研究目的
To enhance the photocatalytic activity of tantalum nitride (Ta3N5) by suppressing charge recombination in bulk, interface, and surface for efficient solar hydrogen generation.
研究成果
The synergistic approach combining hollow structure, Mg doping, MgO interfacial layer, and dual cocatalysts effectively suppresses charge recombination, leading to a significantly improved H2 evolution rate of 56.3 μmol h-1, which is 38 times higher than the bulk counterpart. This strategy can be applied to optimize other photocatalysts for solar energy conversion.
研究不足
The apparent quantum efficiency (AQE) is moderate (0.31%) due to low visible-light conversion efficiency of Ta3N5, indicating potential for improvement in light utilization.
1：Experimental Design and Method Selection:
A synergistic three-step engineering approach involving nanostructure control, doping, surface passivation, and dual cocatalyst loading to suppress charge recombination.
2：Sample Selection and Data Sources:
Carbon spheres used as hard templates; TaCl5, Mg(NO3)2·6H2O, and other chemicals from Sigma-Aldrich.
3：List of Experimental Equipment and Materials:
Teflon-lined autoclave, centrifuges, tube furnace, CHI 660d electrochemical workstation, Labsolar-Ⅲ AG system, SEM, TEM, HRTEM, XRD, Raman, EDS, ICP-OES, BET surface area analyzer, XPS, photoluminescence spectroscopy, UV-vis spectrophotometer.
4：Experimental Procedures and Operational Workflow:
Synthesis of carbon spheres, Mg-doped Ta2O5 hollow spheres, surface modification with MgO, nitridation to Ta3N5, deposition of CoOx and Pt cocatalysts, characterization, photoelectrochemical measurements, photocatalytic H2 evolution tests.
5：Data Analysis Methods:
XRD and Raman for crystal structure, SEM/TEM for morphology, XPS for chemical states, UV-vis for optical properties, Mott-Schottky analysis for carrier concentration, GC for H2 quantification.
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glucose
Sigma-Aldrich
Used in the preparation of carbon spheres as a template.
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TaCl5
Sigma-Aldrich
Precursor for synthesizing Ta2O5 and Ta3N5.
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Mg(NO3)2·6H2O
Sigma-Aldrich
Source of Mg dopant for doping into Ta3N5.
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MgSO4
Sigma-Aldrich
Used for surface modification to form MgO layer.
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cobalt nitrate
Sigma-Aldrich
Precursor for depositing CoOx cocatalyst.
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H2PtCl6
Precursor for depositing Pt cocatalyst via photodeposition.
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Teflon-lined autoclave
Used for hydrothermal synthesis of carbon spheres.
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centrifuge
Used for separating and washing samples.
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tube furnace
Used for calcination and nitridation processes under controlled atmosphere.
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CHI 660d electrochemical workstation
CHI 660d
Used for electrochemical measurements including Mott-Schottky and linear sweep voltammetry.
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Labsolar-Ⅲ AG system
Labsolar-Ⅲ AG
Beijing Perfectlight Technology co. LTD
Photocatalytic reaction system for H2 evolution tests.
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SEM
Used for morphological characterization of samples.
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TEM
Used for high-resolution imaging and microstructural analysis.
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HRTEM
Used for detailed lattice imaging.
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XRD
Used for crystal structure identification.
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Raman spectrometer
Used for microstructural analysis.
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EDS
Used for elemental analysis and mapping.
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ICP-OES
Used for quantitative elemental analysis.
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BET surface area analyzer
Used for measuring specific surface areas.
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XPS
Used for investigating chemical components and states.
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