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Why acetaldehyde kills the DERA aldolase

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Crotonaldehyde, the acetaldehyde aldol product, covalently bridges catalytic K167 to nearby C47; a C47M mutant survives 300 mM acetaldehyde.

Source

Mechanism-based inhibition of an aldolase at high concentrations of its natural substrate acetaldehyde: structural insights and protective strategies

Dick M, Hartmann R, Weiergräber OH, et al. · Chemical science · 2016

doi.org/10.1039/c5sc04574fRead the full paper ↗28 citationscc by

What they did

Authors combined crystallography, 13C NMR, and a C47M mutation to learn how E. coli DERA dies in concentrated acetaldehyde and how to protect it for synthesis.

What they found

After 200–300 mM acetaldehyde the enzyme is irreversibly inactivated. Crotonaldehyde forms a Schiff base at K167 and a covalent link to C47. Crotonaldehyde inhibits more than 100-fold more potently than acetaldehyde (1 mM, <1 h). C47 is conserved in 91% of orthologues. C47M keeps 60 ± 5% activity and loses none after 16 h in 300 mM acetaldehyde.

The limits

What it doesn't show

The work does not deliver a process-scale biocatalytic plant or map every aldehyde side product; only one protective mutation is fully characterized.

Key terms

DERA
2-Deoxy-D-ribose-5-phosphate aldolase, an acetaldehyde-dependent C–C enzyme.
Crotonaldehyde
α,β-unsaturated aldehyde from dehydrating the acetaldehyde aldol dimer.
Mechanism-based inhibition
A substrate-derived product that covalently inactivates the enzyme.
C47M
Mutation that removes the nucleophilic cysteine and confers acetaldehyde resistance.
Schiff base at K167
Imine between the catalytic lysine and the donor aldehyde.

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The mechanism-based inhibitor is:

Common questions

What is the true inhibitor?

Crotonaldehyde, not acetaldehyde itself.

Which residues are covalently linked?

Catalytic K167 and nearby C47.

Does C47M still work?

Yes—about 60% wild-type activity and no loss after 16 h in 300 mM acetaldehyde.

How common is C47?

Present in 91% of aligned orthologues.

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