The particle‐size distribution (PSD) of a soil expresses the mass fractions of various sizes of mineral particles which constitute the soil material. It is a fundamental soil property, closely ...related to most physical and chemical soil properties and it affects almost any soil function. The experimental determination of soil texture, i.e., the relative amounts of sand, silt, and clay‐sized particles, is done in the laboratory by a combination of sieving (sand) and gravitational sedimentation (silt and clay). In the latter, Stokes' law is applied to derive the particle size from the settling velocity in an aqueous suspension. Traditionally, there are two methodologies for particle‐size analysis from sedimentation experiments: the pipette method and the hydrometer method. Both techniques rely on measuring the temporal change of the particle concentration or density of the suspension at a certain depth within the suspension. In this paper, we propose a new method which is based on the pressure in the suspension at a selected depth, which is an integral measure of all particles in suspension above the measuring depth. We derive a mathematical model which predicts the pressure decrease due to settling of particles as function of the PSD. The PSD of the analyzed sample is identified by fitting the simulated time series of pressure to the observed one by inverse modeling using global optimization. The new method yields the PSD in very high resolution and its experimental realization completely avoids any disturbance by the measuring process. A sensitivity analysis of different soil textures demonstrates that the method yields unbiased estimates of the PSD with very small estimation variance and an absolute error in the clay and silt fraction of less than 0.5%.
Key Points
New methodology for automated particle‐size analysis from sedimentation experiments
Accurate and precise identification of particle‐size distribution in high resolution
Contrary to pipette and hydrometer method, no manual operation necessary, and no disturbance of measurement process occurs
Many industrial catalysts involve nanoscale metal particles (typically 1–100 nm), and understanding their behavior at the molecular level is a major goal in heterogeneous catalyst research. However, ...conventional nanocatalysts have a nonuniform particle size distribution, while catalytic activity of nanoparticles is size dependent. This makes it difficult to relate the observed catalytic performance, which represents the average of all particle sizes, to the structure and intrinsic properties of individual catalyst particles. To overcome this obstacle, catalysts with well-defined particle size are highly desirable. In recent years, researchers have made remarkable advances in solution-phase synthesis of atomically precise nanoclusters, notably thiolate-protected gold nanoclusters. Such nanoclusters are composed of a precise number of metal atoms (n) and of ligands (m), denoted as Au n (SR) m , with n ranging up to a few hundred atoms (equivalent size up to 2–3 nm). These protected nanoclusters are well-defined to the atomic level (i.e., to the point of molecular purity), rather than defined based on size as in conventional nanoparticle synthesis. The Aun (SR)m nanoclusters are particularly robust under ambient or thermal conditions (<200 °C). In this Account, we introduce Au n (SR) m nanoclusters as a new, promising class of model catalyst. Research on the catalytic application of Au n (SR) m nanoclusters is still in its infancy, but we use Au25(SR)18 as an example to illustrate the promising catalytic properties of Au n (SR) m nanoclusters. Compared with conventional metallic nanoparticle catalysts, Au n (SR) m nanoclusters possess several distinct features. First of all, while gold nanoparticles typically adopt a face-centered cubic (fcc) structure, Au n (SR) m nanoclusters (<2 nm) tend to adopt different atom-packing structures; for example, Au25(SR)18 (1 nm metal core, Au atomic center to center distance) has an icosahedral structure. Secondly, their ultrasmall size induces strong electron energy quantization, as opposed to the continuous conduction band in metallic gold nanoparticles or bulk gold. Thus, nanoclusters become semiconductors and possess a sizable bandgap (e.g., ∼1.3 eV for Au25(SR)18). In addition, Au n (SR) m can be doped with a single atom of other metals, which is of great interest for catalysis, because the catalytic properties of nanoclusters can be truly tuned on an atom-by-atom basis. Overall, atomically precise Au n (SR) m nanoclusters are expected to become a promising class of model catalysts. These well-defined nanoclusters will provide new opportunities for achieving fundamental understanding of metal nanocatalysis, such as insight into size dependence and deep understanding of molecular activation, active centers, and catalytic mechanisms through correlation of behavior with the structures of nanoclusters. Future research on atomically precise nanocluster catalysts will contribute to the fundamental understanding of catalysis and to the new design of highly selective catalysts for specific chemical processes.
In recent years, pandemic outbreaks have raised concerns about the spread of respiratory infections and their impact on public health. Since the pathogen emission during human respiration is ...recognized as the primary source, characterizing the physical properties of exhaled particles and airflow has become a crucial focus of attention. This article critically reviews experimental studies in exhaled particles and airflow, examines the uncertainty introduced by different measurement methods, analyzes how it is reflected in measurement outcomes, and provides an in-depth understanding of particle size distribution and airflow behaviors of human respiration. The measurement techniques assessment highlights the variability among particle sizing techniques in detection size range, collection efficiency, hydration status of captured particles, and experimental protocols. A combination of sampling-based instruments and laser imaging systems is recommended for particle sizing to cover a wider detection range, with refined setups in thermal conditions, sampling distance, volume, and duration. Meanwhile, it identifies the complementary nature of qualitative and quantitative measurements of airflow characterization techniques. Image recording systems plus data reconstruction programs are suggested to capture dynamic airflow features while accuracy validation by other techniques is required at the same time. Subsequent analysis of the measurement data showed that the various experimental measurements provided substantial information, but they also revealed disagreements and challenges in quantification. The dominance of submicron aerosols in exhaled particles and jet-like transport in exhaled airflow is obvious. More efforts should be made to measure particles larger than 20 μm, capture airflow dynamics in a high temporal and spatial resolution, and quantify the impact of face coverings to improve the understanding of human respiratory emissions.
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Dynamic Light Scattering (DLS) generated particle size distributions (PSD) of polymer-stabilized nanoparticles are dependent on the optimization parameters used to generate an ...inversion solution fit to the measured autocorrelation function. The accuracy of the DLS PSD average and polydispersity can be determined by comparing analyzed Transmission Electron Microscopy (TEM) images with the DLS results if the TEM measured sizes can be corrected for the thickness of the hydrated polymer corona that impacts particle hydrodynamics but is a collapsed, desiccated shell in the TEM images.
Nanoparticles were prepared by Flash NanoPrecipitation with either poly(ethylene glycol) (PEG) or hydroxypropyl methylcellulose acetate succinate (HPMCAS) stabilizing polymers. Solvated nanoparticle size distributions were measured by DLS in aqueous media. The same nanoparticle dispersions were lyophilized onto TEM grids and stained by ruthenium tetroxide (RuO4) vapor to improve electron contrast. Desiccated particle size distributions were generated by measuring a minimum of 300 particle diameters in the stained TEM images.
Using our protocol for staining soft matter nanoparticles in TEM measurements, we have quantitatively analyzed the correlation between DLS and TEM generated PSDs. Average diameters disagree by the hydrated polymer corona thickness for each stabilizer due to the high-vacuum TEM environment, with 21.4 nm for PEG and 51.2 nm for HPMCAS. While corrected average diameter agrees within 10% for each technique, DLS consistently over-estimates the standard deviation of the PSD by 100% compared to the TEM measurement.
Coal samples for low-pressure nitrogen (N2) adsorption measurement in previous work cover a large particle size range (from 0.075 to 4.75 mm). However, minimal attention has been paid to the effect ...of coal particle size on pore structure using gas adsorption methods. Anthracite coal collected from the Zhina Coalfield, China, was crushed, subsampled, and sieved to eight particle size ranges: 1–2 mesh (8000–25400 µm), 40–50 mesh (270–380 µm), 50–70 mesh (212–270 µm), 70–90 mesh (160–212 µm), 90–160 mesh (96–160 µm), 160–200 mesh (75–96 µm), 200–300 mesh (48–75 µm), and >300 mesh (<48 µm). The adsorption–desorption isotherms of each subsample were measured using N2 at 77.35 K to compare differences in pore structure characteristics. The results of the N2 adsorption tests show that particle size has a significant effect on pore volume, specific surface area, and pore size distribution of coal. Specifically, decreasing coal particle size results in continuous increase in macro- and mesopore volumes and specific surface areas. This can be attributed to the fact that smaller-sized coal particles open more of the previously closed pores, which are then accessible to adsorping gas. The contribution of closed pores to the total pore volume is 94.94% in the pore aperture range of 3.1–370 nm. The volume of closed macropores varies from 48.96 to 84.69% of the total closed pore volume. According to optical microscope and SEM observations of the Zhina Coalfield subsamples, massive gas pores exist in an isolated form with poor connectivity; some plant tissue pores are filled by pyrites and clay minerals, and may be totally occluded. Thus, gas pores contribute the dominant amount of the closed pore volume. In addition, different Zhina Coalfield subsamples show varied hysteresis loop shapes, indicating that closed pores in coal possess a variety of pore morphologies and sizes. To improve the accuracy and comparability of the pore structure of coal, we propose >300 mesh as the preferred particle size of coal for all low-pressure N2 adsorption measurement in future work. Furthermore, caution must be used in evaluating coal bed methane resource recovery potential as coal possesses high closed porosity; failure to account for this will result in an overestimation of the amount of gas that can be recovered from coal seams during production.
Mixed‐Matrix Membranes Dechnik, Janina; Gascon, Jorge; Doonan, Christian J. ...
Angewandte Chemie International Edition,
August 1, 2017, Letnik:
56, Številka:
32
Journal Article
Recenzirano
Odprti dostop
Research into extended porous materials such as metal‐organic frameworks (MOFs) and porous organic frameworks (POFs), as well as the analogous metal‐organic polyhedra (MOPs) and porous organic cages ...(POCs), has blossomed over the last decade. Given their chemical and structural variability and notable porosity, MOFs have been proposed as adsorbents for industrial gas separations and also as promising filler components for high‐performance mixed‐matrix membranes (MMMs). Research in this area has focused on enhancing the chemical compatibility of the MOF and polymer phases by judiciously functionalizing the organic linkers of the MOF, modifying the MOF surface chemistry, and, more recently, exploring how particle size, morphology, and distribution enhance separation performance. Other filler materials, including POFs, MOPs, and POCs, are also being explored as additives for MMMs and have shown remarkable anti‐aging performance and excellent chemical compatibility with commercially available polymers. This Review briefly outlines the state‐of‐the‐art in MOF‐MMM fabrication, and the more recent use of POFs and molecular additives.
Challenging separations: The need for greater energy efficiency and the maximum use of limited resources has focused attention on improved separation technologies. For gas separations, mixed‐matrix membranes can provide enhanced separation performance and lead to more energy‐efficient, sustainable, and cost‐effective commercial applications.
•New sub-2μm C18 fully porous particles with narrow particle size distribution (nPSD).•Kinetic performance of nPSD columns is studied from a theoretical viewpoint.•Excellent kinetic performance comes ...from very small eddy dispersion term.•B- and C-term of van Deemter equation similar to those of fully porous C18 columns.
Columns packed with new commercially available 1.9 fully porous particles of narrow particle size distribution (nPSD) are characterized by extremely high efficiency. Under typical reversed phase conditions, these columns are able to generate very high number of theoretical plates (in the order of 300,000plates/m and more). In this paper, we investigate the origin of the high performance of these nPSD columns by performing a series of measurements that include, in addition to the traditional determination of the van Deemter curve, peak parking, pore blocking and inverse size exclusion experiments. Two nPSD columns (both 100×3.0mm) have been considered in this study: the first one, packed with particles of 80Å pore size, is commercially available. The second one is a prototype column packed with 1.9 fully porous particles of 120Å pore size.
The main conclusion of our study is that these nPSD columns are characterized by extremely low eddy dispersion, while longitudinal diffusion and mass transfer kinetics are substantially equivalent to those of other fully porous particles of similar chemistry.
Methylammonium lead halide perovskites are attracting intense interest as promising materials for next-generation solar cells, but serious issues related to long-term stability need to be addressed. ...Perovskite films based on CH
NH
PbI
undergo rapid degradation when exposed to oxygen and light. Here, we report mechanistic insights into this oxygen-induced photodegradation from a range of experimental and computational techniques. We find fast oxygen diffusion into CH
NH
PbI
films is accompanied by photo-induced formation of highly reactive superoxide species. Perovskite films composed of small crystallites show higher yields of superoxide and lower stability. Ab initio simulations indicate that iodide vacancies are the preferred sites in mediating the photo-induced formation of superoxide species from oxygen. Thin-film passivation with iodide salts is shown to enhance film and device stability. The understanding of degradation phenomena gained from this study is important for the future design and optimization of stable perovskite solar cells.
•Effect of hydrate saturation, morphology and particle size on HBS permeability.•Analysis of pore-scale flow behavior at pore throat on HBS permeability.•Abrupt permeability reduction identified at ...SH = 33.9% for pore-filling HBS.•A new model proposed for HBS permeability calculation considering tortuosity.•HBS permeability comparison between uniform and non-uniform settings.
The distribution pattern of CH4 hydrate in hydrate-bearing sediments (HBS) significantly impacts the permeability, which is one of the critical flow properties controlling the fluid production in the exploitation of natural gas hydrate (NGH) reservoirs. Thus, it warrants investigation on the key influencing factors, i.e., (a) hydrate saturation; (b) hydrate distribution patterns; (c) sediment particle size on the associated permeability of HBS especially at pore-scale. In this study, a series of two-dimensional geometric models were constructed that best represent the commonly-observed hydrate distribution patterns. The pore-scale flow behavior of the resulting models was simulated through computational fluid dynamics. The simulation results suggest that the reduction of permeability is dependent on the distribution pattern of hydrate. The permeability of grain-coating HBS decreases by a maximum of five orders of magnitude at SH = 0.3. Additionally, increasing SH results in new pore throats and induces clogging in fluid flow that controls permeability reduction. A strong log-log linear relationship was identified between sediment particle size and the simulated permeability. A modified empirical model for the estimation of HBS permeability was proposed considering both tortuosity and effective porosity. Moreover, a heterogeneous sediment particle distribution model was constructed for the first time that accurately described the particle size distribution of a hydrate-bearing core sample recovered from Japan Nankai Trough. Compared to the homogeneous model, a heterogeneous model results in a more substantial reduction of permeability with SH and better represents the permeability of the HBS core sample. The finding of this study can be significant in understanding the pore-scale flow behavior in HBS and are meaningful for the design of safe and effective production methods in the exploitation of NGH reservoirs.
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Understanding the particle size distribution in the air and patterns of environmental contamination of SARS-CoV-2 is essential for infection prevention policies. Here we screen surface and air ...samples from hospital rooms of COVID-19 patients for SARS-CoV-2 RNA. Environmental sampling is conducted in three airborne infection isolation rooms (AIIRs) in the ICU and 27 AIIRs in the general ward. 245 surface samples are collected. 56.7% of rooms have at least one environmental surface contaminated. High touch surface contamination is shown in ten (66.7%) out of 15 patients in the first week of illness, and three (20%) beyond the first week of illness (p = 0.01, χ
test). Air sampling is performed in three of the 27 AIIRs in the general ward, and detects SARS-CoV-2 PCR-positive particles of sizes >4 µm and 1-4 µm in two rooms, despite these rooms having 12 air changes per hour. This warrants further study of the airborne transmission potential of SARS-CoV-2.
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