研究目的
To develop a scalable fabrication process for particle-based photoanodes and investigate the effects of scaling up from lab size (1 cm2) to demonstrator size (40 cm2) on the performance of LaTiO2N photoanodes for photoelectrochemical water splitting.
研究成果
The scalable fabrication process was successfully developed, but scale-up to 40 cm2 electrodes resulted in significant photocurrent density losses, particularly for high-performing configurations. Improvements in substrate conductivity recovered only minor losses, and electrode size effects were evident, necessitating future collaboration with modeling to optimize electrode geometry and contact points for large-scale applications.
研究不足
The scale-up process faced challenges with uniform annealing in NH3 for large electrodes, leading to the use of air annealing which reduced performance. Charge transport issues persisted, and photocurrent densities dropped significantly for larger electrodes, indicating limitations in substrate conductivity and potential distribution. The study was constrained to specific materials and conditions, and further simulations are needed for full understanding.
1:Experimental Design and Method Selection:
The study involved designing a scalable process for fabricating photoanodes using electrophoretic deposition, annealing in air or ammonia, and dip coating. Methods were selected for their scalability and ability to ensure charge transport.
2:Sample Selection and Data Sources:
LaTiO2N (LTON) particles and LTON/multiwall carbon nanotube (MWCNT) composites were synthesized and used. Electrodes were fabricated on FTO substrates of sizes 1 cm2 and 40 cm
3:List of Experimental Equipment and Materials:
Equipment included an ultrasonic stirrer (Bandelin SONOPLUS HD 3100), X-ray diffractometer (PANanalytical X'Pert PRO), scanning electron microscope (FEI NovaNanoSEM), profilometer (Bruker DektakX), UV-Vis spectrophotometer (Shimadzu UV-3600), optical microscope (Zeiss Axioplan), potentiostat (VersaSTAT 4), Xe lamp (Lot Oriel), and gas chromatograph (Inficon). Materials included FTO substrates (Solaronix TCO22-15 and TCO11-7), I2 (Sigma-Aldrich), acetone (Merck), TiCl4, TaCl5, Ni(NO3)2, Co(NO3)2, Na2SO4, NaOH, and ammonia.
4:Experimental Procedures and Operational Workflow:
Electrodes were prepared by electrophoretic deposition with stirring (magnetic for 1 cm2, ultrasonic for 40 cm2), followed by necking via dipping in TiCl4 solution and annealing (in NH3 for lab scale or air for scale-up). Optional co-catalyst coatings (Ta2O5, NiOx, CoOx) were applied by dip coating and annealing. Characterization included XRD, SEM, profilometry, UV-Vis, optical microscopy, and photoelectrochemical measurements in a three-electrode setup with Pt counter and Ag/AgCl reference electrodes under AM1.5G illumination.
5:5G illumination. Data Analysis Methods:
5. Data Analysis Methods: Data were analyzed using techniques such as comparing photocurrent densities at 1.23 V vs. RHE, front-to-back illumination ratios, Faraday efficiencies from gas chromatography, and statistical evaluation of reproducibility.
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X-ray diffractometer
X'Pert PRO
PANanalytical
Used for structural characterization of materials via X-ray diffraction.
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Scanning electron microscope
NovaNanoSEM
FEI
Used for morphological study of particles and electrodes.
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Profilometer
DektakX
Bruker
Used to measure film thickness of electrodes.
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UV-Vis spectrophotometer
UV-3600
Shimadzu
Used to acquire UV-Vis transmission spectra of electrodes.
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Optical microscope
Axioplan
Zeiss
Used to study electrode morphology via optical microscopy.
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Potentiostat
VersaSTAT 4
Used for photoelectrochemical measurements, including current density acquisition.
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Xe lamp
Lot Oriel
Used as a light source for illumination during photoelectrochemical experiments.
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Gas chromatograph
Inficon
Used to measure gas evolution (H2, O2, N2) for Faraday efficiency calculations.
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Ultrasonic stirrer
SONOPLUS HD 3100
Bandelin
Used for homogenizing suspensions during electrophoretic deposition of large electrodes.
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FTO substrate
TCO22-15
Solaronix
Used as a conducting substrate for electrode fabrication.
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FTO substrate
TCO11-7
Solaronix
Used as an alternative conducting substrate with lower resistivity.
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