Diaminated Cellulose Beads as a Sustainable Support for Industrially Relevant Lipases
Califano, Davide ; Schoevaart, Rob ; Barnard, Katie E. ; Callaghan, Ciarán ; Mattia, Davide and Edler, Karen J. LU
(2024)
In ACS Sustainable Chemistry and Engineering
12(20).
p.7703-7712
- Abstract
Environmentally persistent polystyrene or polyacrylic beads are used as supports in enzyme large-scale bioprocesses, including conversion glucose isomerization for high-fructose corn syrup production, hydrolysis of lactose, and synthesis of active pharmaceutical ingredients. In this paper, we report the development of a novel sustainable and scalable method to produce diaminated cellulose beads (DAB) as highly efficient alternative supports for industrially relevant lipases. Regenerated cellulose beads were grafted with diaminated aliphatic hydrocarbons via periodate oxidation and reductive amination. The oxidation step indicated that aldehyde content can be easily tuned through the reaction time and concentration of reactants.... (More)
Environmentally persistent polystyrene or polyacrylic beads are used as supports in enzyme large-scale bioprocesses, including conversion glucose isomerization for high-fructose corn syrup production, hydrolysis of lactose, and synthesis of active pharmaceutical ingredients. In this paper, we report the development of a novel sustainable and scalable method to produce diaminated cellulose beads (DAB) as highly efficient alternative supports for industrially relevant lipases. Regenerated cellulose beads were grafted with diaminated aliphatic hydrocarbons via periodate oxidation and reductive amination. The oxidation step indicated that aldehyde content can be easily tuned through the reaction time and concentration of reactants. Reductive amination of dialdehyde cellulose was more efficient as the length of the diaminated hydrocarbon compound increased. Morphological analysis of DAB showed that cellulose chemical grafting enabled the preservation of the bead shape and internal structure upon freeze-drying. Enzymatic degradability studies demonstrated that chemical functionalization did not undermine enzyme cellulose hydrolysis. The addition of aminated moieties on cellulose dramatically increased absorption efficiency for all industrially relevant lipases used, reaching 100% for Thermomyces lanuginosus lipase (TLL). Storage and recyclability experiments demonstrated that enzymes were retained and recyclable for at least nine cycles, although the activity gradually declined after each cycle. Medium chain triacylglycerol hydrolysis in a SpinChem reactor using TLL immobilized on 1,6 DAB exhibited higher activity compared to acrylic beads (588 vs 459 U/g) suggesting that biodegradable cellulose-based materials could be a valid and attractive alternative to plastics carriers.
(Less)
- author
- Califano, Davide
; Schoevaart, Rob
; Barnard, Katie E.
; Callaghan, Ciarán
; Mattia, Davide
and Edler, Karen J.
LU
- publishing date
- 2024
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- biocatalysis, biotransformation, cellulose beads, enzyme immobilization, lipases, mitigation plastic pollution, renewable biodegradable carrier
- in
- ACS Sustainable Chemistry and Engineering
- volume
- 12
- issue
- 20
- pages
- 10 pages
- publisher
- The American Chemical Society (ACS)
- external identifiers
-
- pmid:38783841
- scopus:85192835439
- ISSN
- 2168-0485
- DOI
- 10.1021/acssuschemeng.3c07849
- language
- English
- LU publication?
- no
- additional info
- Publisher Copyright: © 2024 The Authors. Published by American Chemical Society.
- id
- ce08533f-1f5e-4b30-a040-21b14ad19b8b
- date added to LUP
- 2024-05-27 11:28:21
- date last changed
- 2024-10-29 02:53:08
@article{ce08533f-1f5e-4b30-a040-21b14ad19b8b,
abstract = {{<p>Environmentally persistent polystyrene or polyacrylic beads are used as supports in enzyme large-scale bioprocesses, including conversion glucose isomerization for high-fructose corn syrup production, hydrolysis of lactose, and synthesis of active pharmaceutical ingredients. In this paper, we report the development of a novel sustainable and scalable method to produce diaminated cellulose beads (DAB) as highly efficient alternative supports for industrially relevant lipases. Regenerated cellulose beads were grafted with diaminated aliphatic hydrocarbons via periodate oxidation and reductive amination. The oxidation step indicated that aldehyde content can be easily tuned through the reaction time and concentration of reactants. Reductive amination of dialdehyde cellulose was more efficient as the length of the diaminated hydrocarbon compound increased. Morphological analysis of DAB showed that cellulose chemical grafting enabled the preservation of the bead shape and internal structure upon freeze-drying. Enzymatic degradability studies demonstrated that chemical functionalization did not undermine enzyme cellulose hydrolysis. The addition of aminated moieties on cellulose dramatically increased absorption efficiency for all industrially relevant lipases used, reaching 100% for Thermomyces lanuginosus lipase (TLL). Storage and recyclability experiments demonstrated that enzymes were retained and recyclable for at least nine cycles, although the activity gradually declined after each cycle. Medium chain triacylglycerol hydrolysis in a SpinChem reactor using TLL immobilized on 1,6 DAB exhibited higher activity compared to acrylic beads (588 vs 459 U/g) suggesting that biodegradable cellulose-based materials could be a valid and attractive alternative to plastics carriers.</p>}},
author = {{Califano, Davide and Schoevaart, Rob and Barnard, Katie E. and Callaghan, Ciarán and Mattia, Davide and Edler, Karen J.}},
issn = {{2168-0485}},
keywords = {{biocatalysis; biotransformation; cellulose beads; enzyme immobilization; lipases; mitigation plastic pollution; renewable biodegradable carrier}},
language = {{eng}},
number = {{20}},
pages = {{7703--7712}},
publisher = {{The American Chemical Society (ACS)}},
series = {{ACS Sustainable Chemistry and Engineering}},
title = {{Diaminated Cellulose Beads as a Sustainable Support for Industrially Relevant Lipases}},
url = {{http://dx.doi.org/10.1021/acssuschemeng.3c07849}},
doi = {{10.1021/acssuschemeng.3c07849}},
volume = {{12}},
year = {{2024}},
}