Journal
ACS ENERGY LETTERS
Volume 6, Issue 5, Pages 1980-1989Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.1c00563
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Funding
- Energy & Biosciences Institute (EBI) through the EBI-Shell program
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This study investigates the chemistry triggered by aliphatic alcohols used as sacrificial agents in the photoinduced synthesis of Au nanoparticles. The results show that the Lewis-acidic metal center of the [AuCl4](-) complex activates atypical reactions, enhanced by the photoexcited carriers generated by the Au nanoparticles. This work presents a unique example of interplay between a heterogeneous photocatalyst and a metal complex, which may lead to new catalytic reactions.
In photocatalytic schemes, it is common practice to employ a sacrificial agent for scavenging photogenerated holes and enhancing the yield and efficiency of electron harvesting. However, little attention is paid to the chemistry triggered by hole-mediated oxidation. Here, we trace the chemical fate of aliphatic alcohols used as hole scavengers in the photoinduced synthesis of Au nanoparticles. Under the action of visible light and the [AuCl4](-) precursor, the alcohol undergoes a sequence of reactions, including oxidation, C-C bond scission, and chlorination, to form a chloroalkane and a carbonyl compound. Mechanistic and parametric studies show that this atypical chemistry is activated by the Lewis-acidic metal center of [AuCl4](-) and enhanced by photoexcited carriers generated by interband excitation of Au nanoparticles. This work presents a unique example of interplay between a heterogeneous photocatalyst and a metal complex. Exploiting such synergy can be a route to new catalytic reactions.
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