Browsing by Author "Leng, Weinan"
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- Aerosol microdroplets exhibit a stable pH gradientWei, Haoran; Vejerano, Eric P.; Leng, Weinan; Huang, Qishen; Willner, Marjorie R.; Marr, Linsey C.; Vikesland, Peter J. (2018-07-10)Suspended aqueous aerosol droplets (< 50 mu m) are microreactors for many important atmospheric reactions. In droplets and other aquatic environments, pH is arguably the key parameter dictating chemical and biological processes. The nature of the droplet air/water interface has the potential to significantly alter droplet pH relative to bulk water. Historically, it has been challenging to measure the pH of individual droplets because of their inaccessibility to conventional pH probes. In this study, we scanned droplets containing 4-mercaptobenzoic acid-functionalized gold nanoparticle pH nanoprobes by 2D and 3D laser confocal Raman microscopy. Using surface-enhanced Raman scattering, we acquired the pH distribution inside approximately 20-mu m-diameter phosphate-buffered aerosol droplets and found that the pH in the core of a droplet is higher than that of bulk solution by up to 3.6 pH units. This finding suggests the accumulation of protons at the air/water interface and is consistent with recent thermodynamic model results. The existence of this pH shift was corroborated by the observation that a catalytic reaction that occurs only under basic conditions (i.e., dimerization of 4-aminothiophenol to produce dimercaptoazobenzene) occurs within the high pH core of a droplet, but not in bulk solution. Our nanoparticle probe enables pH quantification through the cross-section of an aerosol droplet, revealing a spatial gradient that has implications for acid-base-catalyzed atmospheric chemistry.
- Green Manufacturing and Direct Recycling of Lithium-Ion BatteriesLu, Yingqi (Virginia Tech, 2020-09-03)According to the International Energy Agency, the global Electric Vehicle (EV) sales are experiencing approximately 24% annual growth and the total market could reach 4 million in 2020 and 21.5 million by 2030. However, the mass production of lithium-ion batteries (LIBs) to power EV creates concerns over environmental impacts and the long-term sustainability of critical elements for producing the major battery components. Although much investment has been made, it is still imperative to develop an effective LIB production and recycling process. This dissertation demonstrates a green and sustainable paradigm for LIBs where the batteries are manufactured and direct recycled to form a closed loop. The water-based cathode electrode delivers comparable cycle life and rate performance to the ones from the conventional organic solvent-based process. The direct recycling process has the advantages to regenerate the cathode material from electrode instead of decomposing into elements. Utilization of a water-soluble binder enables separating the cathode compound from spent electrodes using water, which is then successfully regenerated to deliver comparable electrochemical performance to the pristine one. When scaled up, the degraded cathode material can be directly regenerated by an optimized relithiation thermal synthesis (RTS) method to resynthesize the homogeneous cathode powder of high quality. The key factors and sintering procedures are studied to ensure the performance of the product. The pilot scale test successfully scales up to Kg-level with recycled output materials delivering good electrochemical performance. To automate the direct recycling process and improve the efficiency, machine learning and sensors are utilized in a novel battery disassembly platform. It can classify different batteries based on their types and sizes. The processing temperature is instantly monitored using thermal imager, and the prediction model is trained to give the prediction for measures taken by a closed loop control system. Furthermore, the image recognition is employed for quality control after the cutting process and the defect can be mitigated to ensure effective dismantling of End-of-life (EOL) batteries. The integration of machine learning techniques makes the elaborate dismantling process safer and more efficient.
- Inward and outward effectiveness of cloth masks, a surgical mask, and a face shieldPan, Jin; Harb, Charbel; Leng, Weinan; Marr, Linsey C. (Virginia Tech, 2020-11-20)We evaluated the effectiveness of 11 face coverings for material filtration efficiency, inward protection efficiency on a manikin, and outward protection efficiency on a manikin. At the most penetrating particle size, the vacuum bag, microfiber cloth, and surgical mask had material filtration efficiencies >50%, while the other materials had much lower filtration efficiencies. However, these efficiencies increased rapidly with particle size, and many materials had efficiencies >50% at 2 μm and >75% at 5 μm. The vacuum bag performed best, with efficiencies of 54-96% for all three metrics, depending on particle size. The thin acrylic and face shield performed worst. Inward protection efficiency and outward protection efficiency were similar for many masks; the two efficiencies diverged for stiffer materials and those worn more loosely (e.g., bandana) or more tightly (e.g., wrapped around the head) compared to a standard earloop mask. Discrepancies between material filtration efficiency and inward/outward protection efficiency indicated that the fit of the mask was important. We calculated that the particle size most likely to deposit in the respiratory tract when wearing a mask is ∼2 μm. Based on these findings, we recommend a three-layer mask consisting of outer layers of a flexible, tightly woven fabric and an inner layer consisting of a material designed to filter out particles. This combination should produce an overall efficiency of >70% at the most penetrating particle size and >90% for particles 1 μm and larger if the mask fits well.
- Preparation and evaluation of nanocellulose-gold nanoparticle nanocomposites for SERS applicationsWei, Haoran; Rodriguez, Katia; Renneckar, Scott; Leng, Weinan; Vikesland, Peter J. (The Royal Society of Chemistry, 2015-06-09)Nanocellulose is of research interest due to its extraordinary optical, thermal, and mechanical properties. The incorporation of guest nanoparticles into nanocellulose substrates enables production of novel nanocomposites with a broad range of applications. In this study, gold nanoparticle/bacterial cellulose (AuNP/BC) nanocomposites were prepared and evaluated for their applicability as surface-enhanced Raman scattering (SERS) substrates. The nanocomposites were prepared by citrate mediated in situ reduction of Au3+ in the presence of a BC hydrogel at 303 K. Both the size and morphology of the AuNPs were functions of the HAuCl4 and citrate concentrations. At high HAuCl4 concentrations, Au nanoplates form within the nanocomposites and are responsible for high SERS enhancements. At lower HAuCl4 concentrations, uniform nanospheres form and the SERS enhancement is dependent on the nanosphere size. The time-resolved increase in the SERS signal was probed as a function of drying time with SERS ‘hot-spots’ primarily forming in the final minutes of nanocomposite drying. The application of the AuNP/BC nanocomposites for detection of the SERS active dyes MGITC and R6G as well as the environmental contaminant atrazine is illustrated as is its use under low and high pH conditions. The results indicate the broad applicability of this nanocomposite for analyte detection.
- Protein-aided formation of triangular silver nanoprisms with enhanced SERS performanceGeng, Xi; Leng, Weinan; Carter, Nathan A.; Vikesland, Peter J.; Grove, Tijana Z. (Royal Society of Chemistry, 2016-05-10)In this work, we present a modified seed-mediated synthetic strategy for the growth of silver nanoprisms with low shape polydispersity, narrow size distribution and tailored plasmonic absorbance. During the seed nucleation step, consensus sequence tetratricopeptide repeat (CTPR) proteins are utilized as potent stabilizers to facilitate the formation of planar-twinned Ag seeds. Ag nanoprisms were produced in high yield in a growth solution containing ascorbic acid and CTPR-stabilized Ag seeds. From the time-course UV-Vis and transmission electron microscopy (TEM) studies, we postulate that the growth mechanism is the combination of facet selective lateral growth and thermodynamically driven Ostwald ripening. The resultant Ag nanotriangles (NTs) exhibit excellent surface enhanced Raman spectroscopy (SERS) performance. The enhancement factor (EF) measured for the 4-mercapto benzoic acid (4-MBA) reporter is estimated to be 3.37 × 105 in solution and 2.8 × 106 for the SERS substrate.
- Pulmonary Exposure to Magnéli Phase Titanium Suboxides Results in Significant Macrophage Abnormalities and Decreased Lung FunctionMcDaniel, Dylan K.; Ringel-Scaia, Veronica M.; Morrison, Holly A.; Coutermarsh-Ott, Sheryl; Council-Troche, McAlister; Angle, Jonathan W.; Perry, Justin B.; Davis, Grace; Leng, Weinan; Minarchick, Valerie; Yang, Yi; Chen, Bo; Reece, Sky W.; Brown, David A.; Cecere, Thomas E.; Brown, Jared M.; Gowdy, Kymberly M.; Hochella, Michael F. Jr.; Allen, Irving C. (Frontiers, 2019-11-28)Coal is one of the most abundant and economic sources for global energy production. However, the burning of coal is widely recognized as a significant contributor to atmospheric particulate matter linked to deleterious respiratory impacts. Recently, we have discovered that burning coal generates large quantities of otherwise rare Magnéli phase titanium suboxides from TiO2 minerals naturally present in coal. These nanoscale Magnéli phases are biologically active without photostimulation and toxic to airway epithelial cells in vitro and to zebrafish in vivo. Here, we sought to determine the clinical and physiological impact of pulmonary exposure to Magnéli phases using mice as mammalian model organisms. Mice were exposed to the most frequently found Magnéli phases, Ti6O11, at 100 parts per million (ppm) via intratracheal administration. Local and systemic titanium concentrations, lung pathology, and changes in airway mechanics were assessed. Additional mechanistic studies were conducted with primary bone marrow derived macrophages. Our results indicate that macrophages are the cell type most impacted by exposure to these nanoscale particles. Following phagocytosis, macrophages fail to properly eliminate Magnéli phases, resulting in increased oxidative stress, mitochondrial dysfunction, and ultimately apoptosis. In the lungs, these nanoparticles become concentrated in macrophages, resulting in a feedback loop of reactive oxygen species production, cell death, and the initiation of gene expression profiles consistent with lung injury within 6 weeks of exposure. Chronic exposure and accumulation of Magnéli phases ultimately results in significantly reduced lung function impacting airway resistance, compliance, and elastance. Together, these studies demonstrate that Magnéli phases are toxic in the mammalian airway and are likely a significant nanoscale environmental pollutant, especially in geographic regions where coal combustion is a major contributor to atmospheric particulate matter.
- Room temperature seed mediated growth of gold nanoparticles: mechanistic investigations and life cycle assesmentLeng, Weinan; Pati, Paramjeet; Vikesland, Peter J. (The Royal Society of Chemistry, 2015-08-04)In this study, we report the first room temperature seed-mediated synthesis of gold nanoparticles (AuNPs) in the presence of citrate and a gold salt. In contrast to citrate-reduction in boiling water, these mild reaction conditions provide expanded capacity to probe the mechanism of seed-mediated growth following gold salt addition. Moreover, comparative life cycle assessment indicates significant reductions in the environmental impacts for the room temperature synthesis. For this study, highly uniform gold seeds with Z-average diameter of 17.7 +/- 0.8 nm and a polydispersity index of 0.03 +/- 0.01 were prepared by a pH controlled protocol. We investigated the AuNP growth mechanism via time resolved UV-vis spectroscopy, dynamic light scattering, and transmission electron microscopy. This study indicates that citrate and its oxidation byproduct acetone dicarboxylate serve to bridge and gather Au(iii) ions around gold nanoparticle seeds in the initial growth step.
- Scalable Electrochemical Surface Enhanced Raman Spectroscopy (EC-SERS) for bio-chemical analysisXiao, Chuan (Virginia Tech, 2021-10-06)Conducting vertical nanopillar arrays can serve as three-dimensional nanostructured electrodes with improved performance for electrical recording and electrochemical sensing in bio-electronics applications. However, vertical nanopillar-array electrodes made of inorganic conducting materials by conventional nanofabrication approach still faces challenges in high manufacturing costs, poor scalability, and limited choice of carrier substrates. Here, we report a new type of conducting nanopillar arrays composed of multi-walled carbon nanotubes (MWCNTs) doped polymeric nanocomposites, which are manufactured over the wafer-scale on both rigid and flexible substrates by direct nanoimprinting of perfluoropolyether nanowell-array templates into uncured MWCNT/polymer mixtures. By controlling the MWCNT ratios and the annealing temperatures during the fabrication process, MWCNT/polymer nanopillar arrays can possess outstanding electrical properties with high DC conductivity (~4 S/m) and low AC electrochemical impedance (~104 Ω at 1000 Hz). Moreover, by electrochemical impedance spectroscopy (EIS) measurements and equivalent circuit modeling-analysis, we can decompose the overall impedance of MWCNT/polymer nanopillar arrays in the electrolyte into multiple bulk and interfacial circuit components, and thus can illustrate their different dependence on the MWCNT ratios and the annealing temperatures. In particular, we find that a proper annealing process can significantly reduce the anomalous ion diffusion impedance and improve the impedance properties of MWCNT/polymer nanopillars in the electrolyte.