TY - JOUR
T1 - Reducing end thiol-modified nanocellulose: Bottom-up enzymatic synthesis and use for templated assembly of silver nanoparticles into biocidal composite material
AU - Zhong, Chao
AU - Nidetzky, Bernd
PY - 2021/5/15
Y1 - 2021/5/15
N2 - Nanoparticle-polymer composites are important functional materials but structural control of their assembly is challenging. Owing to its crystalline internal structure and tunable nanoscale morphology, cellulose is promising polymer scaffold for templating such composite materials. Here, we show bottom-up synthesis of reducing end thiol-modified cellulose chains by iterative bi-enzymatic β-1,4-glycosylation of 1-thio-β-D-glucose (10 mM), to a degree of polymerization of ∼8 and in a yield of ∼41% on the donor substrate (α-D-glucose 1-phosphate, 100 mM). Synthetic cellulose oligomers self-assemble into highly ordered crystalline (cellulose allomorph II) material showing long (micrometers) and thin nanosheet-like morphologies, with thickness of 5–7 nm. Silver nanoparticles were attached selectively and well dispersed on the surface of the thiol-modified cellulose, in excellent yield (≥ 95%) and high loading efficiency (∼2.2 g silver/g thiol-cellulose). Examined against Escherichia coli and Staphylococcus aureus, surface-patterned nanoparticles show excellent biocidal activity. Bottom-up approach by chemical design to a functional cellulose nanocomposite is presented. Synthetic thiol-containing nanocellulose can expand the scope of top-down produced cellulose materials.
AB - Nanoparticle-polymer composites are important functional materials but structural control of their assembly is challenging. Owing to its crystalline internal structure and tunable nanoscale morphology, cellulose is promising polymer scaffold for templating such composite materials. Here, we show bottom-up synthesis of reducing end thiol-modified cellulose chains by iterative bi-enzymatic β-1,4-glycosylation of 1-thio-β-D-glucose (10 mM), to a degree of polymerization of ∼8 and in a yield of ∼41% on the donor substrate (α-D-glucose 1-phosphate, 100 mM). Synthetic cellulose oligomers self-assemble into highly ordered crystalline (cellulose allomorph II) material showing long (micrometers) and thin nanosheet-like morphologies, with thickness of 5–7 nm. Silver nanoparticles were attached selectively and well dispersed on the surface of the thiol-modified cellulose, in excellent yield (≥ 95%) and high loading efficiency (∼2.2 g silver/g thiol-cellulose). Examined against Escherichia coli and Staphylococcus aureus, surface-patterned nanoparticles show excellent biocidal activity. Bottom-up approach by chemical design to a functional cellulose nanocomposite is presented. Synthetic thiol-containing nanocellulose can expand the scope of top-down produced cellulose materials.
KW - 1-Thio-β-D-glucose (PubChem CID: 444809)
KW - Bottom-up enzymatic synthesis
KW - Crystalline nanocellulose
KW - D-Glucose (PubChem CID: 5793)
KW - Glycoside phosphorylase
KW - Nanoparticle-polymer composite
KW - p-Nitro-phenyl-phosphate (PubChem CID: 378)
KW - Reducing-end thiol group
KW - Silver nitrate (PubChem CID: 24470)
KW - Site-selective attachment
KW - Sodium citrate (PubChem CID: 6224)
KW - α-D-Glucose 1-phosphate (PubChem CID: 65533)
UR - http://www.scopus.com/inward/record.url?scp=85101302173&partnerID=8YFLogxK
U2 - 10.1016/j.carbpol.2021.117772
DO - 10.1016/j.carbpol.2021.117772
M3 - Article
SN - 0144-8617
VL - 260
JO - Carbohydrate Polymers
JF - Carbohydrate Polymers
M1 - 117772
ER -