Synthesis of 3-Amino-4-(Hydroxymethyl)-β-Lactam Branch Point and Its Late-Stage C4 Functionalization with Ceftaroline-Sidechain Monobactams and Their Biological Evaluation
Monocyclic β-lactams are an underexplored subclass of β-lactam antibiotics active against Gram-negative pathogens, but access to them requires long sequences reported across the patent and primary literature. We compare two alternative routes to 3-amino-4-(hydroxymethyl)-2-azetidinone, a synthon carrying handles at N1, C3 and C4, starting from ethyl glyoxylate and from (R)-glyceraldehyde acetonide. Both are assembled from published transformations; reported here are isolated yields for every step, including the conditions that failed, and execution of the β-lactam-forming sequence on a 50 g scale. Removal of the 2,4-dimethoxybenzyl group was strongly concentration-dependent, giving 94% on the glyoxylate-derived ester against 70% on the acetonide-derived alcohol, whereas the acetonide route replaces a low-yielding NaBH4 ester reduction (43 to 57%) with a near-quantitative oxidative cleavage/reduction sequence. Diverting one late-stage intermediate through copper-catalyzed azide–alkyne cycloaddition or direct thioether alkylation gave three sulfonated monobactams bearing a ceftaroline-derived C4 sidechain, in 0.10 to 0.29% overall yield over 15 steps. None reduced S. pneumoniae PBP1b activity below 50% at 100 μM, against an IC50 of 4.93 μM for aztreonam, and none inhibited wild-type E. coli or S. aureus at 128 μg/mL; weak inhibition was seen only in efflux-deficient and outer-membrane-permeabilized E. coli. C4 substitution through either linkage supports activity when the appended group also provides an uptake vector, which the ceftaroline-derived side chain does not, and it conferred no measurable target affinity either.
Authors
- Stanislav Gobec (ORCID: https://orcid.org/0000-0002-9678-3083)
- Majda Golob (ORCID: https://orcid.org/0000-0001-9526-0152)
- Martina Hrast (ORCID: https://orcid.org/0000-0003-0488-2445)
- A. Meden (ORCID: https://orcid.org/0000-0003-3594-6579)
- Vid Kavaš (ORCID: https://orcid.org/0009-0004-7875-3640)
Institutions
- University of Ljubljana (SI)
Publication Details
- Journal
- Molecules
- Published
- 2026-10-12
- DOI
- https://doi.org/10.3390/molecules31203637
- Primary Topic
- Synthesis of β-Lactam Compounds
- Type
- article
- Field-Weighted Citation Impact
- 0.00