Abstract
Photocatalytic hydrogen evolution activity of CdS QDs is 175 times higher in pH neutral water when surface capping ligands are removed.
Highlights
Converting the energy in sunlight into chemical fuels is a potential solution to meet our need for sustainable energy storage.[1,2,3] Many synthetic systems have been developed with the hope of emulating natural photosynthesis to produce renewable fuels such as H2
quantum dots (QDs) used in photocatalytic systems have previously been functionalised with hydrophilic, thiol-based ligands, such as thioglycolic acid (TGA), 3-mercaptopropionic acid (MPA), or dihydrolipoic acid (DHLA), in order to prevent aggregation and to induce solubility in aqueous solution
We propose that desorption of surface capping groups is integral to QD/catalyst activity and show that the use of bare QDs results in a two orders of magnitude increase in catalytic rate compared to the equivalent MPA-capped QD/catalyst system
Summary
Converting the energy in sunlight into chemical fuels is a potential solution to meet our need for sustainable energy storage.[1,2,3] Many synthetic systems have been developed with the hope of emulating natural photosynthesis to produce renewable fuels such as H2. QDs used in photocatalytic systems have previously been functionalised with hydrophilic, thiol-based ligands, such as thioglycolic acid (TGA), 3-mercaptopropionic acid (MPA), or dihydrolipoic acid (DHLA), in order to prevent aggregation and to induce solubility in aqueous solution. These capping ligands are not innocent and have been proposed to have secondary roles such as acting as a physical[33] or electronic barrier.[34] They have been shown to interfere with co-catalysts by denaturing enzymes,[19] and by altering metal-based. Na2SO3 buffer solutions were titrated with dilute HCl to the desired pH value at 25 C
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