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Frontiers of Materials Science

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ISSN 2095-0268(Online)

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Front. Mater. Sci.    2021, Vol. 15 Issue (3) : 431-447    https://doi.org/10.1007/s11706-021-0565-5
RESEARCH ARTICLE
Polymer-capped gold nanoparticles and ZnO nanorods form binary photocatalyst on cotton fabrics: Catalytic breakdown of dye
Bharat BARUAH1(), Christopher KELLEY1, Grace B. DJOKOTO2, Kelly M. HARTNETT2
1. Department of Chemistry and Biochemistry, Kennesaw State University, Kennesaw, GA 30144-5591, USA
2. Division of Natural Sciences, Oglethorpe University, Atlanta, GA 30319, USA
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Abstract

This work reports the immobilization of zinc oxide (ZnO) nanostructures and gold nanoparticles (AuNPs) on cotton fabrics (CFs). The ZnO and AuNPs containing CF composite materials demonstrated excellent photocatalytic activity towards degradation of the model organic dye molecule. A two-step method was used to first create zinc oxide nanorods (ZnONRs) on the CF fibers. Subsequently, these ZnONRs were decorated with cationic polymer-capped AuNPs to yield the composite materials. A one-pot synthetic route was developed to synthesize polymer-capped AuNPs. The water-soluble cationic polymers used here are polyguanidino oxanorbornenes (PGONs) at 20 kDa and polyamino oxanorbornenes (PAONs) at 20 kDa. UV–vis was utilized to monitor the composite materials’ photocatalytic activity in degrading model organic dye molecules. All the materials were characterized by FTIR, UV–visible DRS, SEM, EDX, and XRD. The composite materials exhibited excellent photocatalytic activity and recyclability in the presence of UV light.
Keywords cationic polymer      polymer-capped nanoparticles      ZnO nanorods      fabric      photocatalysis     
Corresponding Author(s): Bharat BARUAH   
Online First Date: 02 September 2021    Issue Date: 24 September 2021
 Cite this article:   
Bharat BARUAH,Christopher KELLEY,Grace B. DJOKOTO, et al. Polymer-capped gold nanoparticles and ZnO nanorods form binary photocatalyst on cotton fabrics: Catalytic breakdown of dye[J]. Front. Mater. Sci., 2021, 15(3): 431-447.
 URL:  
https://academic.hep.com.cn/foms/EN/10.1007/s11706-021-0565-5
https://academic.hep.com.cn/foms/EN/Y2021/V15/I3/431
Fig.1  Scheme 1 Illustration of the creation of CF-based binary composite materials.
Fig.2  Digital pictures (upper) and corresponding SEM images (lower) of different composites: (a)(a?) CF; (b)(b?) ZnONR?CF; (c)(c?) AuNP?PAON?ZnONR?CF; (d)(d?) AuNP?PGON?ZnONR?CF.
Fig.3  EDX spectra of bare CF, ZnONR?CF, AuNP?PAON?ZnONR?CF, and AuNP?PGON?ZnONR?CF.
Fig.4  (a) Vibrational signals of solid PAON (black line) and AuNP?PAON (red line) conjugates (solid AuNP?PAON samples are created by centrifuging the colloidal conjugate and discarding the supernatant). (b) FTIR spectra of PGON (black line) and AuNP?PGON (red line) conjugates (samples created similar to the method of AuNP?PAON). Insets show the molecular structures of PAON and PGON.
Sample νN−H/cm−1 νC=O/cm−1 νC−N(aryl)/cm−1 νC−N(alkyl)/cm−1
PAON 3540 1670/1697 1185 1129
AuNP?PAON 3521 1705 1198 1136
PGON 3196/3352 1679 1263 1142
AuNP?PGON 3204/3360 1662 1315 1147
Tab.1  FTIR signal assignments of PAON, AuNP?PAON, PGON, and AuNP?PGON
Fig.5  XRD motifs of bare CF (a), ZnONR?CF (b), AuNP?PAON?ZnONR?CF (c), and AuNP?PGON?ZnONR?CF (d).
Fig.6  UV?visible DRS spectra of bare CF, ZnONR?CF, AuNP?PAON?ZnONR?CF, and AuNP?PGON?ZnONR?CF.
Fig.7  Depiction of the catalytic breakdown of RhB under UV light with and without photocatalyst: the continuous drop in the absorption maxima of RhB at 553 nm indicates the photocatalytic activity of (a) AuNP?PAON?ZnONR?CF and (b) AuNP?PGON?ZnONR?CF; the plots of photocatalytic degradation of RhB with various composites of (c)At/A0 against time and (d) ln(At/A0) against time.
Catalyst load Degradation (min/%) k/(10−3 s−1) Diameter/nm of AuNP/ZnO Dye/(c/(μmol·L−1)) Light Ref.
ZnO/Au 60/100 2.75 ~37/(100–150) MB/30 UV [38]
GNP/ZnO (10 mg/80 mL) 60/100 1.04 42/100 MO/6.11 UV [39]
4%Au–ZnO (50 mg/50 mL) 450/84 0.027 ~20/162 R6G/21.0 UV [40]
ZnO–rGO–Au (1 mg·mL−1) 32/– 3.09–3.43 (20–50)/(40–750) R6G/10.0 UV [41]
ZnO–Au ((25–100) mg/50 mL) (60–270)/c dependent 0.15–0.49 –/150 R6G/20.0 sunlight [42]
Au–ZnO (40 mg/100 mL) 70/98 7.17 ~20/(2000–3000) RhB/10.0 UV [34]
Au–ZnONRs ((3 cm × 1 cm)/4 mL) 60/30 0.65 (7.0–23)/(50–100) MB/10.0 visible [43]
rGO–Au–ZnO (10 mg/50 mL) 40/96 1.08 (30–100)/~20 RhB/40 UV [44]
2x-Au–ZnONRs (4 mg/50 mL) 180/45 0.059 40/500 RhB/10.4 visible [45]
AuNP@ZnO urchin-like (100 mg/100 mL) 60/– 0.38 (8.0–25)/(100–200) MB/30.3 UV [46]
Au/ZnO/rGO foam (3.57 mg/50 mL) 180/94 0.24 ~50/100 RhB/10.4 UV [24]
Au/ZnO/CPS ((1.5 cm × 1.5 cm)/25 mL) 90/97 0.63 ~50/~100 RhB/10.4 UV [15]
rGO/Au/ZnO (3.57 mg/50 mL) 30/c dependent 0.24 (11.0–48)/100 MB/(5.0–25) sunlight [14]
CF–ZnONRs–AuNPs ((0.9 cm × 3 cm)/3.0 mL) 90/98 0.38 ~18/69 RhB/8.0 UV [29]
AuNP–PAON–ZnONR–CF, AuNP–PGON–?ZnONR–CF ((0.9 cm × 3 cm)/3.0 mL) 50/(99–100) 1.26/1.75 ~6.9/182 RhB/8.0 UV this work
Tab.2  Photocatalytic activity comparison of ZnONRs?AuNP nanocomposites for dye degradation
Fig.8  The possible mechanism of catalytic breakdown of RhB by binary photocatalyst, AuNP–ZnONR–CF in the presence of UV light.
Fig.9  (a) Catalytic decomposition of RhB by AuNP–PGON–ZnONR–CF without (black line) and with radical trapping agents. (b) Demonstration of reusability of photocatalyst, AuNP–PGON–ZnONR–CF up to five catalytic cycles.
  Fig. S1 UV?vis spectra of NaAuCl4 aqueous solution (black line) (A), aqueous solution of PGON (red dashed line) (B), aqueous solution of PAON (blue dashed line) (C), AuNP?PGON colloid (red line) (D), and AuNP?PAON colloid (blue line) (E). Corresponding digital photographs are depicted in the inset.
  Fig. S2 SEM images of CF, ZnONR?CF, and AuNP?PAON?ZnONR?CF, and AuNP?PGON?ZnONR?CF at 2.0–4.0 µmol·L−1 scale.
  Fig. S3 TEM images of (a) AuNP?PAON and (b) AuNP?PGON colloids. Images were taken with a Hitachi H-7500 transmission electron microscope at an accelerating voltage of 120 kV. Samples were prepared by spreading a drop of aqueous sample on an ultrathin 300 mesh Formvar/carbon-film on copper grid and dried in air. The insets show the size distribution of AuNPs.
  Fig. S4 Assessment of photocatalytic degradation of 8.0 µmol·L−1 RhB by UV?visible absorption spectroscopy under 365 nm UV light and in the presence and absence of composite materials. The absorbance at 554 nm continuously decreases as a result of the photocatalytic activity of (a) CF and (b) ZnONR?CF.
  Fig. S5(a) The UV?visible absorption spectra of 50 µmol·L−1 benzidine and Au3+ concentration from 0.0 to 18.0 µmol·L−1 at pH 2.0. The inset shows the 425 nm absorbnace region of 5.0–18.0 µmol·L−1 Au3+. (b) The linear calibration curve of Au3+ identification is monitoring the absorbance at 425 nm against various concentrations of Au3+. The inset shows the digital picture of the colorimetric variation of Au3+ and benzidine complex formation.
  Fig. S6(a) The changes in the UV?visible absorption spectra of 50 µmol·L−1 8-hydroxyquinoline in absence (black line) and presence of various concentrations of Zn2+ from 1.0 (blue line) to 12.5 µmol·L−1 (pink line) Zn2+; the red line represents only 50 µmol·L−1 Zn2+ in absence of 8-hydroxyquinoline. (b) Linear calibration plot for Zn2+ detection considering absorbance at 254 nm against Zn2+ concentration.
Sample ηa(ZnO)/% ηa(Au)/% UV light ηal(ZnO)/% ηal(Au)/%
CF?ZnO?NRs 2.55±0.22 – no
CF?ZnO?NRs 2.13±0.60 – yes 0.046±0.004
AuNP?PAON?ZnONR?CF 2.27±0.56 0.087±0.016 no 0.0
AuNP?PAON?ZnONR?CF 2.24±0.14 0.084±0.007 yes 0.039±0.011 0.0
AuNP?PGON?ZnONR?CF 2.29±0.16 0.089±0.006 no 0.0
AuNP?PGON?ZnONR?CF 2.25±0.22 0.085±0.014 yes 0.038±0.007 0.0
  Table S1 Amount of ZnO and Au loaded on the CF and leach of ZnO and Au after photocatalytic reaction under UV light determined by the UV?visible spectroscopic method with the help of clibration curves shown in Figs. S5 and S6
  Fig. S7 UV?visible spectra: (a) 20 µmol·L−1 BQ in the absence of UV light (i), 20 µmol·L−1 BQ in UV light for 90 min (ii), 20 µmol·L−1 BQ without UV light after 90 min (iii), and 20 µmol·L−1 BQ in UV light in the presence of PhC (photocatalyst, AuNP?PGON?ZnONR?CF) for 90 min (iv); (b) 20 µmol·L−1 TPA-Na (sodium salt of terephthalic acid) (i), 20 µmol·L−1 TPA-Na in UV light for 45 min (ii), 20 µmol·L−1 TPA-Na without UV light after 90 min (iii), and 20 µmol·L−1 TPA-Na in UV light in the presence of PhC (photocatalyst, AuNP?PGON?ZnONR?CF) for 45 min (iv).
  Fig. S8 SEM image and digital picture of of AuNP?PGON?ZnONR?CF after the use in five photocatalytic cycles.
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