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At least 1,045 records · Page 58
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Warming Stimulates Iron-Mediated Carbon and Nutrient Cycling in Mineral-Poor Peatlands

We know that iron (Fe) plays a key role in elemental cycling at terrestrial–aquatic interfaces by stabilizing carbon (C), phosphorus (P), and nutrient cations through physicochemical associations and by potentially releasing these elements following the reduction of Fe(III) to Fe(II). However, the ecosystem-scale importance of Fe redox cycling and its responses to climate change remain unclear in precipitation-fed peatlands (bogs), C-rich wetlands with very low mineral content. We tested impacts of Fe redox cycling on C and nutrient release in two bogs in northern Minnesota and in Spruce and Peatland Responses Under Changing Environments (SPRUCE), an ecosystem-scale warming experiment. Concentrations of Fe(III) declined from the peat surface to 50 cm depth (31 to 0.5 µmol g -1 ) and co-occurred with Fe(II) (10 to 30 µmol g -1 ). Chemical reduction of Fe(III) released C and P from variably saturated (0–30 cm) peat (106–1006 µmol C g -1 ; 0.6–5 µmol P g -1 ), and Fe-bound C was similar to previous measurements from upland mineral soils. Concentrations of Fe(II) and dissolved organic carbon (DOC) were strongly (R 2 = 0.56–0.78) and positively correlated in water samples measured at SPRUCE enclosure outlets and ambient near-surface porewater. Concentrations of Fe(II) also correlated positively with P at warmer SPRUCE temperature treatments and increased with experimental warming, but stabilized at the highest temperature treatments as water depth declined. Although bogs have low total mineral content, mass balance measurements indicated that atmospheric deposition could in principle sustain significant Fe cycling and hydrologic losses in these ecosystems. Overall, Fe redox cycling significantly impacted C and nutrient dynamics in these mineral-poor bogs, contributing to strong correlations between Fe(II) and DOC in water samples. Increased Fe(III) reduction with warmer temperatures will likely promote peatland C and nutrient release, impacting ecosystem C budgets both directly and indirectly by enhancing decomposition and productivity.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Integrating Reservoirs into the Dissolved Organic Matter Versus Primary Production Paradigm: How Does Chlorophyll-$a$ Change Across Dissolved Organic Carbon Concentrations in Reservoirs?

Primary production in freshwater ecosystems is largely a function of light and nutrient availability, both of which have been changing in many lakes and reservoirs in response to anthropogenic pressures. Recent studies focusing on natural lakes have found a hump-shaped response of primary production (sometimes measured as chlorophyll-$a$) to dissolved organic matter (DOM, measured as dissolved organic carbon, DOC), which has both light-absorbing chromophoric properties and DOM-bound nutrients. We used the United States National Lakes Assessment dataset to integrate reservoirs into this paradigm in comparison with natural lakes and assessed the relative differences in the predicted response’s model structure, regression parameter values, and drivers of the chlorophyll-$a$ residuals. We found that chlorophyll-$a$ in reservoirs exhibited a hump-shaped response to DOC, while natural lakes from this dataset were better fit with a linear response, differing from previous studies focused on boreal lakes. Despite this, reservoirs had a greater maximum chlorophyll-a response compared to natural lakes in this study (45.5 versus 33.8 μg L -1 ), which occurred at a lower DOC concentration threshold (18.3 versus 26.4 mg L -1 ) when compared using quadratic models. Reservoirs had lower median light:nutrient values compared to natural lakes, and greater median surface area and total phosphorus (TP), that can all influence the light environment and the peak chlorophyll-a responses. In both reservoirs and natural lakes, chlorophyll-$a$ residuals were most strongly influenced by TP, where TP < 25-30 µg L -1 suppressed chlorophyll-a residuals and higher TP amplified them. Light:nutrient values were somewhat important predictors, and patterns with chlorophyll-$a$ residuals supported previous work showing low light:nutrient values amplified chlorophyll-$a$ responses and higher values suppressed them. In conclusion, quantifying the shape of the response of primary production to DOM quantity and quality as well as the drivers of the residuals, namely TP for lakes and reservoirs in this dataset, will be important for understanding the effects that changes in water quality may have on primary production and freshwater ecosystem processes.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2016

Model-based analysis of environmental controls over ecosystem primary production in an alpine tundra dry meadow

We investigated several key limiting factors that control alpine tundra productivity by developing an ecosystem biogeochemistry model. The model simulates the coupled cycling of carbon (C), nitrogen (N), and phosphorus (P) and their interactions with gross primary production (GPP). It was parameterized with field observations from an alpine dry meadow ecosystem using a global optimization strategy to estimate the unknown parameters. The model, along with the estimated parameters, was first validated against independent data and then used to examine the environmental controls over plant productivity. Our results show that air temperature is the strongest limiting factor to GPP in the early growing season, N availability becomes important during the middle portion of the growing season, and soil moisture is the strongest limiting factors by late in the growing season. Overall, the controls over GPP during the growing season, from strongest to weakest, are soil moisture content, air temperature, N availability, and P availability. This simulation provides testable predictions of the shifting nature of physical and nutrient limitations on plant growth. The model also indicates that changing environmental conditions in the alpine will likely lead to changes in productivity. For example, warming eliminates the control of P availability on GPP and makes N availability surpass air temperature to become the second strongest limiting factor. In contrast, an increase in atmospheric nutrient deposition eliminates the control of N availability and enhances the importance of P availability. Furthermore, these analyses provide a quantitative and conceptual framework that can be used to test predictions and refine ecological analyses at this long-term ecological research site.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2025

The Freundlich isotherm equation best represents phosphate sorption across soil orders and land use types in tropical soils of Puerto Rico

Biomass production in the lowland wet tropical forest is greater than in any other biome, and it is typically limited by soil phosphorus (P) availability. However, the mechanisms involved in the P cycle remain poorly represented in Earth System Models (ESMs). Soil P sorption processes are key in the P cycle and for understanding the extent of P limitation for plant productivity. Currently, a few ESMs include isotherm equations to model these processes. Although the Langmuir equation is widely cited, other isotherm equations may better describe sorption in tropical soils. Here, we use a diverse range of soil samples from Puerto Rico to test the validity of the Langmuir, Freundlich, and Temkin equation. We found that across four soil orders (Inceptisols, Mollisols, Oxisols, Ultisols), and forested and cultivated land use types, the Freundlich equation best represented soil P sorption. Furthermore, the Langmuir and the Temkin equations poorly represent soil P adsorption, especially at low P concentrations. Specifically, the Langmuir equation underestimated soil P adsorption by 40% and the Temkin equation overestimated adsorption by 76%. We also found, as expected, that soil clay content and pH were the most important parameters explaining the variability of the Freundlich (K f ) constant. Greater clay content and lower pH, common in highly weathered Ultisols and Oxisols which are abundant in the tropics, led to greater K f values. Overall, our results suggest that a diversity of soils can prompt underestimation of P sorption when using the Langmuir isotherm, which leads to an overestimation of available P that can have repercussions on ESM predictions of the P cycle and tropical forest productivity.

Earth system models↗
DOE OSTI2018

Biodegradable Polymer Composites as Coating Materials for Granular Fertilizers

The composites consisting of poly(vinyl alcohol), horn meal, rapeseed cake, glycerol and phosphogypsum were proposed for the encapsulation of mineral fertilizers. Poly(vinyl alcohol) was used as a binder. The other components making ca. 70% of the mass of the composites were waste materials or by-products. They contain phosphorus, nitrogen, calcium, potassium and sulphur, which are useful nutrients for plants. The effect of the amount of glycerol and of the composition of the mixture of the fillers on the mechanical, sorption properties, water vapour permeability, solubility in water, dimensional stability of the composite films was studied. The addition of phosphogypsum and increase of the concentration of glycerol in the composites lead to the decrease of the tensile strength, water vapour permeability and to the increase of elongation at break and of the solubility of the composite films in water. The composites prepared were used for encapsulation of fertilizers. It was established that encapsulation resulted in the increase of the time of release of the fertilizers. In addition, encapsulation improved mechanical properties of the fertilizers. The fertilizer granules were coated with composite films and tested in the cultivation of tomato sprouts. They showed considerable positive effect on the development of the roots of the plants.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

Reactions of cyclohexene-annulated 3а,6а-diaza-1,4-diphosphapentalene with sulfur, selenium, and CS{sub 2}: structural features of zwitterionic products

The reactions of b- and f-face cyclohexene-annulated 3a,6a-diaza-1,4-diphosphapentalene (CADDP) with elemental sulfur and selenium result in the addition of two chalcogen atoms to one phosphorus atom of CADDP. A specific feature of these structures is that the diazadiphosphapentalene skeleton retains planar geometry, with a significant elongation of the N—P bond. These compounds are zwitterions, as evidenced by their electronic structures, with considerable delocalization of the negative charge in the PS{sub 2} (PSe{sub 2}) moieties and of the positive charge in the diazaphosphole ring. The reaction of CADDP with carbon disulfide is a more complicated process accompanied by the decomposition of the CS{sub 2} molecule to form a molecule containing three structurally different CADDP moieties, one of which is a stabilized carbene complex.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Synthesis and structures of zirconium complexes [Et{sub 2}H{sub 2}N]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–}, [Me{sub 3}NCH{sub 2}Ph]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–}•MeCN, [Ph{sub 3}PC{sub 6}H{sub 4}(CHPh{sub 2}-4)]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–}•2 MeCN, and [Ph{sub 4}Sb]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–}

The complexes [Et{sub 2}H{sub 2}N]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–} (1), [Me{sub 3}NCH{sub 2}Ph]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–}•MeCN (2), [Ph{sub 3}PC{sub 6}H{sub 4}(CHPh{sub 2}-4)]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–}•2 MeCN (3), and [Ph{sub 4}Sb]{sup +}{sub 2}[ZrCl{sub 6}]{sup 2–} (4) were synthesized by the reaction of zirconium tetrachloride with tetraorganylammonium, -phosphonium, and -stibonium chlorides in acetonitrile and structurally characterized. The nitrogen, phosphorus, and antimony atoms in the cations have a distorted tetrahedral geometry. The Zr–Cl distances in the centrosymmetric octahedral [ZrCl{sub 6}]{sup 2−} anions of complexes 1–4 have similar values, the longest bonds being observed in the anion of complex 4. Acetonitrile molecules are involved in the structural organization of the crystals of complex 3via weak hydrogen bonding with phenyl hydrogen atoms of the organylphosphonium cations. In the crystal of 2, no hydrogen bonds between the cations and solvent molecules are observed; acetonitrile molecules fill the cavities formed by cations and anions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Bisdiamidophosphite with a bisoxazoline moiety in palladium-catalyzed enantioselective allylation

A bisdiamidophosphite ligand with stereogenic phosphorus atoms as a part of 1,3,2-diaza-phospholidine rings and a bisoxazoline backbone was synthesized and studied in the Pd-catalyzed asymmetric allylic substitution. The use of this ligand provided up to 93% ee in the alkylation of (E)-1,3-diphenylallyl acetate with dimethyl malonate and up to 77% ee in the amination with pyrrolidine at quantitative conversion of the starting substrate.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Integrated Use of Maize Bran Residue for One-Step Phosphate Bio-Fertilizer Production

The development of bio-fertilizer inoculants is important and desirable. Two phosphate-solubilizing Bacillus subtilis strains were inoculated onto maize bran residue (MBR), which was used as bio-fertilizer carrier and a primary source of nutrients in a medium used for semi-solid fermentation. Water holding capacity, swelling capacity, scanning electron microscopy, and shelf-life assays demonstrated that ground MBR had satisfactory properties for a bio-fertilizer carrier. The maximal soluble phosphorus (P) reached 642.7 ± 0.43 mg l{sup −1} in an orthogonal test under the following optimal conditions: a pH of 7.0, a cultivation temperature of 31 °C, a medium water content of 160%, and a filling capacity of 500 g l{sup −1}. The bio-fertilizer produced by MBR improved the growth of wheat (Triticum aestivum L.) and Chinese cabbage (Brassica rapa pekinensis) with respect to plant height (by up to 18.36%) and the lengths of roots (by up to 34.03%, 27.22%, separately) in a pot experiment. This study integrated the production and storage of a bio-fertilizer to realize the one-step production of a solid bio-fertilizer using MBR.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2011

Influence of strontium on structure, sintering and biodegradation behaviour of CaO-MgO-SrO-SiO2-P2O5-CaF2 glasses

The present study investigates the influence of SrO on structure, apatite forming ability, physico-chemical degradation and sintering behaviour of melt-quenched bioactive glasses with composition: mol.% (36.07 – x) CaO – x SrO - 19.24 MgO – 5.61 P2O5 – 38.49 SiO2 – 0.59 CaF2, where x varies between 0 – 10. The detailed structural analysis of glasses has been made by infra red spectroscopy (FTIR) and magic angle spinning-nuclear magnetic resonance spectroscopy (MAS-NMR). Silicon was predominantly present as Q2 (Si) species while phosphorus was found in orthophosphate type environment in all the investigated glasses. The apatite forming ability of glasses was investigated by immersion of glass powders in simulated body fluid (SBF) for time durations varying between 1 h – 7 days. While increasing Sr2+/Ca2+ ratio in glasses did not affect the structure of glasses significantly, their apatite forming ability was decreased considerably. Further, physico-chemical degradation of glasses has been studied in accordance with ISO 10993-14 “Biological evaluation of medical devices – Part 14: Identification and quantification of degradation products from ceramics” in Tris HCl and citric acid buffer and the possible implications of ion release profile from glasses in different solutions has been discussed. The addition of strontium in glasses led to a 7-fold decrease in chemical degradation of glasses in Tris-HCl. The sintering of glass powders rendered glass-ceramics (GCs) with varying degree of crystallinity and good flexural strength (98-131 MPa) where the mechanical properties depend on the nature and amount of crystalline phases present in GCs.

58 GEOSCIENCES↗
DOE OSTI2011

Alkali-free bioactive glasses for bone tissue engineering: A preliminary investigation

An alkali-free series of bioactive glasses has been designed and developed in the glass system CaO-MgO-SiO2-P2O5-CaF2 along diopside (CaMgSi2O6) – fluorapatite [Ca5(PO4)3F] – tricalcium phosphate (3CaO•P2O5) join. The silicate network in all the investigated glasses is predominantly coordinated in Q2 (Si) units while phosphorus tends to remain in orthophosphate (Q0) environment. The in vitro bioactivity analysis of glasses has been made by immersion of glass powders in simulated body fluid (SBF) while chemical degradation has been studied in Tris-HCl in accordance with ISO-10993-14. Some of the investigated glasses exhibit hydroxyapatite (HA) formation on their surface with in 1-12 h of their immersion in SBF solution. The sintering and crystallization kinetics of glasses has been investigated by differential thermal analysis (DTA) and hot-stage microscopy (HSM), respectively while the crystalline phase evolution in resultant glass-ceramics (GCs) has been studied in the temperature range of 800-900 oC using powder X-ray diffraction (XRD) and scanning electron microscope (SEM). The cell growth and osteogenic differentiation for glasses has been studied in vitro on sintered glass powder compacts using rat bone marrow mesenchymal stem cells. The as designed glasses are ideal candidates for their potential applications in bone tissue engineering in the form of bioactive glasses as well as glass/GC scaffolds.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

CO 2 -assisted ethane aromatization over zinc and phosphorous modified ZSM-5 catalysts

The tandem reactions of CO 2 -assisted oxidative dehydrogenation and aromatization (CO 2 -ODA) of ethane were investigated over ZSM-5 modified with zinc (Zn) and phosphorus (P) by experimental studies and DFT calculations. The nature of active Zn species and their interaction with P were elucidated for understanding Zn/P-ZSM-5 catalyzed CO 2 -ODA reaction of ethane. Compared to the direct dehydrogenation and aromatization (DDA) reaction, the Zn/P-ZSM-5 catalyst possessed higher ethane conversion, enhanced aromatics yield, and better stability in the CO 2 -ODA reaction. Here, the presence of CO 2 reduced the carbon deposition, stabilized the Zn species, and thereby facilitated the generation of more liquid aromatics in CO 2 -assisted ethane aromatization. In situ characterization and DFT calculations provided insight into the mechanisms of CO 2 -ODA over the Zn/P-ZSM-5 catalyst.

36 MATERIALS SCIENCE↗
DOE OSTI2011

Structural and Mechanistic Insights into C-P Bond Hydrolysis by Phosphonoacetate Hydrolase

Bacteria have evolved pathways to metabolize phosphonates as a nutrient source for phosphorus. In Sinorhizobium meliloti 1021, 2-aminoethylphosphonate is catabolized to phosphonoacetate, which is converted to acetate and inorganic phosphate by phosphonoacetate hydrolase (PhnA). Here we present detailed biochemical and structural characterization of PhnA that provides insights into the mechanism of C-P bond cleavage. The 1.35 {angstrom} resolution crystal structure reveals a catalytic core similar to those of alkaline phosphatases and nucleotide pyrophosphatases but with notable differences, such as a longer metal-metal distance. Detailed structure-guided analysis of active site residues and four additional cocrystal structures with phosphonoacetate substrate, acetate, phosphonoformate inhibitor, and a covalently bound transition state mimic provide insight into active site features that may facilitate cleavage of the C-P bond. These studies expand upon the array of reactions that can be catalyzed by enzymes of the alkaline phosphatase superfamily.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2012

Ab Initio Study of Defect Properties in YPO4

Ab initio methods based on density functional theory have been used to calculate the formation energies of intrinsic defects, including vacancies, interstitials, antisites and Frenkel pairs in YPO4 under the O-rich and Y2O3-rich, and the O-rich and Y-rich conditions. The larger size of the yttrium atom may give rise to higher formation energy of the phosphorus antisite defect. In general, the formation energies of anion interstitials are much smaller than those of cation interstitials for both conditions considered. It is of greatly interest to find that the relative stabilities among the same types of interstitials are independent of the reference states. The most stable configuration for oxygen interstitials is an O-O split interstitial near the Ta site, while the most stable configuration for cation interstitials is a tetrahedral interstitial near the Ta site. The cation split interstitials are unfavorable in YPO4, with much higher formation energies. Furthermore, the properties of Frenkel pairs are compared with those calculated using empirical potentials. The results reveal that both ab initio and empirical potential calculations show a similar trend in the formation energies of Frenkel pairs, but the formation energies obtained by empirical potentials are much larger than those calculated by ab initio method.

36 MATERIALS SCIENCE↗
DOE OSTI2023

ARSK1 activates TORC1 signaling to adjust growth to phosphate availability in Arabidopsis

Nutrient sensing and signaling are essential for adjusting growth and development to available resources. Deprivation of the essential mineral phosphorus (P) inhibits root growth. The molecular processes that sense P limitation to trigger early root growth inhibition are not known yet. Target of rapamycin (TOR) kinase is a central regulatory hub in eukaryotes to adapt growth to internal and external nutritional cues. How nutritional signals are transduced to TOR to control plant growth remains unclear. Here, we identify Arabidopsis-root-specific kinase 1 (ARSK1), which attenuates initial root growth inhibition in response to P limitation. We demonstrate that ARSK1 phosphorylates and stabilizes the regulatory-associated protein of TOR 1B (RAPTOR1B), a component of the TOR complex 1, to adjust root growth to P availability. Finally, these findings uncover signaling components acting upstream of TOR to balance growth to P availability.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Hedonic Price Estimates of Lake Water Quality: Valued Attribute, Instrumental Variables, and Ecological-Economic Benefits

We estimate the effect of lake water quality on residential housing prices using cross-sectional data on water clarity from 113 lakes across the United States. An instrumental-variables approach is developed to address potential endogeneity bias in the water-clarity variable. Three lake-based physical variables serve as instrumental variables: total nitrogen concentration in lake water, total phosphorus concentration in lake water, and water temperature near the lake surface. The econometric results include three methodological findings: the instruments are valid and strong; the ordinary-least-squares estimate of the coefficient on the water-clarity variable is unbiased; and water clarity is the attribute of water quality valued in the housing market. The estimated water-clarity effect shows that a one-tenth of a meter change in water clarity leads to a one-percent change in housing price, or an elasticity of 0.20 at mean clarity. Coupling this effect with estimates of an ecological production function, a lake-specific benefit index is developed that shows the effect on housing values of bringing lakes into compliance with the US Environmental Protection Agency's regional recommendations for phosphorous concentration in lake waters.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2011

High voltage stability of LiCoO2 particles with a nano-scale Lipon coating

For high-voltage cycling of rechargeable Li batteries, a nano-scale amorphous Li-ion conductor, lithium phosphorus oxynitride (Lipon), has been coated on surfaces of LiCoO{sub 2} particles by combining a RF-magnetron sputtering technique and mechanical agitation of LiCoO{sub 2} powders. LiCoO{sub 2} particles coated with 0.36 wt% ({approx}1 nm thick) of the amorphous Lipon, retain 90% of their original capacity compared to non-coated cathode materials that retain only 65% of their original capacity after more than 40 cycles in the 3.0-4.4 V range with a standard carbonate electrolyte. The reason for the better high-voltage cycling behavior is attributed to reduction in the side reactions that cause increase of the cell resistance during cycling. Further, Lipon coated particles are not damaged, whereas uncoated particles are badly cracked after cycling. Extending the charge of Lipon-coated LiCoO{sub 2} to higher voltage enhances the specific capacity, but more importantly the Lipon-coated material is also more stable and tolerant of high voltage excursions. A drawback of Lipon coating, particularly as thicker films are applied to cathode powders, is the increased electronic resistance that reduces the power performance.

25 ENERGY STORAGE↗
DOE OSTI2018

Combining biotechnology with circular bioeconomy: From poultry, swine, cattle, brewery, dairy and urban wastewaters to biohydrogen

Highlights: • Poultry, swine, cattle, brewery, dairy and urban WWs could be microalga-based treated. • Removal efficiency ranges were 95–100% for N, 63–99% for P and 48–70% for COD. • Higher biohydrogen production yield was obtained using poultry and swine wastewaters. The ability of microalgae to grow in nutrient-rich environments and to accumulate nutrients from wastewaters (WW) makes them attractive for the sustainable and low-cost treatment of WW. The valuable biomass produced can be further used for the generation of bioenergy, animal feed, fertilizers, and biopolymers, among others. In this study, Scenedesmus obliquus was able to remove nutrients from different wastewaters (poultry, swine and cattle breeding, brewery and dairy industries, and urban) with removal ranges of 95–100% for nitrogen, 63–99% for phosphorus and 48–70% for chemical oxygen demand. The biomass productivity using wastewaters was higher (except for poultry) than in synthetic medium (Bristol), the highest value being obtained in brewery wastewater (1025 mg/(L.day) of freeze-dried biomass). The produced biomass contained 31–53% of proteins, 12–36% of sugars and 8–23% of lipids, regardless of the type of wastewater. The potential of the produced Scenedesmus obliquus biomass for the generation of BioH{sub 2} through batch dark fermentation processes with Enterobacter aerogenes was evaluated. The obtained yields ranged, in mL H{sub 2}/g Volatile Solids (VS), from 50.1 for biomass from anaerobically digested cattle WW to 390 for swine WW, whereas the yield with biomass cultivated in Bristol medium was 57.6 mL H{sub 2}/g{sub VS}.

60 APPLIED LIFE SCIENCES↗