To develop a smart free-standing surface enhanced Raman scattering(SERS) substrate,silver nanoparticles(AgNPs) embedded temperature-sensitive nanofibrous membrane was fabricated by electrospinning their aqueous soluti...To develop a smart free-standing surface enhanced Raman scattering(SERS) substrate,silver nanoparticles(AgNPs) embedded temperature-sensitive nanofibrous membrane was fabricated by electrospinning their aqueous solution containing the copolymer poly(N-isopropylacrylamide-co-Nhydroxymethylacrylamide),followed by heat treatment to form crosslinking structure within its constituent nanofibers.To avoid negative effect of the additive like stabilizer and the reactant like reductant on their SERS efficiency,the AgNPs were in-situ synthesized through reducing Ag^+ions dissolved in the polymer solution by ultraviolet irradiation.The prepared hybrid nanofibrous membrane with high stability in aqueous medium can reach its swelling or deswelling equilibrium state within 15 seconds with the medium temperature changing between 25℃and 50℃alternately.When it was used as a free-standing SERS substrate,10^-12 mol/L of 4-nitrothiophenol in aqueous solution can be detected at room temperature,and elevating detection temperature can further lower its low detection limit.Since its generated SERS signal has desirable reproducibility,it can be used as SERS substrate for quantitative analysis.Moreover,the hybrid membrane as SERS substrate is capable of real-time monitoring the reduction of 4-nitrothiophenol into 4-aminothiophenol catalyzed by its embedded AgNPs,and the detected intermediate indicates that the reaction proceeds via a condensation route.展开更多
In the pursuit of advancing molecular sensing through surface-enhanced Raman spectroscopy(SERS),the combination of plasmonic nanoparticles and metal-organic frameworks(MOFs)has emerged as a highly effective approach t...In the pursuit of advancing molecular sensing through surface-enhanced Raman spectroscopy(SERS),the combination of plasmonic nanoparticles and metal-organic frameworks(MOFs)has emerged as a highly effective approach to enhance the sensitivity and selectivity of SERS substrates.However,most prior investigations have predominantly focused on MOF-coated plasmonic nanoparticles in core@shell or layer-by-layer configurations,leaving a notable knowledge gap in exploring alternative configurations.Herein we present a facile method to construct a particle-on-mirror architecture by selectively coating a MOF,zeolitic imidazolate framework-8(ZIF-8),onto the tips of Au nanostars and subsequently depositing the resultant nanoparticles onto a Au film.This design integrates the electric field enhancement at the sharp tips and nanogaps,along with the molecular enrichment function within the porous MOF immobilized at the tips and nanogaps,leading to a substantial boost in the SERS signal intensity.Such a unique SERS platform enables consistent and outstanding SERS performance for analytes of different sizes.This work opens up a promising strategy for constructing multifunctional nanostructures for sensitive SERS detection in real-life scenarios.展开更多
Plasmonic surface of flexible multilayered nanofibers possesses special superiority for the surface-enhanced Raman scattering(SERS)sensing of molecules and microbial cells.However,the fabrication of flexible plasmonic...Plasmonic surface of flexible multilayered nanofibers possesses special superiority for the surface-enhanced Raman scattering(SERS)sensing of molecules and microbial cells.However,the fabrication of flexible plasmonic nanofibers with high sensitivity and reproducibility is difficult.Herein,we report a smart strategy for fabricating flexible plasmonic fibers,in which compact and homogeneous gold nanoparticles(Au NPs)are in-situ grown on the high-curvature surface of multilayered fibers of electrospun polyvinylidene fluoride(PVDF).Firstly,the surface of PVDF fibers is changed electrically,and Au seeds are deposited on the surface of PVDF fibers using electrostatic driving force.Secondly,a stable AuI_(4)−complex is formed employing coordination between I−and AuCl4−ions,which could decrease the reduction potential of AuCl4−and restrain the self-nucleation,and then the reduction reaction of AuI4−is initiated by introducing PVDF@Au seeds to pull down the barrier of potential energy.Finally,in-situ growth of AuNPs is generated on the high-curvature surface of PVDF nanofibers,and large-scale hotspots are generated by adjacent AuNPs coupling in the three-dimensional(3D)space of multilayered fibers.Membrane of PVDF@Au nanofibers also realizes the sensitive detection of thiram molecules(low limit of detection of 0.1 nM)and good reproducibility(relative standard deviation of 10.6%).Meanwhile,due to the multilayered construction of PVDF@Au nanofibers,a valid SERS signal on 3D surface of bacteria could be generated.3D distribution of hotspots on multilayered PVDF@Au nanofibers gives a clear advantage for SERS sensing of organic molecules and microbial cells.展开更多
A new method for preparing SERS-active substrate was reported. The prefabricated silver substrate was immersed into the mixture of silver enhancer and initiator for several seconds and then rinsed by tridistilled wate...A new method for preparing SERS-active substrate was reported. The prefabricated silver substrate was immersed into the mixture of silver enhancer and initiator for several seconds and then rinsed by tridistilled water. The measurements of the UV-Vis adsorption spectra and AFM show that the average particle size increases with increasing the immersing time. The optimum immersing time is 20 s. Furthermore, the measurements of the SERS spectra of BPENB indicate that such substrate could be kept active for more than 90 d.展开更多
基金the National Natural Science Foundation of China(Nos.51503033,51373030)
文摘To develop a smart free-standing surface enhanced Raman scattering(SERS) substrate,silver nanoparticles(AgNPs) embedded temperature-sensitive nanofibrous membrane was fabricated by electrospinning their aqueous solution containing the copolymer poly(N-isopropylacrylamide-co-Nhydroxymethylacrylamide),followed by heat treatment to form crosslinking structure within its constituent nanofibers.To avoid negative effect of the additive like stabilizer and the reactant like reductant on their SERS efficiency,the AgNPs were in-situ synthesized through reducing Ag^+ions dissolved in the polymer solution by ultraviolet irradiation.The prepared hybrid nanofibrous membrane with high stability in aqueous medium can reach its swelling or deswelling equilibrium state within 15 seconds with the medium temperature changing between 25℃and 50℃alternately.When it was used as a free-standing SERS substrate,10^-12 mol/L of 4-nitrothiophenol in aqueous solution can be detected at room temperature,and elevating detection temperature can further lower its low detection limit.Since its generated SERS signal has desirable reproducibility,it can be used as SERS substrate for quantitative analysis.Moreover,the hybrid membrane as SERS substrate is capable of real-time monitoring the reduction of 4-nitrothiophenol into 4-aminothiophenol catalyzed by its embedded AgNPs,and the detected intermediate indicates that the reaction proceeds via a condensation route.
基金supported by Hong Kong Innovation and Technology Commission(Innovation and Technology Support Programme(Seed),No.ITS/176/22)Shenzhen Science and Technology Innovation Commission(No.JSGGKQTD20221101115701006)+1 种基金the University Development Fund(No.UDF01002665)the Program of Guangdong Introducing Innovative and Entrepreneurial Teams(No.2019ZT08L101).
文摘In the pursuit of advancing molecular sensing through surface-enhanced Raman spectroscopy(SERS),the combination of plasmonic nanoparticles and metal-organic frameworks(MOFs)has emerged as a highly effective approach to enhance the sensitivity and selectivity of SERS substrates.However,most prior investigations have predominantly focused on MOF-coated plasmonic nanoparticles in core@shell or layer-by-layer configurations,leaving a notable knowledge gap in exploring alternative configurations.Herein we present a facile method to construct a particle-on-mirror architecture by selectively coating a MOF,zeolitic imidazolate framework-8(ZIF-8),onto the tips of Au nanostars and subsequently depositing the resultant nanoparticles onto a Au film.This design integrates the electric field enhancement at the sharp tips and nanogaps,along with the molecular enrichment function within the porous MOF immobilized at the tips and nanogaps,leading to a substantial boost in the SERS signal intensity.Such a unique SERS platform enables consistent and outstanding SERS performance for analytes of different sizes.This work opens up a promising strategy for constructing multifunctional nanostructures for sensitive SERS detection in real-life scenarios.
基金This work is supported by the National Natural Science Foundation of China(No.81801122)Natural Science Basic Research Program of Shaanxi(No.2020JQ-529)+4 种基金Scientific Research Program Funded by Shaanxi Provincial Education Department(No.20JK0658)The industry-University-Research collaborative innovation project of Keqiao Textile Industry Innovation Institute of Xi’an Polytechnic University(No.19KQZD01)Xi’an Science and Technology Project(GXYD7.3)Key R&D projects of Shaanxi(No.2020GY-273)Project of China National Textile Industry Association(No.2020047)。
文摘Plasmonic surface of flexible multilayered nanofibers possesses special superiority for the surface-enhanced Raman scattering(SERS)sensing of molecules and microbial cells.However,the fabrication of flexible plasmonic nanofibers with high sensitivity and reproducibility is difficult.Herein,we report a smart strategy for fabricating flexible plasmonic fibers,in which compact and homogeneous gold nanoparticles(Au NPs)are in-situ grown on the high-curvature surface of multilayered fibers of electrospun polyvinylidene fluoride(PVDF).Firstly,the surface of PVDF fibers is changed electrically,and Au seeds are deposited on the surface of PVDF fibers using electrostatic driving force.Secondly,a stable AuI_(4)−complex is formed employing coordination between I−and AuCl4−ions,which could decrease the reduction potential of AuCl4−and restrain the self-nucleation,and then the reduction reaction of AuI4−is initiated by introducing PVDF@Au seeds to pull down the barrier of potential energy.Finally,in-situ growth of AuNPs is generated on the high-curvature surface of PVDF nanofibers,and large-scale hotspots are generated by adjacent AuNPs coupling in the three-dimensional(3D)space of multilayered fibers.Membrane of PVDF@Au nanofibers also realizes the sensitive detection of thiram molecules(low limit of detection of 0.1 nM)and good reproducibility(relative standard deviation of 10.6%).Meanwhile,due to the multilayered construction of PVDF@Au nanofibers,a valid SERS signal on 3D surface of bacteria could be generated.3D distribution of hotspots on multilayered PVDF@Au nanofibers gives a clear advantage for SERS sensing of organic molecules and microbial cells.
文摘A new method for preparing SERS-active substrate was reported. The prefabricated silver substrate was immersed into the mixture of silver enhancer and initiator for several seconds and then rinsed by tridistilled water. The measurements of the UV-Vis adsorption spectra and AFM show that the average particle size increases with increasing the immersing time. The optimum immersing time is 20 s. Furthermore, the measurements of the SERS spectra of BPENB indicate that such substrate could be kept active for more than 90 d.
