Digitizing protocols into single reactors for the one-pot synthesis of nanomaterials

Nanomaterials exhibit unique properties that are tunable depending on their morphology and composition. However, widely used methods can fail due to incomplete or assumed knowledge of the synthesis protocol. A digital synthesis method could unambiguously capture the synthesis process, including required hardware, reagent inputs, and process description, thereby increasing accessibility and improving reproducibility. Our method encodes synthetic procedures into single reactors by imprinting synthetic parameters to the reactor’s morphology, which are described using a chemical description language, χDL. This approach is consolidated into three single reactors that automate complex processes such as one-time, dropwise, and sequential addition for the synthesis of eight time-resolved CdSe quantum dots, CdSe@ZnSe core-shell nanoparticles, and Pt-Fe3O4 Janus nanoparticles, respectively. This method of translating synthetic parameters into physical instances of a reactor enables the automation of nanomaterial synthesis in a simple, reliable, and reproducible manner, making nanomaterials accessible to researchers from various fields on demand

Silanol-Assisted Carbinolamine Formation in an Amine-Functionalized Mesoporous Silica Surface: Theoretical Investigation by Fragmentation Methods

The aldol reaction catalyzed by an amine-substituted mesoporous silica nanoparticle (amine-MSN) surface was investigated using a large molecular cluster model (Si392O958C6NH361) combined with the surface integrated molecular orbital/molecular mechanics (SIMOMM) and fragment molecular orbital (FMO) methods. Three distinct pathways for the carbinolamine formation, the first step of the amine-catalyzed aldol reaction, are proposed and investigated in order to elucidate the role of the silanol environment on the catalytic capability of the amine-MSN material. The computational study reveals that the most likely mechanism involves the silanol groups actively participating in the reaction, forming and breaking covalent bonds in the carbinolamine step. Therefore, the active participation of MSN silanol groups in the reaction mechanism leads to a significant reduction in the overall energy barrier for the carbinolamine formation. In addition, a comparison between the findings using a minimal cluster model and the Si392O958C6NH361 cluster suggests that the use of larger models is important when heterogeneous catalysis problems are the target

Interaction of Mesoporous Silica Nanoparticles with Human Red Blood Cell Membranes: Size and Surface Effects

The interactions of mesoporous silica nanoparticles (MSNs) of different particle sizes and surface properties with human red blood cell (RBC) membranes were investigated by membrane filtration, flow cytometry, and various microscopic techniques. Small MCM-41-type MSNs (∼100 nm) were found to adsorb to the surface of RBCs without disturbing the membrane or morphology. In contrast, adsorption of large SBA-15-type MSNs (∼600 nm) to RBCs induced a strong local membrane deformation leading to spiculation of RBCs, internalization of the particles, and eventual hemolysis. In addition, the relationship between the degree of MSN surface functionalization and the degree of its interaction with RBC, as well as the effect of RBC−MSN interaction on cellular deformability, were investigated. The results presented here provide a better understanding of the mechanisms of RBC−MSN interaction and the hemolytic activity of MSNs and will assist in the rational design of hemocompatible MSNs for intravenous drug delivery and in vivo imaging