Browsing by Author "Rahman, Asifur"

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    Highly porous gold supraparticles as surface-enhanced Raman spectroscopy (SERS) substrates for sensitive detection of environmental contaminants
    Kang, Seju; Wang, Wei; Rahman, Asifur; Nam, Wonil; Zhou, Wei; Vikesland, Peter J. (Royal Society of Chemistry, 2022-11-15)
    Surface-enhanced Raman spectroscopy (SERS) has great potential as an analytical technique for environmental analyses. In this study, we fabricated highly porous gold (Au) supraparticles (i.e., ∼100 μm diameter agglomerates of primary nano-sized particles) and evaluated their applicability as SERS substrates for the sensitive detection of environmental contaminants. Facile supraparticle fabrication was achieved by evaporating a droplet containing an Au and polystyrene (PS) nanoparticle mixture on a superamphiphobic nanofilament substrate. Porous Au supraparticles were obtained through the removal of the PS phase by calcination at 500 °C. The porosity of the Au supraparticles was readily adjusted by varying the volumetric ratios of Au and PS nanoparticles. Six environmental contaminants (malachite green isothiocyanate, rhodamine B, benzenethiol, atrazine, adenine, and gene segment) were successfully adsorbed to the porous Au supraparticles, and their distinct SERS spectra were obtained. The observed linear dependence of the characteristic Raman peak intensity for each environmental contaminant on its aqueous concentration reveals the quantitative SERS detection capability by porous Au supraparticles. The limit of detection (LOD) for the six environmental contaminants ranged from ∼10 nM to ∼10 μM, which depends on analyte affinity to the porous Au supraparticles and analyte intrinsic Raman cross-sections. The porous Au supraparticles enabled multiplex SERS detection and maintained comparable SERS detection sensitivity in wastewater influent. Overall, we envision that the Au supraparticles can potentially serve as practical and sensitive SERS devices for environmental analysis applications.
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    Life Cycle Impact Assessment of Iron Oxide (Fe3O4/γ-Fe2O3) Nanoparticle Synthesis Routes
    Rahman, Asifur; Kang, Seju; McGinnis, Sean; Vikesland, Peter J. (2022)
    The synthesis of superparamagnetic iron oxide nanoparticles (FeOx-NPs) has rapidly developed over the past decade due to their wide-ranging applications in research and technology. However, at present there exists very limited knowledge about the environmental impacts of the various input materials and the energy required for different FeOx-NP synthesis approaches. In this study, we used cradle-to-gate life cycle assessment (LCA) to analyze and compare the environmental impacts of FeOx-NPs produced via seven common synthesis routes. Four different functional units (i.e., mass, mean particle size, specific surface area, and saturation magnetization) were used to normalize the environmental impacts and evaluate the corresponding changes. Overall, physical and biological synthesis routes exhibited high environmental impacts due to their higher input material and energy requirements. Interestingly, biological syntheses had the highest environmental impacts due to their reliance on bacterial culture media. All of the chemical synthesis routes had lower environmental impacts except the thermal decomposition method, which had higher environmental impacts due its use of non-polar organic solvents during synthesis. The lab-scale LCA inventory data and analysis presented here addresses the existing data gaps and helps guide future research for FeOx-NP synthesis under industrial conditions. The information generated by this effort aids in the identification of environmentally friendly and sustainable production pathways for FeOx-NPs.
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    Sustainable Nanomaterials Combined with Raman Spectroscopy-based Techniques to Advance Environmental Sensing
    Rahman, Asifur (Virginia Tech, 2023-02-22)
    The propagation of contaminants in the environment continues to threaten public health and safety. Conventional analytical techniques for environmental detection require centralized facilities and intensive resources for operation. An effective implementation of a wide network of field deployable point-of-use (POU) sensors can potentially enable real-time monitoring of water quality parameters and inform decision making on public health outbreaks. The use of nanotechnology and field-deployable analytical tools can potentially advance the development of POU sensors for future field application. In this dissertation, we developed environmental sensing techniques that utilize nanocomposites made of low-cost, biocompatible, and sustainable nanomaterials combined with Raman spectroscopy. First, a technology pre-assessment was performed that included a comprehensive evaluation of cellulose-derived nanocomposites and nanobiotechnology enabled techniques for their sustainable long-term environmental application. Furthermore, to contribute to the better understanding of the potential environmental implications of nanomaterial production and application, life cycle assessment (LCA) was used to evaluate the environmental impacts of six iron precursors and seven iron oxide nanoparticle synthesis methods. Secondly, in the technology development step, gold (Au) and iron oxide (Fe3O4) nanoparticles were incorporated onto bacterial cellulose nanocrystals and nanoscale magnetite were synthesized. As proof-of-concept environmental applications, the Au@Fe3O4@BCNCs were applied for the magnetic separation and surface-enhanced Raman scattering (SERS) detection of malachite green isothiocyanate (MGITC), and nanoscale magnetite were applied for phosphate (PO43-) removal and recovery from synthetic urine matrices. Finally, in the technological application step, three environmental sensing applications are presented that use nanomaterial-based sensor platforms and/or Raman spectroscopic techniques. The first application involved using Lectin-modified BCNCs coupled SERS and machine learning for discrimination of bacterial strains. The second application presents a simple Raman-stable isotope labeling approach for the study of viral infection of bacteria. The third application involved use of SERS pH nanoprobes for measuring pH in droplets of complex matrices (e.g., DMEM cell culture media, human saliva).