Universität zu Köln

Quan, Zhiyang, Hou, Anwei, Goldfuss, Bernd and Dickschat, Jeroen S. (2022). Mechanism of the Bifunctional Multiple Product Sesterterpene Synthase AcAS from Aspergillus calidoustus. Angew. Chem.-Int. Edit., 61 (13). WEINHEIM: WILEY-V C H VERLAG GMBH. ISSN 1521-3773

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Abstract

The multiproduct chimeric sesterterpene synthase AcAS from Aspergillus calidoustus yielded spirocyclic calidoustene, which exhibits a novel skeleton, besides five known sesterterpenes. The complex cyclisation mechanism to all six compounds was investigated by isotopic labelling experiments in combination with DFT calculations. Chemically synthesised 8-hydroxyfarnesyl diphosphate was converted with isopentenyl diphosphate and AcAS into four oxygenated sesterterpenoids that structurally resemble cytochrome P450 oxidation products of the sesterterpene hydrocarbons. Protein engineering of AcAS broadened the substrate scope and gave significantly improved enzyme yields.

Item Type:	Journal Article
Creators:	Creators Email ORCID ORCID Put Code Quan, Zhiyang UNSPECIFIED UNSPECIFIED UNSPECIFIED Hou, Anwei UNSPECIFIED UNSPECIFIED UNSPECIFIED Goldfuss, Bernd UNSPECIFIED UNSPECIFIED UNSPECIFIED Dickschat, Jeroen S. UNSPECIFIED UNSPECIFIED UNSPECIFIED
URN:	urn:nbn:de:hbz:38-667183
DOI:	10.1002/anie.202117273
Journal or Publication Title:	Angew. Chem.-Int. Edit.
Volume:	61
Number:	13
Date:	2022
Publisher:	WILEY-V C H VERLAG GMBH
Place of Publication:	WEINHEIM
ISSN:	1521-3773
Language:	English
Faculty:	Unspecified
Divisions:	Unspecified
Subjects:	no entry
Uncontrolled Keywords:	Keywords Language GENOME MINING APPROACH; OPHIOBOLIN F SYNTHASE; TERPENE SYNTHASES; BIOSYNTHESIS; DISCOVERY; REVEALS Multiple languages Chemistry, Multidisciplinary Multiple languages
URI:	http://kups.ub.uni-koeln.de/id/eprint/66718