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Discovery of Hydroxylase Activity for PqqB Provides a Missing Link in the Pyrroloquinoline Quinone Biosynthetic Pathway.

Koehn EM, Latham JA, Armand T, Evans RL, Tu X, Wilmot CM, Iavarone AT, Klinman JP
J Am Chem Soc 141 4398-4405 (2019)
Cited: 17 times
EuropePMC logo PMID: 30811189

Abstract

Understanding the biosynthesis of cofactors is fundamental to the life sciences, yet to date a few important pathways remain unresolved. One example is the redox cofactor pyrroloquinoline quinone (PQQ), which is critical for C1 metabolism in many microorganisms, a disproportionate number of which are opportunistic human pathogens. While the initial and final steps of PQQ biosynthesis, involving PqqD/E and PqqC, have been elucidated, the precise nature and order of the remaining transformations in the pathway are unknown. Here we show evidence that the remaining essential biosynthetic enzyme PqqB is an iron-dependent hydroxylase catalyzing oxygen-insertion reactions that are proposed to produce the quinone moiety of the mature PQQ cofactor. The demonstrated reactions of PqqB are unprecedented within the metallo β-lactamase protein family and expand the catalytic repertoire of nonheme iron hydroxylases. These new findings also generate a nearly complete description of the PQQ biosynthetic pathway.

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  1. A Molecular Revolution in the Treatment of Hemophilia. Butterfield JSS, Hege KM, Herzog RW, Kaczmarek R. Mol Ther 28 997-1015 (2020)
  2. Biogenesis of the peptide-derived redox cofactor pyrroloquinoline quinone. Zhu W, Klinman JP. Curr Opin Chem Biol 59 93-103 (2020)
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Articles - 6e13 mentioned but not cited (2)

  1. Discovery of Hydroxylase Activity for PqqB Provides a Missing Link in the Pyrroloquinoline Quinone Biosynthetic Pathway. Koehn EM, Latham JA, Armand T, Evans RL, Tu X, Wilmot CM, Iavarone AT, Klinman JP. J Am Chem Soc 141 4398-4405 (2019)
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Reviews citing this publication (4)

  1. New developments in RiPP discovery, enzymology and engineering. Montalbán-López M, Scott TA, Ramesh S, Rahman IR, van Heel AJ, Viel JH, Bandarian V, Dittmann E, Genilloud O, Goto Y, Grande Burgos MJ, Hill C, Kim S, Koehnke J, Latham JA, Link AJ, Martínez B, Nair SK, Nicolet Y, Rebuffat S, Sahl HG, Sareen D, Schmidt EW, Schmitt L, Severinov K, Süssmuth RD, Truman AW, Wang H, Weng JK, van Wezel GP, Zhang Q, Zhong J, Piel J, Mitchell DA, Kuipers OP, van der Donk WA. Nat Prod Rep 38 130-239 (2021)
  2. Metallo-β-lactamases in the Age of Multidrug Resistance: From Structure and Mechanism to Evolution, Dissemination, and Inhibitor Design. Bahr G, González LJ, Vila AJ. Chem Rev 121 7957-8094 (2021)
  3. RaS-RiPPs in Streptococci and the Human Microbiome. Clark KA, Bushin LB, Seyedsayamdost MR. ACS Bio Med Chem Au 2 328-339 (2022)
  4. Microbial synthesis of pyrroloquinoline quinone. Gao H, Wang Y, Yang J, Qiu M, Lei Z, Zhang W, Jiang W, Xin F, Jiang M. World J Microbiol Biotechnol 40 31 (2023)

Articles citing this publication (8)

  1. MftD Catalyzes the Formation of a Biologically Active Redox Center in the Biosynthesis of the Ribosomally Synthesized and Post-translationally Modified Redox Cofactor Mycofactocin. Ayikpoe RS, Latham JA. J Am Chem Soc 141 13582-13591 (2019)
  2. Structural Properties and Catalytic Implications of the SPASM Domain Iron-Sulfur Clusters in Methylorubrum extorquens PqqE. Zhu W, Walker LM, Tao L, Iavarone AT, Wei X, Britt RD, Elliott SJ, Klinman JP. J Am Chem Soc 142 12620-12634 (2020)
  3. Biochemical and Structural Characterization of XoxG and XoxJ and Their Roles in Lanthanide-Dependent Methanol Dehydrogenase Activity. Featherston ER, Rose HR, McBride MJ, Taylor EM, Boal AK, Cotruvo JA. Chembiochem 20 2360-2372 (2019)
  4. A two-component protease in Methylorubrum extorquens with high activity toward the peptide precursor of the redox cofactor pyrroloquinoline quinone. Martins AM, Martins AM, Latham JA, Martel PJ, Barr I, Iavarone AT, Klinman JP. J Biol Chem 294 15025-15036 (2019)
  5. Fine-tuning ethanol oxidation pathway enzymes and cofactor PQQ coordinates the conflict between fitness and acetic acid production by Acetobacter pasteurianus. Gao L, Wu X, Xia X, Jin Z. Microb Biotechnol 14 643-655 (2021)
  6. Moving Through Barriers in Science and Life. Klinman JP. Annu Rev Biochem 88 1-24 (2019)
  7. Adaptive evolutionary strategy coupled with an optimized biosynthesis process for the efficient production of pyrroloquinoline quinone from methanol. Ren Y, Yang X, Ding L, Liu D, Tao Y, Huang J, Ke C. Biotechnol Biofuels Bioprod 16 11 (2023)
  8. Phenylalanine meta-Hydroxylase: A Single Residue Mediates Mechanistic Control of Aromatic Amino Acid Hydroxylation. Grüschow S, Sadler JC, Sharratt PJ, Goss RJM. Chembiochem 21 417-422 (2020)


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