| Full text | |
| Author(s): |
Total Authors: 4
|
| Affiliation: | [1] Univ Sao Paulo, Inst Chem Sao Carlos, Dept Phys Chem, BR-13566590 Sao Carlos, SP - Brazil
[2] Univ Colorado, Dept Chem & Biol Engn, Boulder, CO 80309 - USA
Total Affiliations: 2
|
| Document type: | Journal article |
| Source: | Journal of Physical Chemistry Letters; v. 11, n. 22, p. 9714-9724, NOV 19 2020. |
| Web of Science Citations: | 0 |
| Abstract | |
While single-molecule (SM) methods have provided new insights to various catalytic processes, bimolecular reactions have been particularly challenging to study. Here, the fluorogenic Knoevenagel condensation of an aromatic aldehyde with methyl cyanoacetate promoted by surface-immobilized piperazine is quantitatively characterized using super-resolution fluorescence imaging and stochastic analysis using hidden Markov modeling (HMM). Notably, the SM results suggest that the reaction follows the iminium intermediate pathway before the formation of a fluorescent product with intramolecular charge-transfer character. Moreover, the overall process is limited by the turnover rate of the catalyst, which is involved in multiple steps along the reaction coordinate. (AU) | |
| FAPESP's process: | 18/17660-7 - Organic reaction at single molecule level: synthesis of a fluorescent imidazole |
| Grantee: | Larissa Schumekel Foltran |
| Support Opportunities: | Scholarships in Brazil - Scientific Initiation |
| FAPESP's process: | 18/22159-5 - Molecular diffusion, trapping and reaction of polymeric catalysts at the solution-solid interface investigated by single molecule fluorescence microscopy |
| Grantee: | Marcelo Henrique Gehlen |
| Support Opportunities: | Scholarships abroad - Research |