本文選題：化學發(fā)光 + 魯米諾��； 參考：《山東農(nóng)業(yè)大學》2015年碩士論文

【摘要】：化學發(fā)光分析因反應靈敏、線性范圍寬、測試速度快,在生物工程、食品分析、環(huán)境監(jiān)測、藥物分析、臨床診斷等多領(lǐng)域有重要應用。魯米諾-H2O2是常用的化學發(fā)光體系之一,具有結(jié)構(gòu)簡單、性質(zhì)穩(wěn)定、不污染環(huán)境的優(yōu)點。但因其反應速率低,常用金屬離子、納米粒子催化以加快反應進行。類水滑石是一類具有層狀結(jié)構(gòu)的無機雙金屬氫氧化物材料,對魯米諾-H2O2體系的化學發(fā)光有一定的增敏作用,但以往研究多集中在類水滑石層間的陰離子,為確定片層金屬組成及類水滑石片層與納米粒子的協(xié)同作用,本論文設計如下:采用原位沉淀還原法制備了銀負載的Mg-Al類水滑石納米粒子,采用混合共沉淀法合成了系列過渡金屬Cr3+、Co2+和Cu2+摻雜的類水滑石,研究了所得材料對魯米諾-H2O2體系化學發(fā)光性能的影響;間苯二酚對魯米諾-H2O2體系的發(fā)光強度有明顯的抑制作用,以此探索類水滑石增敏的魯米諾-H2O2體系能否實現(xiàn)對間苯二酚的靈敏性檢測。本論文主要由以下四部分內(nèi)容組成:1.采用共沉淀法合成Mg-Al水滑石前驅(qū)體,然后原位沉淀還原,將銀納米粒子負載到類水滑石上。利用X射線衍射(XRD)和透射電鏡(TEM)對所得材料進行了表征,用流動注射法對負載銀納米粒子的類水滑石材料進行了催化性能研究,結(jié)果表明合成的負載型納米催化劑具有類水滑石片狀結(jié)構(gòu),且對魯米諾化學發(fā)光體系具有良好的催化活性。催化效果受魯米諾、LDHs-Ag及NaOH濃度影響,最優(yōu)催化條件為NaOH濃度0.05mol/L,魯米諾濃度2.0×10-4 mol/L,LDHs-Ag濃度1g/L。最優(yōu)條件下,在H2O2濃度為1×10-5-1×10-3 mol/L范圍內(nèi),H2O2濃度與體系的發(fā)光強度具有良好的線性關(guān)系:I=22.24+5289.22 c(×103 mol/L)(相關(guān)系數(shù)R2=0.9965),檢測限為7.7×10-6 mol/L(S/N=3),因此該法可以用于微量H2O2的定量分析,具有一定的應用研究價值。2.采用混合共沉淀的方法將過渡金屬Cr3+引入類水滑石層板中,得到了Cr-Mg-Al-LDHs。利用紅外光譜(FTIR)、X射線衍射(XRD)和透射電鏡(TEM)等手段對樣品進行表征,結(jié)果表明Cr3+的摻雜對類水滑石的層狀結(jié)構(gòu)沒有影響,僅降低了類水滑石的結(jié)晶度。利用流動注射分析(FIA)研究了Cr-Mg-Al-LDHs對魯米諾-H2O2化學發(fā)光體系催化作用。在最優(yōu)條件為pH 10.5,魯米諾濃度1.0×10-4 mol/L,LDHs濃度1 g/L,H2O2濃度在1×10-5-1×10-3 mol/L范圍內(nèi),Cr-Mg-Al-LDHs催化的化學發(fā)光體系的發(fā)光強度與H2O2濃度間存在線性方程:I=-101.80+203.57c(×105 mol/L)(相關(guān)系數(shù)R2=0.9918),檢測限為7.5×10-6 mol/L(S/N=3)。3.采用混合共沉淀的方法將Co2+引入類水滑石層板中,得到了Co-Mg-Al-LDHs。利用紅外光譜(FTIR)、X射線衍射(XRD)和透射電鏡(TEM)等手段對樣品進行表征,結(jié)果表明Co2+的摻雜對類水滑石的層狀結(jié)構(gòu)和結(jié)晶度等物理性質(zhì)基本沒有影響。利用流動注射分析(FIA)研究了Co-Mg-Al-LDHs對魯米諾-H2O2化學發(fā)光體系催化作用,研究表明Co2+能夠極大地改善類水滑石材料的催化性能,且催化效果與過渡金屬的含量有關(guān),Co-Mg-Al-LDHs中Co(II)含量越高,其催化活性就越高。最優(yōu)測試條件為p H 10.5,魯米諾濃度1.0×10-4 mol/L,LDHs濃度1 g/L。在最優(yōu)條件下,當H2O2在濃度在1×10-6-1×10-3mol/L范圍內(nèi),Co-Mg-Al-LDHs催化的發(fā)光體系的信號強度與H2O2濃度間存在線性方程:I=-231.53+894.83c(×106 mol/L)(相關(guān)系數(shù)R2=0.9954),檢測限為3.2×10-7mol/L(S/N=3)。4.采用混合共沉淀法得到了Cu-Mg-Al-LDHs。利用紅外光譜(FTIR)、X射線衍射(XRD)和透射電鏡(TEM)等手段對Cu-Mg-Al-LDHs進行表征,并利用流動注射分析(FIA)研究了Cu-Mg-Al-LDHs對魯米諾-H2O2化學發(fā)光體系催化作用。對魯米諾-H2O2體系的最優(yōu)催化條件為:魯米諾濃度1×10-4 mol/L,pH 11.0,LDHs濃度2 g/L時,H2O2在1×10-6-1.2×10-4 mol/L范圍內(nèi),與發(fā)光強度間線性方程為:I=-422.85+230.30 c(×106 mol/L)(相關(guān)系數(shù)R2=0.9998),檢測限為3.8×10-7 mol/L(S/N=3)。將間苯二酚加入Cu-Mg-Al-LDHs增敏的魯米諾-H2O2化學發(fā)光體系,化學發(fā)光強度受到明顯的抑制,在1×10-9-1×10-3 g/L濃度范圍內(nèi),體系的發(fā)光強度I與間苯二酚濃度的對數(shù)lgc呈良好的線性關(guān)系:I=3772-303.14lgc(相關(guān)系數(shù)R2=0.9972),檢測限為3.7×10-10 g/L(S/N=3)。該檢測方法具有靈敏度高,檢測限低,線性范圍寬,操作簡單,成本低等優(yōu)點,可作為定量檢測間苯二酚的簡便方法。
[Abstract]:Chemiluminescence analysis has important applications in many fields, such as biological engineering, food analysis, environmental monitoring, drug analysis and clinical diagnosis. Luminol -H2O2 is one of the commonly used chemiluminescence systems, which has the advantages of simple structure, stable properties and no pollution to the environment. Using metal ions and nanoparticles as a catalyst to accelerate the reaction. Hydrotalcite like hydrotalcite is a class of inorganic bimetal hydroxides with layered structure. It has a certain sensitization effect on the chemiluminescence of the luminol -H2O2 system. However, the previous studies focused on the detachment of the hydrotalcite like layers to determine the composition of lamellar metals and the hydrotalcite like slices. The synergistic effect of layer and nanoparticle is as follows: in this paper, the silver loaded Mg-Al hydrotalcite nanoparticles were prepared by in situ precipitation reduction method. A series of transition metals, Cr3+, Co2+ and Cu2+ doped hydrotalcite were synthesized by the mixed coprecipitation method. The effects of the materials on the chemiluminescence properties of the luminol -H2O2 system were studied. The photoluminescence of the Lumino -H2O2 system has a significant inhibitory effect on the sensitivity of the Lumino -H2O2 system sensitized by hydrotalcite like to realize the sensitivity detection of resorcinol. This paper is mainly composed of the following four parts: 1. the precursor of Mg-Al hydrotalcite is synthesized by coprecipitation method, and then in situ precipitation and reduction, and Silver The nanoparticles were loaded on the hydrotalcite. X ray diffraction (XRD) and transmission electron microscopy (TEM) were used to characterize the obtained materials. The flow injection method was used to study the catalytic properties of the hydrotalcite like nanoparticles loaded with silver nanoparticles. The results showed that the synthesized loaded nanoscale was composed of a hydrotalcite like structure and to luminol. The luminescent system has good catalytic activity. The catalytic effect is influenced by the concentration of Lumino, LDHs-Ag and NaOH. The optimal catalytic condition is NaOH concentration 0.05mol/L, Lumino concentration 2 x 10-4 mol/L, LDHs-Ag concentration 1g/L. optimum condition, H2O2 concentration is 1 x 10-5-1 x 10-3 mol/L range, H2O2 concentration is good with the luminous intensity of the system. Linear relation: I=22.24+5289.22 C (x 103 mol/L) (correlation coefficient R2=0.9965), the detection limit is 7.7 x 10-6 mol/L (S/N=3), so this method can be used for quantitative analysis of trace H2O2. The value.2. uses mixed coprecipitation method to introduce the transition metal Cr3+ into the hydrotalcite like laminates, and obtains Cr-Mg-Al-LDHs. utilization red. The samples were characterized by external spectrum (FTIR), X ray diffraction (XRD) and transmission electron microscopy (TEM). The results showed that the doping of Cr3+ had no effect on the layered structure of hydrotalcite, and only reduced the crystallinity of the hydrotalcite. The catalytic effect of Cr-Mg-Al-LDHs on the luminol -H2O2 chemiluminescence system was studied by flow injection analysis (FIA). The conditions are pH 10.5, Lumino concentration is 1 x 10-4 mol/L, LDHs concentration is 1 g/L, H2O2 concentration is within the range of 1 x 10-5-1 x 10-3 mol/L. There is a linear equation between the luminescence intensity and H2O2 concentration of Cr-Mg-Al-LDHs catalyzed chemiluminescence system: I=-101.80+203.57c (x 105 mol/L) (correlation series R2=0.9918), and the detection limit is 7.5 x 10-6. Co2+ was introduced into the hydrotalcite like laminates by the method of co precipitation. The samples were characterized by Co-Mg-Al-LDHs. using infrared spectroscopy (FTIR), X ray diffraction (XRD) and transmission electron microscopy (TEM). The results showed that the doping of Co2+ had no effect on the physical properties of the layered structure and crystallinity of the hydrotalcite. FIA) studied the catalytic effect of Co-Mg-Al-LDHs on the Lumino -H2O2 chemiluminescence system. The study shows that Co2+ can greatly improve the catalytic performance of the hydrotalcite like material, and the catalytic effect is related to the content of the transition metal. The higher the content of Co (II) in Co-Mg-Al-LDHs, the higher the catalytic activity. The optimum test condition is p H 10.5, and the Lumino concentration is 1. X 10-4 mol/L, LDHs concentration 1 g/L. under the optimal conditions, when H2O2 is in the range of 1 x 10-6-1 * 10-3mol/L, there is a linear equation between the signal intensity of the luminescent system and H2O2 concentration catalyzed by Co-Mg-Al-LDHs: I=-231.53+894.83c (x 106 mol/L) (R2=0.9954), and the detection limit of 3.2 * 10-7mol/L is obtained by a mixed coprecipitation method. Cu-Mg-Al-LDHs. was used to characterize Cu-Mg-Al-LDHs by means of infrared spectroscopy (FTIR), X ray diffraction (XRD) and transmission electron microscopy (TEM). The catalytic effect of Cu-Mg-Al-LDHs on the Lumino -H2O2 chemiluminescence system was studied by flow injection analysis (FIA). The optimum conditions for the Lumino -H2O2 system were as follows: Lumino concentration was 1 x 10-4 mol/L. When the concentration of pH 11 and LDHs is 2 g/L, H2O2 is within the range of 1 x 10-6-1.2 10-4 mol/L, and the linear equation between the luminescence intensity and the luminescence intensity is I=-422.85+230.30 C (x 106 mol/L) (correlation coefficient R2=0.9998), and the detection limit is 3.8 x 10-7 mol/L (S/N=3). In the 1 * 10-9-1 x 10-3 g/L concentration range, the luminescence intensity I of the system has a good linear relationship with the logarithmic LGC of the resorcinol concentration: I=3772-303.14lgc (correlation coefficient R2=0.9972) and the detection limit of 3.7 * 10-10 g/L (S/N=3). The detection method has the advantages of high sensitivity, low detection limit, wide linear range, simple operation and low cost, etc. It can be used as a simple method for quantitative detection of resorcinol.
【學位授予單位】：山東農(nóng)業(yè)大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：TB33;O643.36

【參考文獻】

相關(guān)期刊論文 前3條

1 陳英紅,薛錦珍,侯瑞玲,劉育,李樹本;水滑石類復合氧化物在CO+NO反應中的應用[J];分子催化;2000年04期

2 朱智甲,楊秋青,郝振芳;流動注射膠束增敏光澤精化學發(fā)光法測定谷物中Fe(Ⅲ)[J];理化檢驗(化學分冊);2000年02期

3 李保新,章竹君;化學發(fā)光和生物發(fā)光傳感器的新進展[J];陜西師范大學學報(自然科學版);1999年03期

，

本文編號：1985391