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The Construction And Application Of New Small Molecule Electrochemiluminescent System And Device

Posted on:2021-02-03Degree:DoctorType:Dissertation
Country:ChinaCandidate:F YuanFull Text:PDF
GTID:1361330605979068Subject:Analytical Chemistry
Abstract/Summary:PDF Full Text Request
Electrochemiluminescence(ECL)is the combination of chemiluminescence and electrochemistry,which is endowed with properties such as high sensitivity,wide linear range,uncomplex apparatus,stablility and productivity.ECL has been widely applied in multiple fields such as environmental monitoring,nucleic acid testing,immunoassay and bioimaging.With the development of various emerging technologies nowadays,ECL also shows promising potential in practical applications.To meet the increasing demand for analysis and detection,the construction of new ECL systems and devices has become one of the most important research tasks.Based on the above,this thesis includes the work as follows:1.Oxamic hydrazide was utilized as an efficient co-reactant of Ru(bpy)32+ for the first time.It can enhance the ECL intensity of Ru(bpy)32+ by 100 times.Interestingly,4-nitrobenzaldehyde can reduce the ECL intensity of Ru(bpy)32+/oxamic hydrazide system dramatically.Through the study of the electrochemical property,ECL property and the mechanism of the ECL system,it is concluded that the primary amine of oxamic hydrazide structure makes it easy to be electro-oxidized to generate radicals,increasing the ECL intensity of Ru(bpy)32+.Besides,oxamic hydrazide can react with 4-nitrobenzaldehyde through the nucleophilic addition reaction,causing the ECL intensity decrease.Based on this,an ECL platform was constructed for the detection of 4-nitrobenzaldehyde.A linear range of 20 to 800 μM was obtained with a LOD of 1.1 μM.The detection of 4-nitrobenzaldehyde in tap water was performed with standard adding method and the recoveries range form 97.8%to 103.6%.2.A new small molecule dibutylaminoethyl acrylate(DBAEA)was designed and synthesized successfully.It shows excellent increasing effect on the ECL intensity of Ru(bpy)32+ on the platinum electrode as a new co-reactant of Ru(bpy)32+.Compared with traditional ECL system,the signal intensity of Ru(bpy)32+/DBAEA is 17 times and 10 times as that of Ru(bpy)32+/tripropylamine and Ru(bpy)32+/dibutylethanolamine,respectively.Cysteine can decrease the ECL intensity of Ru(bpy)32+/DBAEA dramatically.That is because cysteine can react with DBAEA and eliminate its acryloyl group.Based on this,a sensor was established for the quantitative detection of cysteine.A linear range of 10 μM to 2 mM was obtained with a LOD of 1.1 μM.When applied for the detection of other amino acid,this method shows excellent specificity.We utilized this method to detect the cysteine in DMEM,good recoveries from 93.5%to 105.6%was gained.3.A reusable low-background bipolar ECL device was constructed by means of drilling technology and applied in the detection of luminol/H2O2 ECL system.The designing thoughts are as follows:glassy carbon was used as the working electrode of the device.On the one hand,it has excellent electrochemical catalytic activity which can increase the detection sensitivity of the device.On the other hand,owing to the polishability of glassy carbon electrode,the detection signal is stable.Furthermore,stainless steel was used as the driving electrode.Due to the low ECL intensity on its surface,stainless steel can reduce the interference of the background.A tire repairing pad was drilled and stuck on the device as a cell,simplifying the construction of the device and lowering the cost.A smart phone was used as a detector,making the device portable and visible.This device was employed for the visual detection of H2O2 in Medicinal hydrogen peroxide,the recoveries range from 98.4%to 101.6%.
Keywords/Search Tags:electrochemiluminescence, co-reactant, bipolar electrode, visual detection
PDF Full Text Request
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