Helical magnetic micromotors decorated with nickel ferrocyanide for the active and rapid adsorption of radiocesium in water.

Separating radioactive cesium from nuclear waste and contaminated environments is critical to mitigate radiological hazards. In response to this need, remote-controllable and Cs-selective micromotor adsorbents have been considered as a promising technology for rapid in-situ cleanup while minimizing secondary waste and radiation exposure to workers. In this study, we demonstrate the active and rapid removal of a radioactive contaminant from water by leveraging the magnetic manipulation capabilities of a helical and magnetic Ni micromotor coated with Cs-selective nickel ferrocyanide (NiFC). The use of polyvinyl alcohol fibers as a template enables the straightforward preparation of the helical wire structure, allowing for precise control over the diameter and pitch of the helix through simple twisting with Ni wires. By harnessing Ni2+ ions eluted from the Ni micromotor in an acid solution, we successfully fabricate NiFC-coated Ni (NiFC/Ni) micromotors that exhibit a selective removal efficiency greater than 98% for 137Cs, even in the presence of high concentrations of competing Na+ ions. Under the influence of an external magnetic field, the NiFC/Ni micromotor demonstrates rapid motion, achieving a pulling motion (100 body lengths per second) through a magnetic gradient and a tumbling motion (46 body lengths per second) induced by a rotating magnetic field. The tumbling motion of the NiFC/Ni micromotor substantially improves the Cs adsorption rate, resulting in a rate that surpasses that achieved under nonmoving conditions by a factor of 21. This improved adsorption rate highlights the considerable potential of magnetically manipulated micromotor self-propulsion for efficient water-pollution treatment.

Surface decontamination of radioactive cesium by a reversibly cross-linkable hydrogel using poly(vinyl alcohol) and phenylboronic acid-grafted poly(methyl vinyl ether-alt-mono-sodium maleate).

Wide-area surface decontamination is essential during the sudden release of radioisotopes to the public, such as nuclear accidents or terrorist attacks. A self-generated hydrogel comprising a reversible complex between poly(vinyl alcohol) (PVA) and phenylboronic acid-grafted poly(methyl vinyl ether-alt-mono-sodium maleate) (PBA-g-PMVE-SM) was developed as a new surface decontamination coating agent to remove radioactive cesium from surfaces. The simultaneous application of PVA and PBA-g-PMVE-SM aqueous polymer solutions containing sulfur-zeolite to contaminated surfaces resulted in the spontaneous formation of a PBA-diol ester bond-based hydrogel. The sulfur-zeolite suspended in the hydrogel selectively removed 137Cs from the contaminated surface and was easily separated from the dissociable used hydrogel. This removal was performed by simple water rinsing without costly incineration to remove the organic materials for final disposal/storage of the radioactive waste, making it suitable for practical wide-area surface decontamination. In radioactive tests, the hydrogel containing sulfur-chabazite (S-CHA) showed substantial 137Cs removal efficiencies of 96.996% for painted cement and 63.404% for cement, which are 2.33 times better than the values for the commercial surface decontamination coating agent DeconGel. Due to its excellent zeolite ion-exchange ability, our hydrogel system has great potential for removing various hazardous contaminants, including radionuclides, from the surface.

How to Change the Reaction Chemistry on Nonprecious Metal Oxide Nanostructure Materials for Electrocatalytic Oxidation of Biomass-Derived Glycerol to Renewable Chemicals.

Au and Pt are well-known catalysts for electrocatalytic oxidation of biomass-derived glycerol. Although some nonprecious-metal-based materials to replace the costly Au and Pt are used for this reaction, the fundamental question of how the nonprecious catalysts affect the reaction chemistry and mechanism compared to Au and Pt catalysts is still unanswered. In this work, both experimental and computational methods are used to understand how and why the reaction performance and chemistry for the electrocatalytic glycerol oxidation reaction (EGOR) change with electrochemically-synthesized CuCo-oxide, Cu-oxide, and Co-oxide catalysts compared to conventional Au and Pt catalysts. The Au and Pt catalysts generate major glyceric acid and glycolic acid products from the EGOR. Interestingly, the prepared Cu-based oxides produce glycolic acid and formic acid with high selectivity of about 90.0%. This different reaction chemistry is related to the enhanced ability of CC bond cleavage on the Cu-based oxide materials. The density functional theory calculations demonstrate that the formic acids are mainly formed on the Cu-based oxide surfaces rather than in the process of glycolic acid formation in the free energy diagram. This study provides critical scientific insights into developing future nonprecious-based materials for electrochemical biomass conversions.

Tannic acid-assisted in-situ interfacial formation of Prussian blue-assembled adsorptive membranes for radioactive cesium removal.

There is a growing interest in advanced materials that can effectively treat wastewater contaminated with radioactive cesium (137Cs), which is an extremely hazardous material. Here, we report a new class of Cs-adsorptive membranes compactly assembled with Cs-adsorptive Prussian blue (PB) particles. The PB particle assembly was formed via an in-situ interfacial reaction between two PB precursors in the presence of tannic acid (TA) as a binder on a porous support. While the interfacial reaction enabled the formation of a defect-less PB network, TA enhanced the PB-PB and PB-support compatibilities, consequently producing a uniform, densely packed PB assembly near the support surface. The fabricated TA-assisted PB membrane (PB/TA-M) synergistically rejected Cs via a combination of adsorption and membrane filtration, although adsorption predominantly determined Cs rejection initially. Hence, the PB/TA-M membrane showed considerably higher Cs removal performance than commercial nanofiltration (NF) and reverse osmosis (RO) polyamide (PA) membranes for a sufficiently long operation time. Furthermore, the PB/TA-M membrane displayed excellent radioactive 137Cs removal performance, significantly exceeding those of commercial NF and RO PA membranes due to its higher radiation stability, indicating its viability for application in treating actual radioactive wastewater.

Sleep Pattern Analysis in Unconstrained and Unconscious State.

Sleep accounts for one-third of an individual's life and is a measure of health. Both sleep time and quality are essential, and a person requires sound sleep to stay healthy. Generally, sleep patterns are influenced by genetic factors and differ among people. Therefore, analyzing whether individual sleep patterns guarantee sufficient sleep is necessary. Here, we aimed to acquire information regarding the sleep status of individuals in an unconstrained and unconscious state to consequently classify the sleep state. Accordingly, we collected data associated with the sleep status of individuals, such as frequency of tosses and turns, snoring, and body temperature, as well as environmental data, such as room temperature, humidity, illuminance, carbon dioxide concentration, and ambient noise. The sleep state was classified into two stages: nonrapid eye movement and rapid eye movement sleep, rather than the general four stages. Furthermore, to verify the validity of the sleep state classifications, we compared them with heart rate.

Systemic Lupus Erythematosus and Lung Involvement: A Comprehensive Review.

Systemic lupus erythematosus (SLE) is a complex autoimmune disease with multiorgan manifestations, including pleuropulmonary involvement (20-90%). The precise mechanism of pleuropulmonary involvement in SLE is not well-understood; however, systemic type 1 interferons, circulating immune complexes, and neutrophils seem to play essential roles. There are eight types of pleuropulmonary involvement: lupus pleuritis, pleural effusion, acute lupus pneumonitis, shrinking lung syndrome, interstitial lung disease, diffuse alveolar hemorrhage (DAH), pulmonary arterial hypertension, and pulmonary embolism. DAH has a high mortality rate (68-75%). The diagnostic tools for pleuropulmonary involvement in SLE include chest X-ray (CXR), computed tomography (CT), pulmonary function tests (PFT), bronchoalveolar lavage, biopsy, technetium-99m hexamethylprophylene amine oxime perfusion scan, and (18)F-fluorodeoxyglucose positron emission tomography. An approach for detecting pleuropulmonary involvement in SLE includes high-resolution CT, CXR, and PFT. Little is known about specific therapies for pleuropulmonary involvement in SLE. However, immunosuppressive therapies such as corticosteroids and cyclophosphamide are generally used. Rituximab has also been successfully used in three of the eight pleuropulmonary involvement forms: lupus pleuritis, acute lupus pneumonitis, and shrinking lung syndrome. Pleuropulmonary manifestations are part of the clinical criteria for SLE diagnosis. However, no review article has focused on the involvement of pleuropulmonary disease in SLE. Therefore, this article summarizes the literature on the epidemiology, pathogenesis, diagnosis, and management of pleuropulmonary involvement in SLE.

Perovskite-based electrocatalysts for oxygen evolution reaction in alkaline media: A mini review.

Water electrolysis is one of the attractive technologies for producing clean and sustainable hydrogen fuels with high purity. Among the various kinds of water electrolysis systems, anion exchange membrane water electrolysis has received much attention by combining the advantages of alkaline water electrolysis and proton exchange membrane water electrolysis. However, the sluggish kinetics of the oxygen evolution reaction, which is based on multiple and complex reaction mechanisms, is regarded as a major obstacle for the development of high-efficiency water electrolysis. Therefore, the development of high-performance oxygen evolution reaction electrocatalysts is a prerequisite for the commercialization and wide application of water electrolysis systems. This mini review highlights the current progress of representative oxygen evolution reaction electrocatalysts that are based on a perovskite structure in alkaline media. We first summarize the research status of various kinds of perovskite-based oxygen evolution reaction electrocatalysts, reaction mechanisms and activity descriptors. Finally, the challenges facing the development of perovskite-based oxygen evolution reaction electrocatalysts and a perspective on their future are discussed.

Unveiling the enhanced electrocatalytic activity at electrochemically synthesized Pt-WOx hybrid nanostructure interfaces.

Here we report a simple synthesis strategy for Pt-WOx hybrid nanostructures using a metal-dissolution-based electrodeposition technique. The hybrid nanostructures demonstrate an excellent catalytic hydrogen evolution reaction performance with an approximately 17 times higher Pt mass activity and a 7.4 times higher turnover frequency than those of commercial Pt catalysts. The enhanced electrocatalytic performance is related to the creation of Pt-WOx interfacial sites.

Active and selective removal of Cs from contaminated water by self-propelled magnetic illite microspheres.

We report the fabrication of clay-mineral-based Janus microspheres that exhibit remotely steerable self-propulsion in water, facilitating their selective and active removal of radiocesium from a contaminated solution. The spray-drying of slurries of intrinsically Cs-selective illite containing iron oxide nanoparticles led to magnetic illite microspheres with superior 137Cs adsorption capability and superparamagnetic behavior. The Janus micromotor adsorbent was prepared by depositing catalytic Pt onto the half-surface of magnetic illite microspheres. The micromotor adsorbents exhibited self-propulsion at speeds as high as ~265 µm/s via asymmetric bubble generation in water containing H2O2 as a fuel. The self-propulsion of the adsorbent improved the Cs adsorption kinetics six-folds compared with the kinetics in the corresponding stationary liquid. The magnetic properties of the micromotor adsorbent enabled convenient separation and direction control of the adsorbents under an external magnetic field. In particular, the micromotor adsorbent could successfully remove more than 98.6% of 137Cs from aqueous media containing competing ions including K+, Na+, Ca2+ and Mg2+.

Sulfur-encapsulated zeolite micromotors for the selective removal of cesium from high-salt water with accelerated cleanup times.

Bubble-propelled sulfur-encapsulated NaX zeolite (S-NaX) micromotors were developed for the selective removal of cesium from high-salt conditions with accelerated cleanup times. NaX was first modified with sulfur to provide additional Lewis acid-base interactions with Cs+ for enhanced Cs+ selectivity, and then Pt was half-deposited on S-NaX for bubble propulsion via the catalytic decomposition of H2O2. The average velocity of the resulting S-NaX/Pt micromotors in 5 wt% H2O2 is 39.7 ± 17.1 µm/s, which is higher than that of a previously reported Cs adsorbent micromotor (35.4 µm/s). The Cs+ ion-exchange kinetics of the S-NaX micromotor is 1.32 times higher than that of the NaX micromotor in a 5 wt% H2O2 solution where the molar ratio of Na+ to Cs+ is 200, even though the sulfur in the S-NaX micromotor causes an adverse effect on the propulsion speed due to the sulfur poisoning effect. Moreover, the S-NaX micromotor in simulated groundwater also exhibited excellent Cs+ removal performance with distribution coefficient (Kd) values at least 3.2 times higher than those of the nonpropelled S-NaX and NaX micromotor, demonstrating the great potential for the treatment of radioactive Cs+-contaminated water.

Application of Desalination Membranes to Nuclide (Cs, Sr, and Co) Separation.

Desalination and nuclide separation, with cesium (Cs), strontium (Sr), and cobalt (Co), using commercial polymeric membranes are investigated under room temperature (298 K) to elucidate the permeation mechanism and possibility of applying commercial membranes to the separation of radioactive nuclides. The physicochemical properties of membranes are characterized by multiple techniques. The thickness of the selective layer and the boundary between the layers of membranes are observed by scanning electron microscopy. The chemical structure of selective and support layers is assessed by direct Fourier transform infrared/attenuated total reflection measurements on membrane samples. Thermogravimetric analysis demonstrates the composition comparison between membranes, which describes the relative amount of selective layers consisting of polyamide. The separation performance of polyamide-based commercial membranes is tested on simulated seawater (35,000 ppm of NaCl) and single- and multi-component aqueous nuclide solutions (10 ppm). Nanofiltration (NF) membranes exhibit a high flux of 160-210 L m-2 h-1 with low 31-64% rejection on the permeation of simulated seawater, while reverse osmosis (RO) membranes display a low flux of 13-22 L m-2 h-1 with nearly 80% rejection. This reveals RO membranes to be more effective for the rejecting nuclides (Cs, Sr, and Co) in dilute aqueous solutions, and NF membranes have advantage on high throughput. RO membranes reject above 93% for single components and even higher for mixed nuclide separation (>98%), and NF membranes permeate high flux above 230 L m-2 h-1. This study indicates that the desalination membranes (NF and RO) can be potential candidates for nuclide separation with combination.

The Delay in Confirming COVID-19 Cases Linked to a Religious Group in Korea.

OBJECTIVES: As of March 3, 2020, the Shincheonji religious group accounted for the majority of Korean cases of coronavirus disease 2019 (COVID-19). Nonetheless, the most likely cause of the broad spread of COVID-19 among members of the Shincheonji religious group remains largely unknown. METHODS: We obtained data of laboratory-confirmed cases related to the Shincheonji religious group from press releases by Korean public health authorities and news reports. We measured the period from the date of illness onset to the date of COVID-19 confirmation. RESULTS: We analysed data from 59 cases (median age, 30 years). The estimated median period between the date of symptom onset and the date of COVID-19 confirmation was 4 days (95% confidence interval, 1-12). CONCLUSIONS: There was a delay in COVID-19 confirmation from the date of illness onset among the cases linked to the Shincheonji religious group. This delay likely contributed to the occurrence of many cases of COVID-19 in the group.

Poly(acryloyl hydrazide)-grafted cellulose nanocrystal adsorbents with an excellent Cr(VI) adsorption capacity.

In this study, we prepared poly(acryloyl hydrazide) (PAH)-grafted cellulose nanocrystal (CNC-PAH) particles via the atom transfer radical polymerization method for application to Cr(VI) adsorption. The closely-packed PAH chains grafted on the cellulose nanocrystal (CNC) surface provide a high density of amine groups that can adsorb Cr(VI) through strong electrostatic, hydrogen bonding and chelating interactions. CNC-PAH exhibited the optimum Cr(VI) adsorption capacity at the solution pH = 3, where its electrostatic attraction with Cr(VI) was maximized. Cr(VI) was chemisorbed in CNC-PAH by following the Langmuir isotherm mechanism (homogeneous monolayer adsorption). The Cr(VI) adsorption kinetics of CNC-PAH was controlled predominantly by intra-particle diffusion resistance imparted by the PAH shell layer. Thermodynamic analysis revealed that Cr(VI) adsorption of CNC-PAH is a spontaneous and endothermic process. Importantly, CNC-PAH grafted with the higher Mw (∼50 kg mol-1) PAH exhibited a rapid Cr(VI) adsorption rate and remarkably high Cr(VI) adsorption capacity (∼457.6 mg g-1 at 298.15 K), exceeding those of previously reported adsorbents owing to its numerous Cr(VI)-adsorptive amine groups provided by the closely-packed grafted PAH polymers. Furthermore, CNC-PAH showed excellent reusability to maintain its high adsorption ability during repeated adsorption-desorption cycles owing to the covalently binding nature of the PAH polymers.

Sustainable production of alkyl esters via thermal process in the presence of carbon black.

In this study, it is introduced a sustainable synthetic route of alkyl esters, considered value-added industrial chemicals and fuels, from volatile fatty acids (VFAs) that can potentially be generated from organic waste. In the presence of a porous carbon material, the thermally induced reaction could be conducted under an initial pressure of 1 atm. Even though the reaction was finished within <10 s, they gave a high yield of target products: the conversion of six VFAs into their corresponding methyl esters which can be further converted into gasoline alternatives with >90 wt% yields. The carbon black showed better performance for both reactions than other commercially available porous material such as silica. This work suggests that carbon is a good option of being used as a porous material for thermal esterification to produce renewable alternative chemicals from waste-derived feedstocks.

Production of high-octane gasoline via hydrodeoxygenation of sorbitol over palladium-based bimetallic catalysts.

A methodology for the synthesis of gasoline-range fuels from carbon neutral resources is introduced. Sorbitol, a sugar-based compound, was employed as a raw material because the compound is readily obtained from cellulose. Gasoline-range hydrocarbons were produced via hydrodeoxygenation (HDO) on zirconium phosphate-supported Pd-bimetallic (Pt-Pd, Ru-Pd, Ni-Pd, Fe-Pd, Co-Pd, W-Pd) catalysts. Among the tested catalysts, the bimetallic W-Pd/ZrP catalyst exhibited the highest yield of gasoline products, peaking at ∼70%. However, with the bimetallic Fe-Pd and Co-Pd catalysts, high-octane gasoline products were made (research octane number (RON) of the products was higher than 100). The Fe-Pd catalyst also showed the highest initial activity for the HDO of sorbitol. This study demonstrates that HDO in the Pd-system is a promising option to produce high-quality gasoline-range hydrocarbons from lignocellulosic biomass.

Plasmon-enhanced photoelectrochemical water splitting with size-controllable gold nanodot arrays.

Size-controllable Au nanodot arrays (50, 63, and 83 nm dot size) with a narrow size distribution (± 5%) were prepared by a direct contact printing method on an indium tin oxide (ITO) substrate. Titania was added to the Au nanodots using TiO(2) sols of 2-3 nm in size. This created a precisely controlled Au nanodot with 110 nm of TiO(2) overcoats. Using these precisely controlled nanodot arrays, the effects of Au nanodot size and TiO(2) overcoats were investigated for photoelectrochemical water splitting using a three-electrode system with a fiber-optic visible light source. From UV-vis measurement, the localized surface plasmon resonance (LSPR) peak energy (ELSPR) increased and the LSPR line width (Γ) decreased with decreasing Au nanodot size. The generated plasmonic enhancement for the photoelectrochemical water splitting reaction increased with decreasing Au particle size. The measured plasmonic enhancement for light on/off experiments was 25 times for the 50 nm Au size and 10 times for the 83 nm Au nanodot size. The activity of each catalyst increased by a factor of 6 when TiO2 was added to the Au nanodots for all the samples. The activity of the catalyst was proportional to the quality factor (defined as Q = E(LSPR)/Γ) of the plasmonic metal nanostructure. The enhanced water splitting performance with the decreased Au nanodot size is probably due to more generated charge carriers (electron/hole pair) by local field enhancement as the quality factor increases.

Silylated mesoporous silica membranes on polymeric hollow fiber supports: synthesis and permeation properties.

We report the synthesis and organic/water separation properties of mesoporous silica membranes, supported on low-cost and scalable polymeric (polyamide-imide) hollow fibers, and modified by trimethylsilylation with hexamethyldisilazane. Thin (∼1 µm) defect-free membranes are prepared, with high room-temperature gas permeances (e.g., 20,000 GPU for N2). The membrane morphology is characterized by multiple techniques, including SEM, TEM, XRD, and FT-ATR spectroscopy. Silylation leads to capping of the surface silanol groups in the mesopores with trimethylsilyl groups, and does not affect the integrity of the mesoporous silica structure and the underlying hollow fiber. The silylated membranes are evaluated for pervaporative separation of ethanol (EtOH), methylethyl ketone (MEK), ethyl acetate (EA), iso-butanol (i-BuOH), and n-butanol (n-BuOH) from their dilute (5 wt %) aqueous solutions. The membranes show separation factors in the range of 4-90 and high organic fluxes in the range of 0.18-2.15 kg m(-2) h(-1) at 303 K. The intrinsic selectivities (organic/water permeability ratios) of the silylated membranes at 303 K are 0.33 (EtOH/water), 0.5 (MEK/water), 0.25 (EA/water), 1.25 (i-BuOH/water), and 1.67 (n-BuOH/water) respectively, in comparison to 0.05, 0.015, 0.005, 0.08, and 0.14 for the unmodified membranes. The silylated membranes allow upgradation of water/organics feeds to permeate streams with considerably higher organics content. The selective and high-flux separation is attributed to both the organophilic nature of the modified mesopores and the large effective pore size. Comparison with other organics/water separation membranes reveals that the present membranes show promise due to high flux, use of scalable and low-cost supports, and good separation factors that can be further enhanced by tailoring the mesopore silylation chemistry.

Selective glycerol oxidation by electrocatalytic dehydrogenation.

This study demonstrates that an electrochemical dehydrogenation process can be used to oxidize glycerol to glyceraldehyde and glyceric acid even without using stoichiometric chemical oxidants. A glyceric acid selectivity of 87.0 % at 91.8 % glycerol conversion was obtained in an electrocatalytic batch reactor. A continuous-flow electrocatalytic reactor had over an 80 % high glyceric acid selectivity at 10 % glycerol conversion, as well as greater reaction rates than either an electrocatalytic or a conventional catalytic batch reactor.

Expression of Secreted Protein Acidic and Rich in Cysteine in the Stroma of a Colorectal Carcinoma is Associated With Patient Prognosis.

PURPOSE: Secreted protein acidic and rich in cysteine (SPARC), also known as osteonectin or basement-membrane-40 (BM-40), is a member of a family of matricellular proteins, whose functions are to modulate cell-matrix interactions, growth and angiogenesis in colorectal cancer. In this study, the expression of SPARC was evaluated and its correlations with clinicopathological parameters were investigated. METHODS: The researchers analyzed the expression patterns of SPARC by using immunohistochemistry in 332 cases of colorectal cancer of tissue microarray. The clinicopathological characteristics were defined by using the TNM criteria of the Union for International Cancer Control. Clinicopathological factors such as age, sex, histologic type of the tumor, pathologic tumor stage, TNM stage, and lymphovascular invasion were evaluated according to the SPARC expression. RESULTS: The hazard ratios expressing SPARC in tumor cells, in the stroma, and in both tumor cells and the stroma were 2.10 (P = 0.036), 3.27 (P = 0.003) and 2.12 (P = 0.038), respectively. Patient survival was decreased in patient expressing SPARC in the stroma, and this result showed statistical significance (P = 0.016). CONCLUSION: These findings suggest that SPARC expression in a tumor and in the stroma correlates with disease progression and may be used as a prognostic marker for colorectal cancer.

Electrocatalytic reduction of acetone in a proton-exchange-membrane reactor: a model reaction for the electrocatalytic reduction of biomass.

Acetone was electrocatalytically reduced to isopropanol in a proton-exchange-membrane (PEM) reactor on an unsupported platinum cathode. Protons needed for the reduction were produced on the unsupported Pt-Ru anode from either hydrogen gas or electrolysis of water. The current efficiency (the ratio of current contributing to the desired chemical reaction to the overall current) and reaction rate for acetone conversion increased with increasing temperature or applied voltage for the electrocatalytic acetone/water system. The reaction rate and current efficiency went through a maximum with respect to acetone concentration. The reaction rate for acetone conversion increased with increasing temperature for the electrocatalytic acetone/hydrogen system. Increasing the applied voltage for the electrocatalytic acetone/hydrogen system decreased the current efficiency due to production of hydrogen gas. Results from this study demonstrate the commercial feasibility of using PEM reactors to electrocatalytically reduce biomass-derived oxygenates into renewable fuels and chemicals.