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. 2021 Feb 15;13(4):581.
doi: 10.3390/polym13040581.

α-Cellulose Fibers of Paper-Waste Origin Surface-Modified with Fe3O4 and Thiolated-Chitosan for Efficacious Immobilization of Laccase

Gajanan S Ghodake  1 , Surendra K Shinde  1 , Ganesh D Saratale  2 , Rijuta G Saratale  3 , Min Kim  4 , Seung-Cheol Jee  4 , Dae-Young Kim  1 , Jung-Suk Sung  4 , Avinash A Kadam  3
Affiliations

α-Cellulose Fibers of Paper-Waste Origin Surface-Modified with Fe3O4 and Thiolated-Chitosan for Efficacious Immobilization of Laccase

Gajanan S Ghodake et al. Polymers (Basel). .

Abstract

The utilization of waste-paper-biomass for extraction of important α-cellulose biopolymer, and modification of extracted α-cellulose for application in enzyme immobilization can be extremely vital for green circular bio-economy. Thus, in this study, α-cellulose fibers were super-magnetized (Fe3O4), grafted with chitosan (CTNs), and thiol (-SH) modified for laccase immobilization. The developed material was characterized by high-resolution transmission electron microscopy (HR-TEM), HR-TEM energy dispersive X-ray spectroscopy (HR-TEM-EDS), X-ray diffraction (XRD), vibrating sample magnetometer (VSM), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FT-IR) analyses. Laccase immobilized on α-Cellulose-Fe3O4-CTNs (α-Cellulose-Fe3O4-CTNs-Laccase) gave significant activity recovery (99.16%) and laccase loading potential (169.36 mg/g). The α-Cellulose-Fe3O4-CTNs-Laccase displayed excellent stabilities for temperature, pH, and storage time. The α-Cellulose-Fe3O4-CTNs-Laccase applied in repeated cycles shown remarkable consistency of activity retention for 10 cycles. After the 10th cycle, α-Cellulose-Fe3O4-CTNs possessed 80.65% relative activity. Furthermore, α-Cellulose-Fe3O4-CTNs-Laccase shown excellent degradation of pharmaceutical contaminant sulfamethoxazole (SMX). The SMX degradation by α-Cellulose-Fe3O4-CTNs-Laccase was found optimum at incubation time (20 h), pH (3), temperatures (30 °C), and shaking conditions (200 rpm). Finally, α-Cellulose-Fe3O4-CTNs-Laccase gave repeated degradation of SMX. Thus, this study presents a novel, waste-derived, highly capable, and super-magnetic nanocomposite for enzyme immobilization applications.

Keywords: chitosan; laccase immobilization; super-magnetic; waste-paper-biomass; α-Cellulose.

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Conflict of interest statement

There is no conflict of interest.

Figures

Figure 1
Figure 1
Schematic presentation of a chemical scheme for laccase immobilization on α-Cellulose-Fe3O4-CTNs-SH and its environmental application.
Figure 2
Figure 2
High-resolution transmission electron microscopy (HR-TEM) image of (A) α-Cellulose-Fe3O4-CTNs-SH, (B) Zoomed view of the α-Cellulose-Fe3O4-CTNs-SH HR-TEM image, (C) high-angle annular dark-field imaging (HAADF) analysis of the α-Cellulose-Fe3O4-CTNs-SH, HR-TEM HAADF elemental mapping (D) carbon (C), (E) oxygen (O), (F) nitrogen (N), (G) iron (Fe), and (I) sulfur (S), and (J) HR-TEM EDS profile of the α-Cellulose-Fe3O4-CTNs-SH.
Figure 3
Figure 3
XRD analysis of the α-Cellulose-Fe3O4-CTNs-SH.
Figure 4
Figure 4
Vibrating sample magnetometer (VSM) analysis of the α-Cellulose-Fe3O4-CTNs-SH.
Figure 5
Figure 5
(A) XPS analysis of the α-Cellulose-Fe3O4-CTNs-SH-Laccase, and (B) high-resolution Fe 2p XPS spectrum of α-Cellulose-Fe3O4-CTNs-SH-Laccase.
Figure 6
Figure 6
FT-IR analysis of the α-Cellulose-Fe3O4-CTN-SH and α-Cellulose-Fe3O4-CTN-SH-Laccase.
Figure 7
Figure 7
Laccase loading pattern on α-Cellulose-Fe3O4-CTNs-SH, and laccase activity recovery by α-Cellulose-Fe3O4-CTNs-SH-Laccase.
Figure 8
Figure 8
(A) Temperature stability of free and α-Cellulose-Fe3O4-CTNs-SH-Laccase carried out at 60 °C for 180 min time, (B) pH stability study of free and α-Cellulose-Fe3O4-CTNs-SH-Laccase carried out at pH 1–9 for 1 h incubation time, (C) storage stability study of free and α-Cellulose-Fe3O4-CTNs-SH-Laccase carried out at 4 °C and for 30 days, and (D) reusability study of the α-Cellulose-Fe3O4-CTNs-SH-Laccase in 10 cycles.
Figure 9
Figure 9
Effect of time (A), pH (B), temperatures (C), and shaking conditions (D) on SMX degradation by the α-Cellulose-Fe3O4-CTNs-SH-Laccase.
Figure 10
Figure 10
The repeated cycle degradation of SMX by α-Cellulose-Fe3O4-CTNs-SH-Laccase.
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