Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions
The synthesis of alcohols from amines starting material is an excellent, yet challenging, strategy for the preparation of pharmaceuticals and polymers. Here, we developed a versatile, self-sustaining closed-loop multienzymatic platform for the biocatalytic synthesis of a large range of non-commercia...
| Main Authors: | , |
|---|---|
| Format: | Article |
| Published: |
Nature Publishing Group
2018
|
| Subjects: | |
| Online Access: | https://eprints.nottingham.ac.uk/51950/ |
| _version_ | 1848798611075235840 |
|---|---|
| author | Contente, Martina L. Paradisi, Francesca |
| author_facet | Contente, Martina L. Paradisi, Francesca |
| author_sort | Contente, Martina L. |
| building | Nottingham Research Data Repository |
| collection | Online Access |
| description | The synthesis of alcohols from amines starting material is an excellent, yet challenging, strategy for the preparation of pharmaceuticals and polymers. Here, we developed a versatile, self-sustaining closed-loop multienzymatic platform for the biocatalytic synthesis of a large range of non-commercially available products in continuous flow with excellent yields (80>99%), reaction times and optical purity of secondary alcohols (>99 e.e.). This process was also extended to the conversion of biogenic amines into high value alcohols, such as the powerful anti-oxidant hydroxytyrosol, and the synthesis of enantiopure 2-arylpropanols via dynamic kinetic resolution of commercially affordable racemic amines. The system exploits the in situ immobilisation of transaminases and redox enzymes which were combined to cater for a fully automated, ultra-efficient synthetic platform with cofactor recycling, in-line recovery of benign by-products and recirculation of the aqueous media containing the recycled cofactors in catalytic amount, which increases the efficiency of the system by over 20-fold. |
| first_indexed | 2025-11-14T20:22:31Z |
| format | Article |
| id | nottingham-51950 |
| institution | University of Nottingham Malaysia Campus |
| institution_category | Local University |
| last_indexed | 2025-11-14T20:22:31Z |
| publishDate | 2018 |
| publisher | Nature Publishing Group |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | nottingham-519502020-05-04T19:39:37Z https://eprints.nottingham.ac.uk/51950/ Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions Contente, Martina L. Paradisi, Francesca The synthesis of alcohols from amines starting material is an excellent, yet challenging, strategy for the preparation of pharmaceuticals and polymers. Here, we developed a versatile, self-sustaining closed-loop multienzymatic platform for the biocatalytic synthesis of a large range of non-commercially available products in continuous flow with excellent yields (80>99%), reaction times and optical purity of secondary alcohols (>99 e.e.). This process was also extended to the conversion of biogenic amines into high value alcohols, such as the powerful anti-oxidant hydroxytyrosol, and the synthesis of enantiopure 2-arylpropanols via dynamic kinetic resolution of commercially affordable racemic amines. The system exploits the in situ immobilisation of transaminases and redox enzymes which were combined to cater for a fully automated, ultra-efficient synthetic platform with cofactor recycling, in-line recovery of benign by-products and recirculation of the aqueous media containing the recycled cofactors in catalytic amount, which increases the efficiency of the system by over 20-fold. Nature Publishing Group 2018-06-04 Article PeerReviewed Contente, Martina L. and Paradisi, Francesca (2018) Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions. Nature Catalysis . ISSN 2520-1158 Biocatalysis; Enzymes; Flow chemistry; Synthetic chemistry; methodology; Sustainability https://www.nature.com/articles/s41929-018-0082-9 doi:10.1038/s41929-018-0082-9 doi:10.1038/s41929-018-0082-9 |
| spellingShingle | Biocatalysis; Enzymes; Flow chemistry; Synthetic chemistry; methodology; Sustainability Contente, Martina L. Paradisi, Francesca Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions |
| title | Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions |
| title_full | Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions |
| title_fullStr | Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions |
| title_full_unstemmed | Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions |
| title_short | Self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions |
| title_sort | self-sustaining closed-loop multienzyme mediated conversion of amines into alcohols in continuous reactions |
| topic | Biocatalysis; Enzymes; Flow chemistry; Synthetic chemistry; methodology; Sustainability |
| url | https://eprints.nottingham.ac.uk/51950/ https://eprints.nottingham.ac.uk/51950/ https://eprints.nottingham.ac.uk/51950/ |