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Bergman, Matthew E.; Bhardwaj, Mridula; Phillips, Michael A.
Plant journal, July 2021, 2021-07-00, 20210701, Letnik: 107, Številka: 2Journal Article
Summary Geraniol, citronellol and their esters are high‐value acyclic monoterpenes used in food technology, perfumery and cosmetics. A major source of these compounds is the essential oil of rose‐scented geraniums of the genus Pelargonium. We provide evidence that their biosynthesis mainly takes place in the cytosol of glandular trichomes via geranyl monophosphate (GP) through the action of a Nudix hydrolase. Protein preparations could convert geranyl diphosphate (GDP) to geraniol in in vitro assays, a process which could be blocked by inorganic phosphatase inhibitors, suggesting a two‐step conversion of GDP to geraniol. Pelargonium graveolens chemotypes enriched in either geraniol or (−)‐citronellol accumulate GP or citronellyl monophosphate (CP), respectively, the presumed precursors to their monoterpenoid end products. Geranyl monophosphate was highly enriched in isolated glandular trichomes of lines producing high amounts of geraniol. In contrast, (−)‐isomenthone‐rich lines are depleted in these prenyl monophosphates and monoterpene alcohols and instead feature high levels of GDP, the precursor to plastidic p‐menthane biosynthesis. A Nudix hydrolase cDNA from Pelargonium glandular trichomes, dubbed PgNdx1, encoded a cytosolic protein capable of hydrolyzing GDP to GP with a KM of about 750 nm but is only weakly active towards farnesyl diphosphate. In citronellol‐rich lines, GDP, GP and CP were detected in nearly equimolar amounts, while citronellyl diphosphate was absent, suggesting that citronellol biosynthesis may proceed by reduction of GP to CP in this species. These findings highlight the cytosol as a compartment that supports monoterpene biosynthesis and expands the roles of Nudix hydrolases in the biosynthesis of plant volatiles. Significance Statement Monoterpenes are ordinarily synthesized from geranyl diphosphate in the plastid, but rose‐scented geraniums make acyclic monoterpenes such as geraniol from geranyl monophosphate in the cytosol of glandular trichomes. We show the involvement of a Nudix hydrolase in this process, a family of enzymes with emerging roles in plant terpenoid metabolism.
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