Size, Shape, and Phase of Nanoscale Uric Acid Particles

Uric acid particles are formed due to hyperuricemia, and previous works have focused on understanding the surface forces, crystallization, and growth of micron- and supermicron-sized particles. However, little to no work has furthered our understanding about uric acid nanonuclei that precipitate during the initial stages of kidney stone formation. In this work, we generate nanosized uric acid particles by evaporating saturated solution droplets of uric acid. Furthermore, we quantify the effects of drying rate on the morphology of uric acid nanonuclei. An aerosol droplet drying method generates uric acid nanoparticles in the size range of 20–200 nm from aqueous droplets (1–6 μm). Results show that uric acid nanonuclei are non-spherical with a shape factor value in the range of 1.1–1.4. The shape factor values change with drying rate and indicate that the nanoparticle morphology is greatly affected by drying kinetics. The nanonuclei are amorphous but can grow to form crystalline micron-sized particles. Indeed, a pre-crystallization phase was observed for heterogeneous nucleation of uric acid particles in the size range of a few hundred nanometers. Our findings show that the morphology of uric acid nanonuclei is significantly different from that of crystalline supermicron-sized particles. These new findings imply that the dissolution characteristics, surface properties, elimination, and medical treatment of uric acid nanonuclei formed during the initial stages of nucleation must be reconsidered

Electric Field-Induced Water Condensation Visualized by Vapor-Phase Transmission Electron Microscopy

Understanding the nanoscale water condensation dynamics in strong electric fields is important for improving the atmospheric modeling of cloud dynamics and emerging technologies utilizing electric fields for direct air moisture capture. Here, we use vapor-phase transmission electron microscopy (VPTEM) to directly image nanoscale condensation dynamics of sessile water droplets in electric fields. VPTEM imaging of saturated water vapor stimulated condensation of sessile water nanodroplets that grew to a size of ∼500 nm before evaporating over a time scale of a minute. Simulations showed that electron beam charging of the silicon nitride microfluidic channel windows generated electric fields of ∼108 V/m, which depressed the water vapor pressure and effected rapid nucleation of nanosized liquid water droplets. A mass balance model showed that droplet growth was consistent with electric field-induced condensation, while droplet evaporation was consistent with radiolysis-induced evaporation via conversion of water to hydrogen gas. The model quantified several electron beam–sample interactions and vapor transport properties, showed that electron beam heating was insignificant, and demonstrated that literature values significantly underestimated radiolytic hydrogen production and overestimated water vapor diffusivity. This work demonstrates a method for investigating water condensation in strong electric fields and under supersaturated conditions, which is relevant to vapor–liquid equilibrium in the troposphere. While this work identifies several electron beam–sample interactions that impact condensation dynamics, quantification of these phenomena here is expected to enable delineating these artifacts from the physics of interest and accounting for them when imaging more complex vapor–liquid equilibrium phenomena with VPTEM

Electric Field-Induced Water Condensation Visualized by Vapor-Phase Transmission Electron Microscopy

Understanding the nanoscale water condensation dynamics in strong electric fields is important for improving the atmospheric modeling of cloud dynamics and emerging technologies utilizing electric fields for direct air moisture capture. Here, we use vapor-phase transmission electron microscopy (VPTEM) to directly image nanoscale condensation dynamics of sessile water droplets in electric fields. VPTEM imaging of saturated water vapor stimulated condensation of sessile water nanodroplets that grew to a size of ∼500 nm before evaporating over a time scale of a minute. Simulations showed that electron beam charging of the silicon nitride microfluidic channel windows generated electric fields of ∼108 V/m, which depressed the water vapor pressure and effected rapid nucleation of nanosized liquid water droplets. A mass balance model showed that droplet growth was consistent with electric field-induced condensation, while droplet evaporation was consistent with radiolysis-induced evaporation via conversion of water to hydrogen gas. The model quantified several electron beam–sample interactions and vapor transport properties, showed that electron beam heating was insignificant, and demonstrated that literature values significantly underestimated radiolytic hydrogen production and overestimated water vapor diffusivity. This work demonstrates a method for investigating water condensation in strong electric fields and under supersaturated conditions, which is relevant to vapor–liquid equilibrium in the troposphere. While this work identifies several electron beam–sample interactions that impact condensation dynamics, quantification of these phenomena here is expected to enable delineating these artifacts from the physics of interest and accounting for them when imaging more complex vapor–liquid equilibrium phenomena with VPTEM

Electric Field-Induced Water Condensation Visualized by Vapor-Phase Transmission Electron Microscopy

Understanding the nanoscale water condensation dynamics in strong electric fields is important for improving the atmospheric modeling of cloud dynamics and emerging technologies utilizing electric fields for direct air moisture capture. Here, we use vapor-phase transmission electron microscopy (VPTEM) to directly image nanoscale condensation dynamics of sessile water droplets in electric fields. VPTEM imaging of saturated water vapor stimulated condensation of sessile water nanodroplets that grew to a size of ∼500 nm before evaporating over a time scale of a minute. Simulations showed that electron beam charging of the silicon nitride microfluidic channel windows generated electric fields of ∼108 V/m, which depressed the water vapor pressure and effected rapid nucleation of nanosized liquid water droplets. A mass balance model showed that droplet growth was consistent with electric field-induced condensation, while droplet evaporation was consistent with radiolysis-induced evaporation via conversion of water to hydrogen gas. The model quantified several electron beam–sample interactions and vapor transport properties, showed that electron beam heating was insignificant, and demonstrated that literature values significantly underestimated radiolytic hydrogen production and overestimated water vapor diffusivity. This work demonstrates a method for investigating water condensation in strong electric fields and under supersaturated conditions, which is relevant to vapor–liquid equilibrium in the troposphere. While this work identifies several electron beam–sample interactions that impact condensation dynamics, quantification of these phenomena here is expected to enable delineating these artifacts from the physics of interest and accounting for them when imaging more complex vapor–liquid equilibrium phenomena with VPTEM

Solubility Considerations for Cloud Condensation Nuclei (CCN) Activity Analysis of Pure and Mixed Black Carbon Species

Black carbon (BC) is an aerosol that is released into the atmosphere due to the incomplete burning of biomass and can affect the climate directly or indirectly. BC commonly mixes with other primary or secondary aerosols to undergo aging, thereby changing its radiative properties and cloud condensation nuclei (CCN) activity. The composition of aged BC species in the atmosphere is difficult to measure with high confidence, so their associated CCN activity can be uncertain. In this work, the CCN activity analysis of BC was performed using laboratory measurements of proxy aged BC species. Vulcan XC72R carbon black was used as the representative of BC, and three structural isomers of benzenedicarboxylic acidphthalic acid (PTA), isophthalic acid (IPTA), and terephthalic acid (TPTA)were mixed with BC to generate three different proxies of aged BC species. Most studies related to CCN activity analysis of BC aerosols use the traditional Köhler theory or an adsorption theory (such as the Frenkel–Halsey–Hill adsorption theory). PTA, IPTA, and TPTA fall in the sparingly water-soluble range and therefore do not fully obey either of the aforementioned theories. Consequently, a novel hybrid activity model (HAM) was used for the CCN activity analysis of the BC mixtures studied in this work. HAM combines the features of adsorption theory via the adsorption isotherm with the features of Köhler theory by incorporating solubility partitioning. The results in this work showed that HAM improves the representation of CCN activity of pure and mixed BC aerosol species with high certainty, evident from generally better goodness of fit, R2 > 0.9. This work implies that the hygroscopicity parameterization based on HAM captures the size-dependent variability in the CCN activity of the pure and aged BC species

Electric Field-Induced Water Condensation Visualized by Vapor-Phase Transmission Electron Microscopy

Understanding the nanoscale water condensation dynamics in strong electric fields is important for improving the atmospheric modeling of cloud dynamics and emerging technologies utilizing electric fields for direct air moisture capture. Here, we use vapor-phase transmission electron microscopy (VPTEM) to directly image nanoscale condensation dynamics of sessile water droplets in electric fields. VPTEM imaging of saturated water vapor stimulated condensation of sessile water nanodroplets that grew to a size of ∼500 nm before evaporating over a time scale of a minute. Simulations showed that electron beam charging of the silicon nitride microfluidic channel windows generated electric fields of ∼108 V/m, which depressed the water vapor pressure and effected rapid nucleation of nanosized liquid water droplets. A mass balance model showed that droplet growth was consistent with electric field-induced condensation, while droplet evaporation was consistent with radiolysis-induced evaporation via conversion of water to hydrogen gas. The model quantified several electron beam–sample interactions and vapor transport properties, showed that electron beam heating was insignificant, and demonstrated that literature values significantly underestimated radiolytic hydrogen production and overestimated water vapor diffusivity. This work demonstrates a method for investigating water condensation in strong electric fields and under supersaturated conditions, which is relevant to vapor–liquid equilibrium in the troposphere. While this work identifies several electron beam–sample interactions that impact condensation dynamics, quantification of these phenomena here is expected to enable delineating these artifacts from the physics of interest and accounting for them when imaging more complex vapor–liquid equilibrium phenomena with VPTEM