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The Application Research Of Ruthenium-based Compounds In The Field Of Electrochemiluminescence Sensing And Electrocatalytic Hydrogen Evolution

Posted on:2021-05-07Degree:MasterType:Thesis
Country:ChinaCandidate:J T CaiFull Text:PDF
GTID:2431330611992563Subject:Materials Physics and Chemistry
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Ru belongs to the fifth cycle platinum group element,which is rich in oxidation valence state,making ruthenium metal and its compounds applied in many fields such as sensing,energy and catalysis.In this article,we firstly study the one of the important ruthenium complexes(Ru?bpy?32+),Ru?bpy?32+not only can be used as a light catalyst for photo-induced electron transfer–reversible addition–fragmentation chain transfer?PET-RAFT?polymerization,but also as a sensing probe for electrochemiluminescence?ECL?sensor.Based on this,we successfully construct ECL sensors via the combination of molecular imprinted technolgy?MIT?and ECL techniques.Firstly,negatively-charged Au nanoparticles?AuNPs?were prepared and modified with Ru?bpy?32+via electrostatic incorporation.Then,molecular imprinted polymers?MIPs?were prepared on the surface of AuNPs using melamine?MEL?as the template via PET-RAFT cross-linking polymerization,which Ru?bpy?32+was used as catalyst.The MIPs modified AuNPs?AuNPs-MIPs?were then fixed on the surface of working electrode with Nafion to achieve a solid-state ECL sensing platform employing Ru?bpy?32+as the ECL probes.The as-prepared sensor showed a wide detection range of 5.0×10-13–5.0×10-6 mol/L and a low detection limit of 1.0×10-13 mol/L?S/N?3?was reached in the detection of MEL.Moreover,further tests for analyzing MEL structural analogues proved that the constructed ECL sensing platform could be utilized to detect various substances via specific recognitions.In addition,we also studied the application of Ru nanoparticles in the field of energy catalysis,and designed a porous 3D Ru-based catalyst for hydrogen evolution reaction?HER?.In the experiment,polydopamine?PDA?NPs with uniform sizes of 300 nm are prepared.Then,the Ru nanoclusters?Ru NCs?are uniformly generated inside and on the surface of the PDA NPs to afford the bi-nanospheres?Ru-PDA NPs?.After annealing,the porous carbonized Ru-PDA NPs?Ru-cPDA-750 NPs?with electroactive nitrogen atoms are finally obtained,exhibiting small overpotential(42 mV at the current density of 10 m A cm-2),low value of Tafel slope(35 mV decade-1)and robust stability for hydrogen evolution reaction?HER?,which are comparable to that of Pt/C catalyst.Moreover,the study on the effect of Ru NCs amount on electrocatalytic ability reveals that Ru-cPDA NPs loaded with 0.08 wt%of Ru NCs exhibit the best HER catalytic performance compared with the Ru-cPDA NPs loaded with other amount of Ru NCs?0.04-0.16 wt%?.
Keywords/Search Tags:Ru compound, electrochemiluminescence, molecular imprinted polymer, biosensor, electrocatalysis
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