An Amendment to the Understanding of the Heterogeneous Catalytic Properties of Nanoparticles by Dye-assisted Single-molecule Nanocatalysis
DescriptionNanoparticles are important catalysts for many chemical transformations. However, they areintrinsically heterogeneous and challenging to characterize in ensemble measurements. By asingle-nanoparticle single-turnover approach with assistance of resazurin, although the catalyticproperty of individual Au nanoparticles in solution has been proposed, the following reduction ofcatalytic product, resorufin, to dihydroresorufin was not considered as contributor to the catalyticturnover cycle. In this present project, using single-molecule detection of fluorogenic reactions underboth anaerobic and aerobic condition, we diagnose the contribution of reaction between resorufin anddihydroresorufin in the catalytic turnover cycle which directly impacts the estimating heterogeneouscatalytic properties of nanoparticles through product generation and dissociation on the substrate ofAu nanoparticles. Meanwhile, the same approach is applied to resazurin reduction catalyzed bygraphene oxide, exemplifying the power of the single-molecule approach in revealing the interplay ofcatalysis, heterogeneous reactivity and surface structural dynamics in graphene nanocatalysis.
|Effective start/end date||1/02/19 → …|