High-Voltage Electrodes in Moist Air Accumulate Charge That is Retained after Removing the Electric Field.

Applying a high voltage to a metal electrode that is disconnected from a circuit rapidly induces a capacitive charge, which quickly relaxes after removal of the applied voltage. Here, we report that if the electrode is placed in air at a sufficiently high relative humidity and provided the connection between the high-voltage supply and the electrode is composed of two different metals, the expected capacitive charge is followed by a gradual increase in charge. Surprisingly, this extra charge persists after the removal of the applied voltage and even after physically removing the electrode from the Faraday cup used to measure the charge. We report the median charge, average charge rate, and residual charge for different applied voltages, different metal-metal connections, and varied humidity. We interpret the results in terms of a proposed water ionization mechanism and discuss the implications of the findings for high-voltage fluidic systems.

Acids in coffee: A review of sensory measurements and meta-analysis of chemical composition.

Coffee contains a variety of organic acids (OAs) and chlorogenic acids (CGAs) that contribute to overall sensory properties. Large variations in preparation and measurement methodology across the literature complicate interpretation of general trends. Here, we perform a systematic review and meta-analysis of the published literature to elucidate the concentrations of OAs and CGAs in both Coffea arabica (arabica) and Coffea canephora (robusta), for both green coffee and roasted coffee at multiple roast levels. A total of 129 publications were found to report acid concentration measurements, yielding 8,634 distinct data points. Analysis of the full data set reveals several trends. First, roasted robusta has considerably more acidic compounds than arabica with 2 to 5 times as much total OAs, and much larger amounts of formic and acetic acid. As for CGAs, in both arabica and robusta 5-CQA is the major component, and progressive roasting decreases the concentration of all CGAs. The total amount of CGA present was more dependent on roast level than the type of coffee (arabica vs. robusta). Overall, this meta-analysis suggests that the increases in certain OAs with roast level might play more of a role in the sensory profile of dark roast coffees than previously suspected.

The effect of post-brew holding time and carafe type on the sensory properties of drip brew coffee.

BACKGROUND: Coffee quality is believed to degrade quickly after brewing, and retail establishments discard unsold brewed coffee after a specified holding time period, sometimes as short as 30 min. We used trained sensory panels to evaluate the flavor profiles of light, medium, and dark roast coffees held in three different carafe types (glass on hot plate, thermal jacket, and vacuum insulated) for times ranging from 15 min to 3 h. Furthermore, a panel of 93 coffee-industry professionals performed a blind evaluation of fresh (30 min) versus held (180 min) coffee for overall liking and attribute level adequacy. RESULTS: Sourness increased over time, consistent with acidity increasing over time (i.e., higher titratable acidity, lower pH), but only for the light and medium roasts. Dark roasted coffee became significantly more acidic over 3 h post-brew but was not perceived as more sour over time by the sensory panel. Variations were observed between the thermal jacket and vacuum carafes for the light and dark roast, but few differences were observed with storage type in the medium roast. Surprisingly, the panel of coffee industry professionals showed no preference for fresh over held. CONCLUSIONS: More sensory attributes decreased than increased over time, suggesting that the primary concern with loss of quality during coffee holding may be the loss of volatile aroma compounds. Hedonic ratings suggest that even if the changes over time are noticeable, they may not negatively impact overall liking. © 2022 Society of Chemical Industry.

A perturbation solution to the full Poisson-Nernst-Planck equations yields an asymmetric rectified electric field.

We derive a perturbation solution to the one-dimensional Poisson-Nernst-Planck (PNP) equations between parallel electrodes under oscillatory polarization for arbitrary ionic mobilities and valences. Treating the applied potential as the perturbation parameter, we show that the second-order solution yields a nonzero time-average electric field at large distances from the electrodes, corroborating the recent discovery of Asymmetric Rectified Electric Fields (AREFs) via numerical solution to the full nonlinear PNP equations [Hashemi Amrei et al., Phys. Rev. Lett., 2018, 121, 185504]. Importantly, the first-order solution is analytic, while the second-order AREF is semi-analytic and obtained by numerically solving a single linear ordinary differential equation, obviating the need for full numerical solutions to the PNP equations. We demonstrate that at sufficiently high frequencies and electrode spacings the semi-analytical AREF accurately captures both the complicated shape and the magnitude of the AREF, even at large applied potentials.

Sensory and monosaccharide analysis of drip brew coffee fractions versus brewing time.

BACKGROUND: The composition of drip brew coffee versus brewing time has been chemically characterized in previous studies, and it is known that the total dissolved solids (TDS) systematically decreases with each fraction during the brew. Little information exists regarding the corresponding sensory attributes versus time, however, and it is unclear how TDS correlates with flavor profile. RESULTS: Standard drip brews were fractionated into distinct samples by switching in an empty carafe every 30 s during the brew. Using a trained sensory descriptive panel, we found that most taste and flavor attributes decreased with brew time; for example, the earlier fractions were systematically more bitter and more sour than later fractions. Surprisingly, however, several flavor and taste attributes increased in time; for example, later fractions were systematically sweeter and more floral than earlier fractions. Since later fractions had lower TDS, these results indicate that perceived sweetness in drip brew coffee is negatively correlated with TDS. Mass spectrometry measurements of the monosaccharide content in the brews showed that none of the fractions had perceptible concentrations of any monosaccharide. CONCLUSION: The results of the sensory analysis and the monosaccharide analysis suggest that perceptible sweetness in coffee is a consequence of masking effects and/or the presence of sweet-associated aromas and flavors. The results further suggest that unique flavor profiles could be obtained from the same coffee grounds by judicious combinations of specific fractions. © 2020 Society of Chemical Industry.

Statistical Analysis of Droplet Charge Acquired during Contact with Electrodes in Strong Electric Fields.

Aqueous droplets acquire charge when they contact electrodes in high-voltage electric fields. Although many researchers have investigated droplet charging under various conditions, the droplet charges are typically reported simply in terms of a mean and standard deviation. Here, we show that droplets often acquire significantly less charge for a single contact compared to the previous and subsequent contacts. These "low-charge events," which are not observed with charging of metal balls, yield up to a 60% decrease in charge acquired by the droplet and occur regardless of the applied field strength, droplet conductivity, or droplet volume. In all cases examined here, the occurrence of low-charge events to good approximation follows a negative binomial distribution (i.e., a Pascal distribution) with a mean probability of 13%. We further demonstrate that approximately 16% of charging events are characterized by "irregular" Taylor cone dynamics, suggesting that instabilities in the electrically driven deformation of the approaching liquid interface may be responsible for the low-charge events. The results indicate that workers using systems involving droplet charging should take into account the high likelihood of droplets randomly acquiring less charge than expected.

Extreme Levitation of Colloidal Particles in Response to Oscillatory Electric Fields.

Micron-scale colloidal particles suspended in electrolyte solutions have been shown to exhibit a distinct bifurcation in their average height above the electrode in response to oscillatory electric fields. Recent work by Hashemi Amrei et al. ( Phys. Rev. Lett., 2018, 121, 185504) revealed that a steady, long-range asymmetric rectified electric field (AREF) is formed when an oscillatory potential is applied to an electrolyte with unequal ionic mobilities. In this work, we use confocal microscopy to test the hypothesis that a force balance between gravity and an AREF-induced electrophoretic force is responsible for the particle height bifurcation observed in some electrolytes. We demonstrate that at sufficiently low frequencies, particles suspended in electrolytes with large ionic mobility mismatches exhibit extreme levitation away from the electrode surface (up to 50 particle diameters). This levitation height scales approximately as the inverse square root of the frequency for both NaOH and KOH solutions. Moreover, larger particles levitate smaller distances, while the magnitude of the applied field has little effect above a threshold voltage. A force balance between the AREF-induced electrophoresis and gravity reveals saddle node bifurcations in the levitation height with respect to the frequency, voltage, and particle size, yielding stable fixed points above the electrode that accord with the experimental observations. These results point toward a low-energy, non-fouling method for concentrating colloids at specific locations far from the electrodes.

A spike in mechanotransductive adenosine triphosphate release from red blood cells in microfluidic constrictions only occurs with rare donors.

OBJECTIVE: Wan et al (Proc Natl Acad Sci USA, 105, 2008, 16432) demonstrated that RBCs rapidly and transiently release a spike of 300% more ATP shortly downstream from a short microfluidic constriction where the cells experience a sudden increase in shear stress. More recent work by Cinar et al (Proc Natl Acad Sci USA, 112, 2015, 11783), however, yielded no evidence for a similar spike in ATP release downstream of the constriction. Our aim was to determine whether a transient spike in mechanotransduction is the typical response of RBCs to the sudden onset of increased shear. METHODS: We investigate ATP release downstream of a microfluidic constriction for 15 participants using a luciferase-based photoluminescent assay. RESULTS: While we observe mechanotransductive ATP release from blood drawn from all donors, we find evidence of a spike in ATP concentration after the microfluidic constriction for only 2 of 15 participants. No clear trends in ATP release are found with respect to the magnitude of the applied shear stress, or to the gender, age, or physical activity (Baecke) index of the donor. CONCLUSIONS: In aggregate, all data acquired to date suggest that a spike in mechanotransductive ATP due to a suddenly applied increase in shear stress occurs in blood drawn from only 14% of the population.

Oscillating Electric Fields in Liquids Create a Long-Range Steady Field.

We demonstrate that application of an oscillatory electric field to a liquid yields a long-range steady field, provided the ions present have unequal mobilities. The main physics is illustrated by a two-ion harmonic oscillator, yielding an asymmetric rectified field whose time average scales as the square of the applied field strength. Computations of the fully nonlinear electrokinetic model corroborate the two-ion model and further demonstrate that steady fields extend over large distances between two electrodes. Experimental measurements of the levitation height of micron-scale colloids versus applied frequency accord with the numerical predictions. The heretofore unsuspected existence of a long-range steady field helps explain several long-standing questions regarding the behavior of particles and electrically induced fluid flows in response to oscillatory potentials.

Droplet Conductivity Strongly Influences Bump and Crater Formation on Electrodes during Charge Transfer.

Aqueous droplets acquire charge when they contact electrodes in high voltage electric fields, but the exact mechanism of charge transfer is not understood. Recent work by Elton et al. revealed that electrodes are physically pitted during charge transfer with aqueous droplets. The pits are believed to result when a dielectric breakdown arc occurs as a droplet approaches the electrode and the associated high current density transiently locally melts the electrode, leaving distinct crater-like deformations on the electrode surface. Here we show that the droplet conductivity strongly modulates the pitting morphology but has little effect on the amount of charge transferred. Electron and atomic force microscopy shows that deionized water droplets yield no observable deformations, but as the salt concentration in the droplet increases above 10-3 M, the deformations become increasingly large. The observed intensity of the flash of light released during the dielectric breakdown arc also increases with droplet conductivity. Surprisingly, despite the large difference in pitting morphology and corresponding arc intensity, droplets of any conductivity acquire similar amounts of charge. These results suggest that the energy transferred during dielectric breakdown is primarily responsible for electrode pitting rather than the total amount of energy released during charge transfer.

Measurement of Charge Transfer to Aqueous Droplets in High Voltage Electric Fields.

The electric charge acquired by aqueous droplets when they contact an electrode is a crucial parameter in experimental and industrial applications where electric fields are used to manipulate droplet motion and coalescence. For unclear reasons, many investigators have found that aqueous droplets acquire significantly more positive than negative charge. Extant techniques for determining the droplet charge typically rely on a hydrodynamic force balance that depends on accurate characterization of the drag forces acting on the droplet. Here we present an alternative methodology for measuring the droplet charge via direct measurement of the electric current. As the droplet approaches the electrode the current is observed to gradually increase, followed by a large pulse when the droplet makes apparent contact. We interpret the transient current signals as the superposition of the natural response of an RLC circuit and an induced current described by the Shockley-Ramo theory. Nonlinear regression of the observed current to the theoretical model allows for the droplet charge to be extracted, independent of any assumptions about the force balance on the droplet. We demonstrate that regression of the current signal yields charge values that are on average within 4% of charges measured via a force balance. We use the chronocoulometric methodology to investigate how the charge varies with the applied potential, and we demonstrate that deionized water droplets contacting planar electrodes acquire on average 69% more positive charge than negative charge.

Influence of Electrolyte Concentration on the Aggregation of Colloidal Particles near Electrodes in Oscillatory Fields.

Micron-scale particles suspended in various aqueous electrolytes have been widely observed to aggregate near electrodes in response to oscillatory electric fields, a phenomenon believed to result from electrically induced flows around the particles. Previous work has focused on elucidating the effects of the applied field strength, frequency, and electrolyte type on the aggregation rate of particles, with less attention paid to the ionic strength. Here we demonstrate that an applied field causes micron-scale particles in aqueous NaCl to rapidly aggregate over a wide range of ionic strengths, but with significant differences in aggregation morphology. Optical microscopy observations reveal that at higher ionic strengths (∼1 mM) particles arrange as hexagonally closed-packed (HCP) crystals, but at lower ionic strengths (∼0.05 mM) the particles arrange in randomly closed-packed (RCP) structures. We interpret this behavior in terms of two complementary effects: an increased particle diffusivity at lower ionic strengths due to increased particle height over the electrode and the existence of a deep secondary minimum in the particle pair interaction potential at higher ionic strength that traps particles in close proximity to one another. The results suggest that electrically induced crystallization will readily occur only over a narrow range of ionic strengths.

Simultaneous Aggregation and Height Bifurcation of Colloidal Particles near Electrodes in Oscillatory Electric Fields.

Micrometer-scale particles suspended in NaCl solutions aggregate laterally near the electrode upon application of a low-frequency (∼100 Hz) field, but the same particles suspended in NaOH solutions are instead observed to separate laterally. The underlying mechanism for the electrolyte dependence remains obscure. Recent work by Woehl et al. (PRX, 2015) revealed that, contrary to previous reports, particles suspended in NaOH solutions indeed aggregate under some conditions while simultaneously exhibiting a distinct bifurcation in average height above the electrode. Here we elaborate on this observation by demonstrating the existence of a critical frequency (∼25 Hz) below which particles in NaOH aggregate laterally and above which they separate. The results indicate that the current demarcation of electrolytes as either aggregating or separating is misleading and that the key role of the electrolyte instead is to set the magnitude of a critical frequency at which particles transition between the two behaviors.

Direct observation of aggregative nanoparticle growth: kinetic modeling of the size distribution and growth rate.

Direct observations of solution-phase nanoparticle growth using in situ liquid transmission electron microscopy (TEM) have demonstrated the importance of "non-classical" growth mechanisms, such as aggregation and coalescence, on the growth and final morphology of nanocrystals at the atomic and single nanoparticle scales. To date, groups have quantitatively interpreted the mean growth rate of nanoparticles in terms of the Lifshitz-Slyozov-Wagner (LSW) model for Ostwald ripening, but less attention has been paid to modeling the corresponding particle size distribution. Here we use in situ fluid stage scanning TEM to demonstrate that silver nanoparticles grow by a length-scale dependent mechanism, where individual nanoparticles grow by monomer attachment but ensemble-scale growth is dominated by aggregation. Although our observed mean nanoparticle growth rate is consistent with the LSW model, we show that the corresponding particle size distribution is broader and more symmetric than predicted by LSW. Following direct observations of aggregation, we interpret the ensemble-scale growth using Smoluchowski kinetics and demonstrate that the Smoluchowski model quantitatively captures the mean growth rate and particle size distribution.

Electrolyte-Dependent Aggregation of Colloidal Particles near Electrodes in Oscillatory Electric Fields.

Colloidal particles adjacent to electrodes have been observed to exhibit drastically different aggregation behavior depending on the identity of the suspending electrolyte. For example, particles suspended in potassium chloride aggregate laterally near the electrode upon application of a low-frequency (∼100 Hz) oscillatory electric field, but the same particles suspended in potassium hydroxide are instead observed to separate. Previous work has interpreted the particle aggregation or separation in terms of various types of electrically induced fluid flow around the particle, but the details remain poorly understood. Here we present experimental evidence that the aggregation rate is highly correlated to both the particle zeta potential and the electric field amplitude, both of which depend on the electrolyte type. Measurement of the aggregation rate in 26 unique electrolyte-particle combinations demonstrates that the aggregation rate decreases with increasing zeta potential magnitude (i.e., particles with a large zeta potential tended to separate regardless of sign). Likewise, direct measurements of the oscillatory electric field in different electrolytes revealed that the aggregation rate was negatively correlated with solution conductivity and thus positively correlated with the field strength. We tested the experimentally measured aggregation rates against a previously developed point dipole model and found that the model fails to capture the observed electrolyte dependence. The results point to the need for more detailed modeling to capture the effect of electrolyte on the zeta potential and solution conductivity to predict fluid flow around colloids near electrodes.

Vibrational manipulation of dry granular materials in lab-on-a-chip devices.

We present vibrational techniques to pump, mix, and separate dry granular materials using multifrequency vibrations applied to a solid substrate with a standard audio system. The direction and velocity of the granular flow are tuned by modulating the sign and amplitude, respectively, of the vibratory waveform, with typical pumping velocities of centimeters per second. Different granular materials are mixed by combining them at Y-shaped junctions, and mixtures of granules with different friction coefficients are separated along straight channels by judicious choice of the vibratory waveform. We demonstrate that the observed velocities accord with a theory valid for sufficiently large or fast vibrations, and we discuss the implications for using vibrational manipulation in conjunction with established microfluidic technologies to combine liquid and dry solid handling operations at sub-millimeter length scales.

The effect of roast profiles on the dynamics of titratable acidity during coffee roasting.

Coffee professionals have long known that the "roast profile," i.e., the temperature versus time inside the roaster, strongly affects the flavor and quality of the coffee. A particularly important attribute of brewed coffee is the perceived sourness, which is known to be strongly correlated to the total titratable acidity (TA). Most prior work has focused on laboratory-scale roasters with little control over the roast profile, so the relationship between roast profile in a commercial-scale roaster and the corresponding development of TA to date remains unclear. Here we investigate roast profiles of the same total duration but very different dynamics inside a 5-kg commercial drum roaster, and we show that the TA invariably peaks during first crack and then decays to its original value by second crack. Although the dynamics of the TA development varied with roast profile, the peak TA surprisingly exhibited almost no statistically significant differences among roast profiles. Our results provide insight on how to manipulate and achieve desired sourness during roasting.

Controlling the direction of steady electric fields in liquid using nonantiperiodic potentials.

When applying an oscillatory electric potential to an electrolyte solution, it is commonly assumed that the choice of which electrode is grounded or powered does not matter because the time average of the electric potential is zero. Recent theoretical, numerical, and experimental work, however, has established that certain types of multimodal oscillatory potentials that are "nonantiperiodic" can induce a net steady field toward either the grounded or powered electrode [A. Hashemi et al., Phys. Rev. E 105, 065001 (2022)2470-004510.1103/PhysRevE.105.065001]. Here, we elaborate on the nature of these steady fields through numerical and theoretical analyses of the asymmetric rectified electric field (AREF). We demonstrate that AREFs induced by a nonantiperiodic electric potential, e.g., by a two-mode waveform with modes at 2 and 3Hz, invariably yields a steady field that is spatially dissymmetric between two parallel electrodes, such that swapping which electrode is powered changes the direction of the field. Furthermore, we show that, while the single-mode AREF occurs in asymmetric electrolytes, nonantiperiodic electric potentials create a steady field in electrolytes even if the cations and anions have the same mobilities. Additionally, using a perturbation expansion, we demonstrate that the dissymmetric AREF occurs due to odd nonlinear orders of the applied potential. We further generalize the theory by demonstrating that the dissymmetric field occurs for all classes of zero-time-average (no dc bias) periodic potentials, including triangular and rectangular pulses, and we discuss how these steady fields can tremendously change the interpretation, design, and applications of electrochemical and electrokinetic systems.

A new Coffee Brewing Control Chart relating sensory properties and consumer liking to brew strength, extraction yield, and brew ratio.

The classic Coffee Brewing Control Chart (BCC) was originally developed in the 1950s. It relates coffee quality to brew strength and extraction yield, and it is still widely used today by coffee industry professionals around the world to provide guidance on the brewing of coffee. Despite its popularity, recent experimental studies have revealed that sensory attributes and consumer preferences actually follow much more complicated trends than those indicated by the classic BCC. Here, we present a methodology to synthesize the results of these recent studies on drip-brewed coffee to generate new versions of the BCC: a new Sensory BCC that displays a broad array of statistically significant sensory attributes across typical total dissolved solids and percent extraction ranges, a new Consumer BCC that highlights the existence of two preference clusters with different likes and dislikes across those ranges, a new Sensory and Consumer BCC that combines both sensory descriptive and consumer preferences on the same chart, and a more streamlined BCC that omits consumer preferences and focuses on the overarching sensory descriptive trends. The new BCCs provide more accurate insight on how best to brew coffee to achieve desired sensory profiles. PRACTICAL APPLICATION: Through the manipulation of yield and extraction parameters, the new Sensory and Consumer Coffee Brewing Control Chart presented here can be used by brewers of drip coffee to design coffees with specific sensory profiles and match the preferences of different consumer types.

Impact of beverage temperature on consumer preferences for black coffee.

We recently performed a systematic investigation of consumer preferences for black coffee versus key brewing parameters, including total dissolved solids, extraction yield, and brewing temperature (Cotter et al. in J Food Sci 86(1):194-205, 2021. https://doi.org/10.1111/1750-3841.15561 ). An experimental goal in that work was for participants to taste the coffee at a beverage temperature of 65 °C, but the large sample size of more than 3000 individual tastings, combined with natural variations in the brewing and cooling processes, meant that coffees were assessed over a normally distributed range of temperatures between 56 and 71 °C. Here we use those data to provide a more detailed analysis of the impact of beverage temperature on consumer acceptance of the coffee, with a key objective of identifying beverage temperatures at which no consumers assess the coffee either as too hot or too cold. Using a 5-point just-about-right (JAR) scale, we find that a majority of consumers (> 50%) assessed the temperature as JAR at all temperatures tested up to 70 °C. A substantial fraction of consumers, approximately 6-12%, assessed the coffee as too cold over the range 56-68 °C. Only above 70 °C did a majority of consumers assess the coffee as too hot and none assessed it as too cold, albeit with 40% still assessing it as JAR. Complementary analyses indicate that beverage temperature over this range had little impact on assessments of the adequacy of flavor intensity, acidity, and mouthfeel, but did correlate slightly with overall liking and purchase intent. Overall, the results suggest that temperatures over the range of 58-66 °C maximize consumer acceptance, and that 68-70 °C is the minimum temperature range at which no consumers will assess black coffee as too cold.