In this paper, a convenient method to fabricate flexible and free-standing surface-enhanced Raman scatting (SERS) substrates for direct bacteria detection without aptamer bonding is presented. SiO2 nanofibers were prepared via electrospinning and calcination by using tetraethyl orthosilicate as the precursor. Subsequently, it was coated with polydopamine (PDA) by self-polymerization. Finally, Ag@PDA@SiO2 nanofibrous membranes were obtained through in situ growth of Ag nanoparticles in Tollens’ reagents. The as-prepared Ag@PDA@SiO2 composite nanofibrous membranes were characterized by techniques of scanning electron microscopy, transmission electron microscopy, X-ray powder diffraction, energy-dispersive x-ray spectroscopy and thermo gravimetric analysis. The flexibility of the as-prepared nanofibrous membranes were verified simply through manual folding. Small molecule probes of 4-mercaptophenol (4-MPh) and 4-mercaptobenzoic acid (4-MBA) were chosen to investigate the SERS sensitivity of the as-prepared Ag@PDA@SiO2 as free-standing substrates. Furthermore, Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus), as typical strains of Gram-negative and Gram-positive bacteria, were performed to directly SERS detection by dropping bacteria suspension onto the fibrous membranes without any previous treatment, such as aptamer combination. In addition, the antimicrobial properties of the as-prepared Ag@PDA@SiO2 electrospinning nanofibrous membranes were tested by inhibition zone and turbidity methods. The results show that Ag nanoparticles with an average diameter of 50 nm are uniformly deposited on the surface of electrospinning nanofibers, and the as-prepared Ag@PDA@SiO2 nanofibrous membranes are flexible. As SERS substrates, it shows a rather high detection limitation of 10−11 mol l−1 for 4-MPh and 4-MBA. More importantly, this substrate can be applied for bacteria label-free SERS detection, i.e., complicated procedures are avoided. Meanwihile, the as-prepared Ag@PDA@SiO2 nanofibrous membranes exhibit excellent antibacterial properties. Thus, it has application prospects in trace bacteria detection and water purification.
In this paper, we propose a facile and cost-effective electrospinning technique to fabricate surface-enhanced Raman scattering (SERS) substrates, which is appropriate for multiple analytes detection. First of all, HAuCl4∙3H2O was added into the TEOS/PVP precursor solution, and flexible SiO2 nanofibers incorporated with gold nanoparticles (SiO2@Au) were prepared by electrospinning and calcination. Subsequently, the nanofibrous membranes were immersed in the tannic acid and 3-aminopropyltriethoxysilane solution for surface modification through Michael addition reaction. Finally, the composite nanofibers (Ag@T-A@SiO2@Au) were obtained by the in-situ growth of Ag nanoparticles on the surfaces of nanofibers with tannic acid as a reducing agent. Due to the synergistic enhancement of Au and Ag nanoparticles, the flexible and self-supporting composite nanofibrous membranes have excellent SERS properties. Serving as SERS substrates, they are extremely sensitive to the detection of 4-mercaptophenol and 4-mercaptobenzoic acid, with an enhancement factor of 108. Moreover, they could be utilized to detect analytes such as pesticide thiram at a low concentration of 10−8 mol/L, and the substrates retain excellent Raman signals stability during the durability test of 60 days. Furthermore, the as-fabricated substrates, as a versatile SERS platform, could be used to detect bacteria of Staphylococcus aureus without a specific and complicated bacteria-aptamer conjugation procedure, and the detection limit is up to 103 colony forming units/mL. Meanwhile, the substrates also show an excellent repeatability of SERS response for S. aureus organelles. Briefly, the prime novelty of this work is the fabrication of Au/Ag bimetallic synergetic enhancement substrates as SERS platform for versatile detection with high sensitivity and stability.
The
fabrication of highly active and free-standing surface-enhanced
Raman scattering (SERS) substrates in a simple and low-cost manner
has been a crucial and urgent challenge in recent years. Herein, SiO2 nanofiber substrates modified with size-tunable Ag nanoparticles
were prepared by the combination of electrospinning and in situ chemical
reduction. The results demonstrate the presence and uniform adsorption
of Ag nanoparticles on the SiO2 matrix surface. The free-standing
composite nanofibrous substrates show high-performance SERS response
toward 4-mercaptophenol and 4-mercaptobenzoic acid, and the detection
limit can be as low as 10–10 mol/L. Most importantly,
the as-prepared substrate as a versatile SERS platform can realize
label-free detection of bio-macromolecules of bacteria, i.e., Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli). Furthermore, the substrates also possess
outstanding antibacterial activities against S. aureus and E. coli. Briefly, the significance
of this study is that size-tunable Ag nanoparticles can be decorated
on SiO2 nanofiber surfaces with triethanolamine as a bridging
and reducing agent through a one-pot reaction, and the as-prepared
nanofibrous membranes are expected to act as a candidate for label-free
SERS detection as well as antibacterial dressing.
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