納米粒子發(fā)生氧化還原反應(yīng),從而通過淬滅的發(fā)光強度范圍來檢測環(huán)境中五氯苯酚的含量。在此體系中,石墨烯不僅可以增大金納米簇的電致發(fā)光強度,還可為金納米簇提供一個固定化的平臺,從而解決了發(fā)光強度低和不能循環(huán)使用的問題。構(gòu)建的固定化電致發(fā)光傳感器具有非常好的選擇性,在最優(yōu)檢測條件下,對五氯苯酚有著良好的線性范圍(1.0×10-14 1.0×10-10 M)和超低的檢測限(1.0×10-14 M)。本方法避免了復(fù)雜儀器的操作,具有低毒性,可循環(huán)使用,超高靈敏度檢測等優(yōu)點,為在實際水樣中應(yīng)急及在線檢測PCP提供了一個簡單易行、可供選擇的分析檢測方法。(2)利用電化學(xué)沉積的方法一步電沉積鉑納米簇-石墨烯復(fù)合材料于電極上,通過電致化學(xué)發(fā)光的方法,對銅離子進行快速、痕量檢測。由于石墨烯的存在,相比單獨的鉑納米簇,除了表現(xiàn)在電流強度增強、電致發(fā)光信號增大的方面外,其發(fā)光電位和循環(huán)伏安曲線出現(xiàn)的峰位置也出現(xiàn)前移現(xiàn)象。表明在此體系中石墨烯具有降低能壘,加速電子轉(zhuǎn)移的能力。由于石墨烯和鉑納米簇層層沉積擁有較大的比表面積,使溶液中的銅離子容易吸附于修飾電極的表面,使得此傳感器具有較高的靈敏度。該方法對銅離子的最低檢測限為1.0×10-7 gL-1。(3)利用水熱法制備硫化鎘(CdS)納米纖維,并將其用于鉛離子的電致化學(xué)發(fā)光檢測。為了降低納米顆粒所引起的聚沉對體系檢測所帶來的影響,制備出的CdS納米纖維能夠有效防止聚沉并實現(xiàn)對鉛離子的快速檢測,其對鉛離子的檢測線性范圍為1.0×10-10 1.0×10-6 gL-1,相關(guān)系數(shù)0.994。當(dāng)信噪比S/N=3時,新型固相電致化學(xué)發(fā)光傳感器的構(gòu)建及其對環(huán)境污染物的檢測檢測限達到1.0×10-10 gL-1。因為納米纖維不易發(fā)生聚集且具有較好的穩(wěn)定性,使得此傳感器具有高度穩(wěn)定且重復(fù)性良好的電致化學(xué)發(fā)光性能。
[Abstract]:Electrochemiluminescence detection has many advantages, such as high sensitivity, wide linear range, fast analytical speed and simple instrument operation. Therefore, electrochemiluminescence detection can meet the requirements of trace and even trace pollutants in the environment. But at present the electroluminescent sensor is mainly concentrated on a single material resulting in a low luminescence signal which is difficult to reach the detection range of pollutant concentration; the sensor can not be recycled resulting in waste of resources and so on. How to construct a green, pollution-free, recyclable, and good detection performance of electrochemiluminescence sensors has important significance. Based on the fabrication of immobilized electrochemiluminescence sensors, three kinds of electrochemiluminescence sensors composed of nanomaterials were constructed in this paper. These solid state sensors were used for rapid and sensitive detection of PCP and heavy metal ions in the environment. The immobilized sensors can be reused to reduce the waste of resources and provide a new method for the detection of environmental pollutants. The specific research work can be divided into the following aspects: (1) A novel solid-phase electrochemiluminescence sensor was constructed for graphene gold nanoclusters in the presence of co-reaction agent persulfate. Based on the redox reaction of pentachlorophenol (PCP) with the excited gold nanoparticles, the content of PCP in the environment was determined by the range of luminescence intensity of quenching. In this system, graphene can not only increase the electroluminescent intensity of gold nanoclusters, but also provide an immobilized platform for gold nanoclusters, thus solving the problems of low luminescence intensity and no recycling. The immobilized electroluminescent sensor has very good selectivity. Under the optimal detection conditions, PCP has a good linear range (1.0 脳 10-14 渭 m) and an ultra-low detection limit (1.0 脳 10-14 M). The method avoids the operation of complex instruments and has the advantages of low toxicity, recyclable use, high sensitivity detection, etc. It provides a simple and easy way for emergency and on-line detection of PCP in real water samples. (2) Electrodeposited platinum nanoclusters-graphene composite materials on the electrode by electrochemical deposition. The copper ion was detected quickly and trace by electrochemiluminescence. Because of the existence of graphene, the peak position of the luminescence potential and cyclic voltammetry curve also appears forward shift in addition to the enhancement of the current intensity and the increase of the electroluminescent signal, compared with the single platinum nanoclusters. It is shown that graphene has the ability to reduce barrier and accelerate electron transfer in this system. Because graphene and platinum nanoclusters have a large specific surface area, copper ions in the solution are easily adsorbed on the surface of the modified electrode, which makes the sensor have high sensitivity. The minimum detection limit for copper ions is 1.0 脳 10 ~ (-7) gL-1. (3). Cadmium sulfide (CdS) nanofibers were prepared by hydrothermal method and used for the electrochemiluminescence detection of lead ions. In order to reduce the influence of precipitation caused by nanoparticles on the system detection, the prepared CdS nanofibers can effectively prevent the coalescence and realize the rapid detection of lead ions. The linear range for the detection of lead ions is 1.0 脳 10 ~ (-10) ~ (10) gL-1, 1.0 脳 10 ~ (-6) gL-1, correlation coefficient, 0.994. When S / N = 3, a novel solid-phase electrochemiluminescence sensor and its detection limit for environmental pollutants reach 1.0 脳 10 ~ (-10) gL-1.. Because the nanofibers are not easy to aggregate and have good stability, the sensor has a high stability and good reproducibility of electrochemiluminescence.
【學(xué)位授予單位】：湖南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X830;O657.3
[Abstract]:Electrochemiluminescence detection has many advantages, such as high sensitivity, wide linear range, fast analytical speed and simple instrument operation. Therefore, electrochemiluminescence detection can meet the requirements of trace and even trace pollutants in the environment. But at present the electroluminescent sensor is mainly concentrated on a single material resulting in a low luminescence signal which is difficult to reach the detection range of pollutant concentration; the sensor can not be recycled resulting in waste of resources and so on. How to construct a green, pollution-free, recyclable, and good detection performance of electrochemiluminescence sensors has important significance. Based on the fabrication of immobilized electrochemiluminescence sensors, three kinds of electrochemiluminescence sensors composed of nanomaterials were constructed in this paper. These solid state sensors were used for rapid and sensitive detection of PCP and heavy metal ions in the environment. The immobilized sensors can be reused to reduce the waste of resources and provide a new method for the detection of environmental pollutants. The specific research work can be divided into the following aspects: (1) A novel solid-phase electrochemiluminescence sensor was constructed for graphene gold nanoclusters in the presence of co-reaction agent persulfate. Based on the redox reaction of pentachlorophenol (PCP) with the excited gold nanoparticles, the content of PCP in the environment was determined by the range of luminescence intensity of quenching. In this system, graphene can not only increase the electroluminescent intensity of gold nanoclusters, but also provide an immobilized platform for gold nanoclusters, thus solving the problems of low luminescence intensity and no recycling. The immobilized electroluminescent sensor has very good selectivity. Under the optimal detection conditions, PCP has a good linear range (1.0 脳 10-14 渭 m) and an ultra-low detection limit (1.0 脳 10-14 M). The method avoids the operation of complex instruments and has the advantages of low toxicity, recyclable use, high sensitivity detection, etc. It provides a simple and easy way for emergency and on-line detection of PCP in real water samples. (2) Electrodeposited platinum nanoclusters-graphene composite materials on the electrode by electrochemical deposition. The copper ion was detected quickly and trace by electrochemiluminescence. Because of the existence of graphene, the peak position of the luminescence potential and cyclic voltammetry curve also appears forward shift in addition to the enhancement of the current intensity and the increase of the electroluminescent signal, compared with the single platinum nanoclusters. It is shown that graphene has the ability to reduce barrier and accelerate electron transfer in this system. Because graphene and platinum nanoclusters have a large specific surface area, copper ions in the solution are easily adsorbed on the surface of the modified electrode, which makes the sensor have high sensitivity. The minimum detection limit for copper ions is 1.0 脳 10 ~ (-7) gL-1. (3). Cadmium sulfide (CdS) nanofibers were prepared by hydrothermal method and used for the electrochemiluminescence detection of lead ions. In order to reduce the influence of precipitation caused by nanoparticles on the system detection, the prepared CdS nanofibers can effectively prevent the coalescence and realize the rapid detection of lead ions. The linear range for the detection of lead ions is 1.0 脳 10 ~ (-10) ~ (10) gL-1, 1.0 脳 10 ~ (-6) gL-1, correlation coefficient, 0.994. When S / N = 3, a novel solid-phase electrochemiluminescence sensor and its detection limit for environmental pollutants reach 1.0 脳 10 ~ (-10) gL-1.. Because the nanofibers are not easy to aggregate and have good stability, the sensor has a high stability and good reproducibility of electrochemiluminescence.
【學(xué)位授予單位】：湖南大學(xué)
【學(xué)位級別】：碩士
【學(xué)位授予年份】：2015
【分類號】：X830;O657.3
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