[Show abstract][Hide abstract] ABSTRACT: The carbon dots in this study were small carbon nanoparticles with the particle surface functionalized by oligomeric poly(ethylene glycol) diamine molecules. Upon photoexcitation the brightly fluorescent carbon dots in aqueous solution served the function of excellent electron donors to reduce platinum(IV) and gold(III) compounds into their corresponding metals to be deposited on the dot surface. The deposited metals even in very small amount were found to have dramatic quenching effects on the fluorescence emission intensities, but essentially no effects on the observed fluorescence decays. The obviously exclusive near-neighbor static quenching could be attributed to the disruption of electron-hole radiative recombinations (otherwise responsible for the fluorescence emissions in carbon dots). The results provide important evidence for the availability of photo-generated electrons that could be harvested for productive purposes, which in turn supports the current mechanistic framework on fluorescence emission and photoinduced redox properties of carbon dots.
[Show abstract][Hide abstract] ABSTRACT: Carbon nanomaterials have generated a tremendous amount of attention in the scientific community. While most of the research and development efforts have been on fullerenes, carbon nanotubes, and graphene sheets, carbon nanoparticles (which are often considered as impurities or unwanted complications in the other carbon nanomaterials) have recently emerged as a unique class of highly fluorescent nano-dots. However, little or no attention has been paid to potential uses of carbon nanoparticles as chromophores in photochemical reactions or for photon harvesting and photoconversion in general. In the study reported herein we demonstrate the chromophore-equivalent functions of aqueous-suspended small carbon nanoparticles in harvesting visible photons for the reductive coating of the nanoparticles with silver and gold and, as a result, the preparation of unique carbon-noble-metal core-shell nanostructures.
[Show abstract][Hide abstract] ABSTRACT: Increasing atmospheric CO(2) levels have generated much concern, driving the ongoing carbon sequestration effort. A compelling CO(2) sequestration option is its photocatalytic conversion to hydrocarbons, for which the use of solar irradiation represents an ultimate solution. Here we report a new strategy of using surface-functionalized small carbon nanoparticles to harvest visible photons for subsequent charge separation on the particle surface in order to drive the efficient photocatalytic process. The aqueous solubility of the catalysts enables photoreduction under more desirable homogeneous reaction conditions. Beyond CO(2) conversion, the nanoscale carbon-based photocatalysts are also useful for the photogeneration of H(2) from water under similar conditions.
Journal of the American Chemical Society 03/2011; 133(13):4754-7. DOI:10.1021/ja200804h · 12.11 Impact Factor