研究目的
Understanding selective surface photocatalytic reaction mechanisms is critical for optimizing many energy conversion applications. Measuring time-resolved concentration profiles of the reactants, products, and intermediates during such reactions is a key step in elucidating these reaction mechanisms and understanding the role of hot electrons.
研究成果
In summary, a simple and low-cost approach is proposed to fabricate a Ag plasmonic film for SERS investigation of selective surface photocalyzed reactions, and use this to study the photoreduction of 4-NTP to 4-ATP in a systematic set of controlled environments. In addition to the controlled concentrations possible through deposition of aqueous solutions on the chemical reactant absorbed on the AgPF, selective surface photocatalyed reactions can be observed without a chemical reducing agent. With our AgPF, the first experimental evidence of the formation of the DMAB intermediate is presented in the photocatalyzed reduction of 4-NTP in the absence of a chemical reducing agent which is consistent with previous theoretical study of 4-NTP phtoreduction. Moreover, the influence of different H+- and Cl--concentration on the kinetics of the reaction were quantitatively studied and a reaction mechanism for the reduction reaction that is consistent with our experimental measurements was proposed.
研究不足
The technical and application constraints of the experiments, as well as potential areas for optimization.
1：Experimental Design and Method Selection:
Includes the overall experimental design rationale, the theoretical models or algorithms employed, and detailed procedures of the experimental methods.
2：Sample Selection and Data Sources:
Specifies the samples or datasets used in the experiment, including selection criteria and data acquisition methods.
3：List of Experimental Equipment and Materials:
Enumerates the required instruments, devices, and materials, along with their specifications and intended uses.
4：Experimental Procedures and Operational Workflow:
Provides a step-by-step description of the experimental process, covering equipment setup, data collection techniques, and control of variables during the experiment.
5：Data Analysis Methods:
Explains the approach for analyzing experimental data, including statistical techniques and software tools utilized.
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Silver Nitrate
Sigma Aldrich
Used in the preparation of silver colloid.
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Polyvinylpyrrolidone
Sigma Aldrich
Used to stabilize the silver colloid.
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Tetrabutylammonium Nitrate
Sigma Aldrich
Used in the preparation of the Ag plasmonic film.
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Hydroxylamine Hydrochloride
Sigma Aldrich
Used as a reducing agent in the preparation of silver colloid.
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Dichloromethane
Sigma Aldrich
Used in the preparation of the Ag plasmonic film.
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4-Nitrothiophenol
Sigma Aldrich
Used as a reactant in the photocatalytic reduction reaction.
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Sodium Chloride
Sigma Aldrich
Used to control the Cl--concentration in the reaction environment.
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Hydrochloric Acid
37%
Sigma Aldrich
Used to control the H+-concentration in the reaction environment.
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Sulfuric Acid
95%-98%
Sigma Aldrich
Used to control the H+-concentration in the reaction environment.
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Sodium Hydroxide
MERCK
Used in the preparation of the reducing solution for silver colloid.
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Milli-Q water
Millipore
Used as a solvent in the preparation of solutions.
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Cobolt DPL 532 nm solid state laser
Cobolt AB
Used to initiate and process the photocatalytic reaction.
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WITec Alpha 300 R microscope
WITec GmbH
Used to record the SERS spectra.
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Zeiss Sigma VP field emission scanning electron microscope
Zeiss
Used for SEM images acquisition.
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MFD-3D AFM
Asylum Research
Used to obtain AFM characterization.
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GRAPHTEC cutting plotter CE 6000-40
GRAPHTEC
Used to cut double side-adhesive tape.
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