Beta-lactam explained

A beta-lactam (β-lactam) ring is a four-membered lactam.[1] A lactam is a cyclic amide, and beta-lactams are named so because the nitrogen atom is attached to the β-carbon atom relative to the carbonyl. The simplest β-lactam possible is 2-azetidinone. β-lactams are significant structural units of medicines as manifested in many β-lactam antibiotics.[2] Up to 1970, most β-lactam research was concerned with the penicillin and cephalosporin groups, but since then, a wide variety of structures have been described.[3] [4]

Clinical significance

See main article: β-Lactam antibiotic. The β-lactam ring is part of the core structure of several antibiotic families, the principal ones being the penicillins, cephalosporins, carbapenems, and monobactams, which are, therefore, also called β-lactam antibiotics. Nearly all of these antibiotics work by inhibiting bacterial cell wall biosynthesis. This has a lethal effect on bacteria, although any given bacteria population will typically contain a subgroup that is resistant to β-lactam antibiotics. Bacterial resistance occurs as a result of the expression of one of many genes for the production of β-lactamases, a class of enzymes that break open the β-lactam ring. More than 1,800 different β-lactamase enzymes have been documented in various species of bacteria.[5] These enzymes vary widely in their chemical structure and catalytic efficiencies.[6] When bacterial populations have these resistant subgroups, treatment with β-lactam can result in the resistant strain becoming more prevalent and therefore more virulent. β-lactam derived antibiotics can be considered one of the most important antibiotic classes but prone to clinical resistance. β-lactam exhibits its antibiotic properties by imitating the naturally occurring d-Ala-d-Ala substrate for the group of enzymes known as penicillin binding proteins (PBP), which have as function to cross-link the peptidoglycan part of the cell wall of the bacteria.[7]

The β-lactam ring is also found in some other drugs such as the cholesterol absorption inhibitor drug ezetimibe.

Synthesis

The first synthetic β-lactam was prepared by Hermann Staudinger in 1907 by reaction of the Schiff base of aniline and benzaldehyde with diphenylketene[8] [9] in a [2+2] cycloaddition (Ph indicates a phenyl functional group):

Many methods have been developed for the synthesis of β-lactams.[10] [11] [12]

The Breckpot β-lactam synthesis produces substituted β-lactams by the cyclization of beta amino acid esters by use of a Grignard reagent.[13] Mukaiyama's reagent is also used in modified Breckpot synthesis.

Reactions

Due to ring strain, β-lactams are more readily hydrolyzed than linear amides or larger lactams. This strain is further increased by fusion to a second ring, as found in most β-lactam antibiotics. This trend is due to the amide character of the β-lactam being reduced by the aplanarity of the system. The nitrogen atom of an ideal amide is sp2-hybridized due to resonance, and sp2-hybridized atoms have trigonal planar bond geometry. As a pyramidal bond geometry is forced upon the nitrogen atom by the ring strain, the resonance of the amide bond is reduced, and the carbonyl becomes more ketone-like. Nobel laureate Robert Burns Woodward described a parameter h as a measure of the height of the trigonal pyramid defined by the nitrogen (as the apex) and its three adjacent atoms. h corresponds to the strength of the β-lactam bond with lower numbers (more planar; more like ideal amides) being stronger and less reactive.[14] Monobactams have h values between 0.05 and 0.10 angstroms (Å). Cephems have h values in of 0.20 - 0.25 Å. Penams have values in the range 0.40 - 0.50 Å, while carbapenems and clavams have values of 0.50 - 0.60 Å, being the most reactive of the β-lactams toward hydrolysis.[15]

See also

External links

Notes and References

  1. Book: Gilchrist T . Heterocyclic Chemistry . Longman Scientific . Harlow . 1987 . 978-0-582-01421-3.
  2. Fisher . J. F. . Meroueh . S. O. . Mobashery . S. . Bacterial resistance to β-lactam antibiotics: compelling opportunism, compelling opportunity . 10.1021/cr030102i . Chemical Reviews . 105 . 2 . 395–424 . 2005 . 15700950.
  3. Book: Flynn EH . Cephalosporins and Penicillins : Chemistry and Biology. 1972. Academic Press. New York and London.
  4. Hosseyni S, Jarrahpour A . Recent advances in β-lactam synthesis . Organic & Biomolecular Chemistry . 16 . 38 . 6840–6852 . October 2018 . 30209477 . 10.1039/c8ob01833b .
  5. Brandt C, Braun SD, Stein C, Slickers P, Ehricht R, Pletz MW, Makarewicz O . In silico serine β-lactamases analysis reveals a huge potential resistome in environmental and pathogenic species . Scientific Reports . 7 . 43232 . February 2017 . 28233789 . 5324141 . 10.1038/srep43232 . 2017NatSR...743232B .
  6. Ehmann DE, Jahić H, Ross PL, Gu RF, Hu J, Kern G, Walkup GK, Fisher SL . Avibactam is a covalent, reversible, non-β-lactam β-lactamase inhibitor . Proceedings of the National Academy of Sciences of the United States of America . 109 . 29 . 11663–8 . July 2012 . 22753474 . 3406822 . 10.1073/pnas.1205073109 . 2012PNAS..10911663E . free .
  7. Tipper DJ, Strominger JL . Mechanism of action of penicillins: a proposal based on their structural similarity to acyl-D-alanyl-D-alanine . Proceedings of the National Academy of Sciences of the United States of America . 54 . 4 . 1133–41 . October 1965 . 5219821 . 219812 . 10.1073/pnas.54.4.1133 . 1965PNAS...54.1133T . free .
  8. Tidwell TT . Hugo (Ugo) Schiff, Schiff bases, and a century of beta-lactam synthesis . Angewandte Chemie . 47 . 6 . 1016–20 . 2008 . 18022986 . 10.1002/anie.200702965 .
  9. Staudinger H . Justus Liebigs Ann. Chem. . Zur Kenntniss der Ketene. Diphenylketen . 1907 . 356 . 1–2 . 51–123 . 10.1002/jlac.19073560106 . Hermann Staudinger . 2019-06-27 . 2020-08-02 . https://web.archive.org/web/20200802214234/https://zenodo.org/record/1427571 . live .
  10. 10.1021/cr0307300. Β-Lactams: Versatile Building Blocks for the Stereoselective Synthesis of Non-β-Lactam Products. 2007. Alcaide. Benito. Almendros. Pedro. Aragoncillo. Cristina. Chemical Reviews. 107. 11. 4437–4492. 17649981.
  11. Hosseyni. Seyedmorteza. Jarrahpour. Aliasghar. 2018. Recent advances in β-lactam synthesis. Organic & Biomolecular Chemistry. en. 16. 38. 6840–6852. 10.1039/C8OB01833B. 30209477. 1477-0520.
  12. Pitts. Cody Ross. Lectka. Thomas. 2014-08-27. Chemical Synthesis of β-Lactams: Asymmetric Catalysis and Other Recent Advances. Chemical Reviews. en. 114. 16. 7930–7953. 10.1021/cr4005549. 24555548. 0009-2665. 2020-12-17. 2022-07-21. https://web.archive.org/web/20220721062126/https://pubs.acs.org/doi/10.1021/cr4005549. live.
  13. Web site: Breckpot Synthesis . Bogdanov B, Zdravkovski Z, Hristovski K . Institute of Chemistry Skopje . 2014-12-30 . 2015-11-06 . https://web.archive.org/web/20151106234526/http://www.pmf.ukim.edu.mk/PMF/Chemistry/reactions/breckpot.htm . dead .
  14. Woodward RB . Penems and related substances . Philosophical Transactions of the Royal Society of London. Series B, Biological Sciences . 289 . 1036 . 239–50 . May 1980 . 6109320 . 10.1098/rstb.1980.0042 . 1980RSPTB.289..239W . free .
  15. Nangia A, Biradha K, Desiraju GR . 1996 . Correlation of biological activity in β-lactam antibiotics with Woodward and Cohen structural parameters: A Cambridge database study . J. Chem. Soc. Perkin Trans. . 2 . 5. 943–53 . 10.1039/p29960000943.