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Preparation And Electrocatalysis Application Study Of Porous Carbon And Its Nanocomposite Materials

Posted on:2015-06-12Degree:DoctorType:Dissertation
Country:ChinaCandidate:H WangFull Text:PDF
GTID:1481304313468164Subject:Analytical Chemistry
Abstract/Summary:PDF Full Text Request
With the development of carbon nanomaterials, owing to their massive pores, highspecific surface area and unique frame, porous carbon nanomaterials have received a greatdeal of attention in different fields. Recent years, porous carbon nanomaterials have beenwidely used in electrochemistry area, such as used as catalyst in electrocatalytic reaction andused as electrode material in capacitor. Based on the previously research, we fabricated somenovel porous carbon and its nanocomposite materials, and then researched theirelectrocatalytic application, the content was listed below:(1) We examined the electrocatalytic application of a novel mesoporous carbonnanofiber (M-CNF) that was synthesized using a self templating strategy, it employed as acarbon electrode material for detecting DA, AA and UA and exhibited significantly enhancedelectrocatalytic performance. Moreover, the superior electrocatalytic capability of the M-CNFwas confirmed by its simultaneous detection of DA, AA and UA at a physiological pH of7.4,where it demonstrated a wide linear range and high sensitivity. In addition, other biomoleculessuch as some purines were examined in the presence of the M-CNF, and its outstandingperformance verified that the M-CNF was a promising electrocatalyst. Next, by combiningthe advantages of unique nanostructure and large surface area of M-CNF combined with theelectrocatalytic ability of Au nanoparticles, M-CNF-Au was successfully prepared as ahydrazine catalyst. Low detection limit, wide linear range and short response time providedan opportunity for M-CNF-Au as a promising electrode material for the fabrication of anefficient hydrazine amperometric sensor. Moreover, this nanocomposite suggests greatpotential applications in the design and construction of M-CNF based materials forelectrocatalytic application.(2) PtxPdy/LMC nanocomposites were prepared. In application to electrochemistry,hydrogen peroxide and nitrite were employed as the probes to measure the electrochemicalperformance of PtxPdy/LMC. Comparison of hydrogen peroxide reduction and nitriteoxidation on PtxPdy/LMC/GCE indicated that the Pt1Pd1/LMC/GCE exhibited the highestactivity. The combination the high-efficiency catalysis and synergistic effect of Pt, Pd alloynanoparticles to electrocatalytic reaction and the unique structure of LMC matrix endows theenhanced electrochemical performance of Pt1Pd1/LMC/GCE. It is expected that thePt1Pd1/LMC/GCE is not only a sensitive sensor for hydrogen peroxide and nitrite in practicalapplication, but also can used as a high-performance electrocatalyst for other substances.Inspired by LMC, we reported a one step and green approach for the fabrication of N-LMCby using herring sperm DNA as carbon and nitrogen precursor. N-LMC/GCE was fabricated, and its electrocatalytic performance for the ORR was investigated. With high amounts ofpyridinic N and graphitic N, N-LMC-800exhibited higher electrocatalytic activity for theORR than LMC, which made it a very promising cathode catalyst for fuel cell application.(3) We successfully prepared OMC-S-X with different sulfur contents through varyingthe relative amounts of sucrose and benzyl disulfide in the preparation procedure. Theresulting OMC-S-3served as metal-free catalyst that showed outstanding electrocatalyticactivity, good stability and excellent resistance tocrossover effect for ORR. Moreover, theinfluence of different S-bonding configurations in OMC-S-X for ORR was researched whichproved that C-S-C played an important role in promoting the ORR activity.(4) PDA-HCS-Co with nanoporous hollow sphere morphology was prepared. AlthoughPDA-HCS alone had little catalytic activity for ORR, PDA-HCS-Co exhibited similar highcatalytic activity but superior stability and methanol tolerance compared to commercial Pt-Ccatalyst. This indicates combining the advantages of nitrogen and Co-N for ORR; thesynthesized PDA-HCS-Co is a promising non-precious metal ORR catalyst.(5) We demonstrated the rational design and fabrication of a novel P-GR using copperas an etching agent. In particular, the electrochemical behaviors of various electroactivecompounds were studied on P-GR/GCE, which exhibited more favorable electron transferkinetics than that on GR/GCE. The greatly enhanced electrochemical reactivity of theseprobes on P-GR/GCE is attributed to the unique porous structure, higher amounts of EDSsand more acidic groups of P-GR relative to GR. This research is of great significance not onlybecause it is an innovative strategy of preparing P-GR but also because it constructs a novelelectrochemical biosensing platform based on the freshly prepared P-GR, expand theapplication field of P-GR.
Keywords/Search Tags:Porous Carbon, Nanocomposite Materials, Electrocatalysis, Small BiologicalMolecules, Oxygen Reduction Reaction
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