研究目的
Developing a low-cost and effective oxygen reduction reaction (ORR) catalyst using metal cation vacancies as active sites to substitute for Pt-based catalysts in fuel cells.
研究成果
The ZnS/N–C-900 catalyst with Zn vacancies exhibits superior ORR performance, including high activity, durability, and methanol tolerance, outperforming Pt/C. DFT calculations confirm that Zn vacancies lower the reaction energy for ORR, making it a promising substitute for Pt-based catalysts in fuel cells. The study provides a new strategy for using organic dyes in catalyst design.
研究不足
The study focuses on alkaline medium (0.1 M KOH) and may not generalize to other electrolytes. The catalyst synthesis requires high temperature (900°C) and specific precursors, which could limit scalability. The DFT calculations are theoretical and may not fully capture real-world conditions.
1:Experimental Design and Method Selection:
The catalyst ZnS/N–C-900 was prepared via a one-step pyrolysis method at 900°C using glucose, organic dye (K-GR), and ZnCl2 as precursors. Characterization included XRD, Raman, XPS, TEM, HRTEM, STEM-EDS, and BET analysis. Electrochemical measurements were performed using a three-electrode cell with CV, LSV, and chronoamperometry in 0.1 M KOH. DFT calculations were conducted using VASP to study reaction energies.
2:1 M KOH. DFT calculations were conducted using VASP to study reaction energies. Sample Selection and Data Sources:
2. Sample Selection and Data Sources: Samples included C-900 (pure glucose), N,S-C-900 (glucose and K-GR), and ZnS/N–C-900 (glucose, K-GR, and ZnCl2). Data were obtained from laboratory synthesis and characterization instruments.
3:2). Data were obtained from laboratory synthesis and characterization instruments. List of Experimental Equipment and Materials:
3. List of Experimental Equipment and Materials: Equipment: XRD instrument (Bruker D8), Raman spectrometer (Renishaw), XPS spectrometer (AMICUS/ESCA 3400), TEM (JEM-2100), HRTEM (Tecnai G2 F20), STEM-EDS (LEO 1430 VP), BET analyzer (ASAP 2460), electrochemical station (CHI 760D). Materials: Glucose, K-GR organic dye, ZnCl2, de-ionized water, HCl, ethanol, Nafion, Ag/AgCl reference electrode, glassy carbon disk, graphite rod, Pt/C catalyst.
4:Experimental Procedures and Operational Workflow:
Preparation involved dissolving glucose, K-GR, and ZnCl2 in water, stirring, drying, pyrolysis at 900°C for 2 h, acid treatment, washing, and drying. Characterization steps included XRD, Raman, XPS, TEM, HRTEM, STEM-EDS, and BET analysis. Electrochemical testing involved preparing catalyst ink, drop-coating on electrode, and performing CV, LSV, and stability tests in O2-saturated KOH.
5:Data Analysis Methods:
XRD for crystalline structure, Raman for graphitization degree, XPS for chemical states, TEM for morphology, BET for surface area and porosity, Koutecky–Levich equation for electron transfer number, DFT for adsorption energies and Gibbs free energy changes.
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XRD instrument
D8
Bruker
Characterization of crystalline structure
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HRTEM
Tecnai G2 F20
FEI
High-resolution imaging and defect observation
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Raman spectrometer
Renishaw
Characterization of structural properties and defects
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XPS spectrometer
AMICUS/ESCA 3400
Analysis of chemical states of elements
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TEM
JEM-2100
Study of morphologies
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STEM-EDS
LEO 1430 VP
Element mapping and analysis
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BET analyzer
ASAP 2460
Measurement of surface area, pore volume, and pore size
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Electrochemical station
CHI 760D
Electrochemical measurements including CV, LSV, and chronoamperometry
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Ag/AgCl reference electrode
Reference electrode in electrochemical cell
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Glassy carbon disk
Working electrode
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Graphite rod
Counter electrode
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Pt/C catalyst
20 wt%
Commercial catalyst for comparison in ORR tests
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Nafion
20% wt
Binder in catalyst ink preparation
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