研究目的
To demonstrate the potency of favorable interaction between nanoparticle (NP) catalyst and reactant in suppressing the ligand poisoning effect in the model photocatalytic reaction of ferricyanide reduction.
研究成果
The introduction of favorable interactions through precise surface functionalization helped in achieving an efficient visible-light photocatalysis with AuNPs capped with insulating organic ligands. The favorable interaction arising from electrostatic forces was tuned by varying the surface potential around AuNP catalysts, resulting in an increase in the local concentration of ferricyanide around the NP surface and improving the photocatalytic performances.
研究不足
The formation of irreversible aggregates of [+] AuNPs in the presence of [-] ferricyanide can adversely affect the recyclability prospects of AuNP catalysts.
1:Experimental Design and Method Selection:
The study involved the photocatalytic reduction of ferricyanide by gold nanoparticles (AuNPs) in the presence of ethanol as the hole scavenger. The interaction between NP catalyst and ferricyanide reactant was tuned by varying the surface potential around AuNPs through precise ligand functionalization.
2:Sample Selection and Data Sources:
Cationic ([+]) and anionic ([-]) organic ligands were functionalized on AuNP surface to generate favorable and unfavorable interactions with [-] ferricyanide, respectively.
3:List of Experimental Equipment and Materials:
Gold nanoparticles (AuNPs), N,N,N-trimethyl(11-mercaptoundecyl)ammonium chloride (TMA, [+]), 11-mercaptoundecanoic acid (MUA, [?]), ferricyanide, ethanol, 3W blue Light Emitting Diodes (LEDs).
4:Experimental Procedures and Operational Workflow:
The photocatalytic reduction was monitored through UV-Vis absorption spectroscopy. The progress of ferricyanide reduction was observed by the decrease in its absorption at ~420 nm.
5:Data Analysis Methods:
The first order kinetic analysis was performed on the spectral changes recorded at ~420 nm. Thermodynamic analysis based on Marcus model of outer sphere electron transfer was also conducted.
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