TY - JOUR
T1 - Reversible acetalization of cellulose
T2 - A platform for bio-based materials with adjustable properties and biodegradation
AU - Peil, Stefan
AU - Gojzewski, Hubert
AU - Wurm, Frederik R.
N1 - Funding Information:
This work was supported by NWO XS [21.2.054].
Funding Information:
The authors thank Andreas Hanewald (MPI-P Mainz) and Kaloian Koynov (MPI-P Mainz) for technical assistance and advice with the rheology and stress-strain measurements, Sandra Seywald (MPI-P Mainz) and Christine Rosenauer (MPI-P Mainz) for GPC measurements, Robert Graf (MPI-P Mainz) for solid-state NMR, Petra Räder (MPI-P Mainz) for TGA and DSC support and Elke Muth (MPI-P Mainz) for FT-IR measurements. Clemens Padberg (UT) is acknowledged for SEM imaging. Katharina Landfester (MPI-P Mainz) is acknowledged for continuous support. This work was supported by NWO XS [21.2.054].
Publisher Copyright:
© 2022 The Author(s)
PY - 2023/1/15
Y1 - 2023/1/15
N2 - Bio-based and biodegradable polymers are essential for a sustainable society. Cellulose is the most abundant biopolymer on earth; however, derivatization is necessary for its processing, which slows down its biodegradability dramatically, e.g. used cigarette filters made from cellulose acetate are barely biodegradable. We developed the first reversible modification of cellulose, which allows processing and guarantees full biodegradation even at high degrees of substitution as the linkers, acetals, can be cleaved first during the degradation process releasing native cellulose that biodegrades in a second step. Acetalization is a versatile platform approach to bio-based and fully degradable cellulose-derivatives, which are characterized by solubility in common organic solvents (alcohols, aromatic and chlorinated solvents), adjustable glass transition temperatures (-48 °C < Tg < 80 °C), young's modulus (1.9 MPa < E < 58 MPa) and contact angle (86°< θ < 124°). In contrast to previously known cellulose modifications, cellulose acetals remain fully degradable as the acetal bond is reversible and undergoes an acidic cleavage under desired conditions, for instance in compost, followed by enzymatic degradation of the remaining cellulose backbone. With climate change and plastic pollution, these new and versatile cellulose acetals provide bio-based and biodegradable alternatives to fossil-based and non-degradable polyolefin plastics, leading to a more sustainable future for our planet.
AB - Bio-based and biodegradable polymers are essential for a sustainable society. Cellulose is the most abundant biopolymer on earth; however, derivatization is necessary for its processing, which slows down its biodegradability dramatically, e.g. used cigarette filters made from cellulose acetate are barely biodegradable. We developed the first reversible modification of cellulose, which allows processing and guarantees full biodegradation even at high degrees of substitution as the linkers, acetals, can be cleaved first during the degradation process releasing native cellulose that biodegrades in a second step. Acetalization is a versatile platform approach to bio-based and fully degradable cellulose-derivatives, which are characterized by solubility in common organic solvents (alcohols, aromatic and chlorinated solvents), adjustable glass transition temperatures (-48 °C < Tg < 80 °C), young's modulus (1.9 MPa < E < 58 MPa) and contact angle (86°< θ < 124°). In contrast to previously known cellulose modifications, cellulose acetals remain fully degradable as the acetal bond is reversible and undergoes an acidic cleavage under desired conditions, for instance in compost, followed by enzymatic degradation of the remaining cellulose backbone. With climate change and plastic pollution, these new and versatile cellulose acetals provide bio-based and biodegradable alternatives to fossil-based and non-degradable polyolefin plastics, leading to a more sustainable future for our planet.
KW - Acetal-derivatized
KW - Acetalated
KW - Bio-based
KW - Biodegradable
KW - Compost
KW - Soil-degradable
KW - UT-Hybrid-D
UR - http://www.scopus.com/inward/record.url?scp=85139064510&partnerID=8YFLogxK
U2 - 10.1016/j.cej.2022.139280
DO - 10.1016/j.cej.2022.139280
M3 - Article
AN - SCOPUS:85139064510
SN - 1385-8947
VL - 452
JO - Chemical Engineering Journal
JF - Chemical Engineering Journal
IS - Part 3
M1 - 139280
ER -