Abstract
The continuous development of total synthesis chemistry has allowed many organic and biomolecules to be produced with known synthetic history–that is, a complete set of step reactions in their synthetic routes. Here, we extend such molecular-level precise reaction routes to nanochemistry, particularly to a seed-mediated synthesis of inorganic nanoparticles. By systematically investigating the time−dependent abundance of 35 intermediate species in total, we map out relevant step reactions in a model size growth reaction from molecularly pure Au25 to Au44 nanoparticles. The size growth of Au nanoparticles involves two different size−evolution processes (monotonic LaMer growth and volcano-shaped aggregative growth), which are driven by a sequential 2-electron boosting of the valence electron count of Au nanoparticles. Such fundamental findings not only provide guiding principles to produce other sizes of Au nanoparticles (e.g., Au38), but also represent molecular-level insights on long-standing puzzles in nanochemistry, including LaMer growth, aggregative growth, and digestive ripening.
Highlights
The continuous development of total synthesis chemistry has allowed many organic and biomolecules to be produced with known synthetic history–that is, a complete set of step reactions in their synthetic routes
The success of these theories has fueled the advances of synthetic chemistry of NPs in the past several decades, a lack of molecular-level understanding of growth mechanisms of NPs has become a significant bottleneck in advancing synthetic chemistries, especially in precisely customizing structural attributes of NPs for basic and applied explorations
The synthesis of [Au25(p-MBA)18]− was conducted according to a reported carbon monoxide (CO)-mediated reduction method[30]
Summary
The continuous development of total synthesis chemistry has allowed many organic and biomolecules to be produced with known synthetic history–that is, a complete set of step reactions in their synthetic routes We extend such molecular-level precise reaction routes to nanochemistry, to a seed-mediated synthesis of inorganic nanoparticles. Several recent studies successfully revealed the homogenous nucleation mechanism of Au NPs both theoretically and experimentally, suggesting the importance of chemical states and reduction pathways of Au(I) precursors in Au NP synthesis[39,40,41,42] While these understandings shed some light on fundamental homogeneousnucleation-growth of Au NPs (i.e., from Au(I) precursors to stable Au NCs), a similar molecular-level understanding on the important heterogeneous-nucleation-growth This is possibly due to the difficulty in controlling the growth of NCs at atomic precision while keeping their protecting ligands unaltered
Sign-in/Register to view highlights & summary Sign-in/Register to access full text options 
Talk to us
Join us for a 30 min session where you can share your feedback and ask us any queries you have
Schedule a callDisclaimer: All third-party content on this website/platform is and will remain the property of their respective owners and is provided on "as is" basis without any warranties, express or implied. Use of third-party content does not indicate any affiliation, sponsorship with or endorsement by them. Any references to third-party content is to identify the corresponding services and shall be considered fair use under The CopyrightLaw.
