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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Modeling simultaneous particle shrinkage, dissolution and breakage using the modified moving grid technique

Simultaneous shrinkage, dissolution and breakage are important particle size reduction phenomena that characterize processes like the reactive degradation of solid chemicals. The dynamics of the particle size distribution (PSD) for such processes are non-trivial to model due to the number expending processes brought about by the eventual dissolution of particles. To this end, Population Balance Model (PBM) resolved through the sectional techniques is the natural approach. Here, we introduce a modified Moving Grid technique (m-MGT) to accurately resolve the particle size reduction phenomena. Our technique mimics the perpetual particle shrinkage through a continuously left-moving size grid and incorporates a strategic grid removal routine to capture the disappearance of particles. Coupled with the Fixed Pivot (FP) discretization for breakage, our m-MGT not only preserves the moment-related properties, but also benchmarked very well against the analytical number densities and exhibited a minimum of first-order convergence in all assessed case studies.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2016

Investigating Dissolution and Precipitation Phenomena with a Smartphone Microscope

A novel smartphone microscope can be used to observe the dissolution and crystallization of sodium chloride at a microscopic level. Observation of these seemingly simple phenomena through the microscope at 100× magnification can actually reveal some surprising behavior. These experiments offer the opportunity to discuss some basic concepts such as how the morphological features of the crystals dictates how the dissolution process proceeds, and how materials can be purified by re-crystallization techniques.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Elucidating the Atomic Structures of the Gel Layer Formed during Aluminoborosilicate Glass Dissolution: An Integrated Experimental and Simulation Study

The altered glasses produced during aqueous dissolution of silicate and borosilicate glasses are among the most complex structures to understand at the atomic level due to their amorphous nature, random porosity and various levels of hydration. In this study, we gained insights of the complex atomic structures of altered aluminoborosilicate glasses by combining a range of experimental and computational approaches. The altered glasses were prepared by dissolution of three glasses with varying level of alumina in acid for 7 days. A comprehensive set of experimental [elemental analysis, high-energy X-ray diffraction, 29 Si and 27 Al solid-state nuclear magnetic resonance (NMR), and O 1s X-ray photoelectron spectroscopy (XPS)] and modeling (molecular dynamics (MD) simulations using non-reactive and reactive force fields) were used to study the atomic structures of these altered glasses. Elemental analysis showed that most of the B in the pristine glasses was leached into the solution and was not contained in the altered glass. The 29 Si and 27 Al solid-state NMR spectra revealed that the altered glasses have more polymerized silicate network as compared to those in the pristine glasses due to the reformation of linkages among Si and Al oxygen polyhedral in the altered glasses. The bridging and non-bridging (or hydroxyl O) atoms in the altered glasses were also quantified from their O 1s XPS spectra. Atomic structure models of the altered glasses were constructed by using MD simulations using the reactive force field based on the compositional information obtained from experiments. Various pore structures were generated using the charge-scaling (CS) method by using different initial densities and CS temperatures; the best CS parameters of each alternated glass were then determined by comparing with the experimental structure factors obtained from high energy X-ray diffraction. Pore and the atomic structures and vibrational properties around these pore surfaces were analyzed. Furthermore, these results from this comprehensive study thus provides a realistic insight into the pore morphology, atomic structure, and vibrational properties of altered glasses.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Role of Disproportionation in the Dissolution of Mn from Lithium Manganate Spinel

Dissolution of Mn from lithium-manganese spinel has hindered its commercialization as a cathode material in Li-ion batteries. Disproportionation of near-surface Mn(III), in the presence of acid, has been widely thought to result in dissolved divalent Mn. To what extent stray acidic water in the cell (as opposed to the organic electrolyte) acts as the solvent for Mn ions has not been established. Simulations by Leung show that a small displacement of trivalent Mn from its equilibrium site at an LiMn 2 O 4 (001)/ ethylene carbonate interface leads to its reduction to Mn(II). In the present work, Thermodynamic Integration is performed, based on first-principles molecular dynamics simulations within the Blue-Moon ensemble, for the detachment of Mn(III) ions at the LiMn 2 O 4 (001)/water interface. The results show that reduction of Mn(III) to Mn(II) occurs also in the case of an aqueous interface. The simulations were performed for both neutral and acidic water (in the presence of HF), with the coordination number of the dissolving Mn ion with substrate oxygen ions taken as the reaction coordinate. The simulations indicate that an F - ion strongly binds to a surface Mn(III) ion, and weakens its adhesion to the substrate. Owing to this weakening, a surface Mn-F complex traverses regions of phase space at room temperature where disproportionation becomes energetically favorable. Although this disproportionation occurs close to the substrate, where the Mn coordination number is only slightly lowered from its equilibrium value, we argue that the likelihood of reattachment after disproportionation is small (Leung arrived at a similar interpretation in the case of the LiMn 2 O 4 (001)/ EC interface). We suggest that the critical role of F - in promoting dissolution is to weaken the Mn binding to the substrate so as to enable disproportionation. The partially detached MnF complex may then undergo additional interaction with the solvent to form, e.g., MnF 2 , which would enable transport away from the substrate. In conclusion, the EPR measurements by Shilina et al. which appear to show Mn(III) as the predominant solvated species are discussed.

25 ENERGY STORAGE↗
DOE OSTI2019

Hot Holes Assist Plasmonic Nanoelectrode Dissolution

Strong light-absorbing properties allow plasmonic metal nanoparticles to serve as antennas for other catalysts to function as photocatalysts. To achieve plasmonic photocatalysis, the hot charge carriers created when light is absorbed must be harnessed before they decay through internal relaxation pathways. We demonstrate the role of photogenerated hot holes in the oxidative dissolution of individual gold nanorods with millisecond time resolution while tuning charge-carrier density and photon energy using snapshot hyperspectral imaging. In this work, we show that light-induced hot charge carriers enhance the rate of gold oxidation and subsequent electrodissolution. Importantly, we distinguish how hot holes generated from interband transitions versus hot holes around the Fermi level contribute to photooxidative dissolution. The results provide new insights into hot-hole-driven processes with relevance to photocatalysis while emphasizing the need for statistical descriptions of nonequilibrium processes on innately heterogeneous nanoparticle supports.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Tuning the Selectivity of Carboxylic Acid–Based Eutectic Solvents for the Dissolution and Electrochemical Separation of Metal Oxides

Extracting metals from natural resources and recovering from waste materials with less-hazardous solvents is essential for sustainable technological advancements. The commonly employed method utilizes harsh chemicals for metal dissolution and the ensuing separation. Here, in this study, we examined the potential of eutectic solvents (types III and IV) as alternative media for the selective dissolution of metals and metal oxides and their subsequent electrochemical separation. Notably, type III eutectics composed of betaine:acetic acid and triazole:lactic acid exhibited excellent solubility for cobalt oxide (24.1 g·L –1 ) and copper oxide (30.5 g·L –1 ), respectively. In comparison, the type IV eutectic mixture of Ca(NO 3 ) 2 ·4H 2 O:acetic acid demonstrated the highest conductivity and lowest viscosity with solubility for both copper oxide (6.1 g·L –1 ) and metallic copper (5.4 g·L –1 from a used electronic circuit). Using a Ca(NO 3 ) 2 ·4H 2 O:acetic acid mixture, copper was selectively dissolved from a waste printed circuit board and subsequently electrodeposited onto a nickel electrode. These findings highlight the tunability of DESs for the selective recovery of metals from electronic waste, offering a promising approach for sustainable metal recycling and resource recovery.

electrodeposition↗
DOE OSTI2024

Quantifying Dissolution Dynamics in Porous Media Using a Spatial Flow Focusing Profile

Abstract The diverse range of patterns in porous media formed by dissolution processes depends on the relative magnitude of flow, transport, and chemical reactions at pore surfaces. However, distinguishing between regimes often relies solely on qualitative, visual comparisons of emergent structures. Here, we propose a quantitative measure capable of identifying different regimes using the concept of the spatial flow focusing profile, which segments the medium into cross sections along the flow direction to calculate the flow focusing index for each section. We employ this measure in numerical simulations of a dissolving porous medium using a pore network model. We obtain a morphological phase diagram of dissolution patterns, which we characterize using the flow focusing profile. In particular, we demonstrate that analyzing the temporal changes in the profile allows one to quantitatively distinguish between wormholing and channeling. The transition between them is shown to be affected by the heterogeneity of the system.

58 GEOSCIENCES↗
DOE OSTI2014

Swift heavy ion irradiation of Pt nanocrystals: I. shape transformation and dissolution

We report on the effects of swift heavy ion irradiation of embedded Pt nanocrystals (NCs), which change from spheres to prolate spheroids to rods upon irradiation. Using a broad range of ion irradiation energies and NC mean sizes we demonstrate that the elongation and dissolution processes are energy and size dependent, attaining comparable levels of shape transformation and dissolution upon a given energy density deposited in the matrix. The NC shape transformation remains operative despite discontinuous ion tracks in the matrix and exhibits a constant threshold size for elongation. In contrast, for ion irradiations in which the ion tracks are continuous, the threshold size for elongation is clearly energy dependent.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2019

Fabrication of Uniform Nanoparticulate Gold through Potential-Modulated Electrochemical Deposition and Dissolution of Silver in Ionic Liquids

Nanoparticulate gold (NPG) has been successfully produced from polycrystalline Au by a novel method based on potential-modulated electrochemical deposition and dissolution of silver in an ionic liquid bath comprising of 1-ethyl-3-methylimidazolium chloride and silver nitrate at elevated temperatures. Cyclic voltammetric measurements exhibit that the potential cycles between -1.0 and 0.75 V versus a silver pseudo reference electrode can drive the electrochemical deposition and dissolution of silver onto and away from the Au electrode. Scanning electron microscope studies show that the NPG resulting from the potential cycles has very narrow particle size distribution with an average diameter of approximately 50 nm and is free of elemental Ag residue. As compared to a bulk Au electrode, the NPG electrode demonstrates substantially enhanced electrochemical responses. It exhibits a seven-time higher electro-catalytic activity towards the electrooxidation of nitrite in acidic media.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Testing of the Defense Waste Processing Facility Cold Chemical Dissolution Method in Sludge Batch 9 Qualification

For each sludge batch that is processed in the Defense Waste Processing Facility (DWPF), the Savannah River National Laboratory (SRNL) tests the applicability of the digestion methods used by the DWPF Laboratory for elemental analysis of Sludge Receipt and Adjustment Tank (SRAT) Receipt samples and SRAT Product process control samples. DWPF SRAT samples are typically dissolved using a method referred to as the DWPF Cold Chemical or Cold Chem Method (CC), (see DWPF Procedure SW4- 15.201). Testing indicates that the CC method produced mixed results. The CC method did not result in complete dissolution of either the SRAT Receipt or SRAT Product with some fine, dark solids remaining. However, elemental analyses did not reveal extreme biases for the major elements in the sludge when compared with analyses obtained following dissolution by hot aqua regia (AR) or sodium peroxide fusion (PF) methods. The CC elemental analyses agreed with the AR and PF methods well enough that it should be adequate for routine process control analyses in the DWPF after much more extensive side-by-side tests of the CC method and the PF method are performed on the first 10 SRAT cycles of the Sludge Batch 9 (SB9) campaign. The DWPF Laboratory should continue with their plans for further tests of the CC method during these 10 SRAT cycles.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Final Report of Tank 241-C-105 Dissolution, the Phase 2 Study

Three clamshell grab samples were taken from Tank 241-C-105 in October 2015 in accordance with RPP-PLAN-60011. Analytical results of those samples were issued in the report RPP-RPT-59115 by Wastren Advantage, Inc., Hanford Laboratory. Solid phase characterization results were reported separately in LAB-RPT-15-00011 and in RPP-RPT-59147. The major solid phases reported to be present were dawsonite [NaAlCO 3 (OH) 2 ], trona [Na 3 (HCO 3 )(CO 3 )·2H 2 O], cejkaite [Na 4 (UO 2 )(CO 3 ) 3 ], and an unidentified organic solid, with minor amounts of gibbsite [Al(OH) 3 ], natrophosphate [Na 7 F(PO 4 ) 2 ·19H 2 O], and traces of unidentified iron-rich and manganese-rich phases. Note that the presence of dawsonite, trona, and cejkaite requires a relatively low pH, likely around pH 9 to 10. One aliquot of each grab sample was provided to 222-S Laboratory Process Chemistry for dissolution studies. Phase 1 of the dissolution testing followed the approved test plan, WRPS-1404813, Rev. 3, and examined the behavior of the Tank 241-C-105 solids treated with water, 19M sodium hydroxide, 2M nitric acid, and 0.5M oxalic acid/2M nitric acid. Phase 2 of the testing was conducted in accordance with instructions from the client and emphasized treatment with 19M sodium hydroxide followed by water washing. This is the report of the Phase 2 testing.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2016

Radiochemical purity of Mo and Tc solution obtained after irradiation and dissolution of Mo-100-enriched and ultra-high-purity natural Mo disks

Four irradiations of ultra-high-purity natural Mo targets and one irradiation using 97.4% Mo-100-enriched material were performed. The purpose of these irradiations was to determine whether the presence of Sn stabilizer in the H 2 O 2 used for the dissolution of sintered Mo disks can affect the radiochemical purity of the final K 2 MoO 4 in 5M KOH solution. Results from radiochemical purity tests performed using thin-layer paper chromatography show that even 2– 3× excess of Sn-stabilized H 2 O 2 typically used for dissolution of sintered Mo disks did not affect the radiochemical purity of the final product.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2017

Glass composition and solution speciation effects on stage III dissolution

To understand and mitigate the onset of Stage III corrosion of multicomponent oxides waste glasses. Stage III refers to a resumption of the high initial rate of glass dissolution in some glass samples that have otherwise exhibited dissolution at the much lower residual rate for a long time (Stage II). Although the onset of Stage III is known to occur concurrently with the precipitation of particular alteration products, the root cause of the transition is still unknown. Certain glass compositions (notably AFCI) and high pH environmental conditions are also associated with this observed transition.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Ruthenium Volatiliazation During Dissolution of Spent Nuclear Fuels in H-Canyon Dissolvers

During nuclear material processing, many radioactive elements form volatile species under certain process conditions which may allow release to the environment unless they are removed from offgas streams. Ruthenium, a product from the fission of U, will form a volatile compound (RuO 4 ) under highly oxidizing conditions which may be released during spent nuclear fuel (SNF) dissolution. The principal Ru isotopes of concern are 103 Ru and 106 Ru with half-lives of 39.27 and 372.6 days, respectively. Ruthenium-103 will decay to less than 1% of its initial activity within one year; therefore, its presence is not a concern for fuel cooled more than one year after discharge. However, the half-life of 106 Ru is sufficiently long that it will persist for many years at levels of concern. The isotope does not decay to less than 1% of its initial activity until approximately 6.8 years. Therefore, the dissolution of SNF cooled for less than approximately 7 years is defined as processing short-cooled fuel as it relates to Ru volatilization.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Microbial- and thiosulfate-mediated dissolution of mercury sulfide minerals and transformation to gaseous mercury

Mercury (Hg) is a toxic heavy metal that poses significant environmental and human health risks. Soils and sediments, where Hg can exist as the Hg sulfide mineral metacinnabar (β-HgS), represent major Hg reservoirs in aquatic environments. Metacinnabar has historically been considered a sink for Hg in all but severely acidic environments, and thus disregarded as a potential source of Hg back to aqueous or gaseous pools. In this study, we conducted a combination of field and laboratory incubations to identify the potential for metacinnabar as a source of dissolved Hg within near neutral pH environments and the underpinning (a)biotic mechanisms at play. We show that the abundant and widespread sulfur-oxidizing bacteria of the genus Thiobacillus extensively colonized metacinnabar chips incubated within aerobic, near neutral pH creek sediments. Laboratory incubations of axenic Thiobacillus thioparus cultures led to the release of metacinnabar-hosted Hg(II) and subsequent volatilization to Hg(0). This dissolution and volatilization was greatly enhanced in the presence of thiosulfate, which served a dual role by enhancing HgS dissolution through Hg complexation and providing an additional metabolic substrate for Thiobacillus . These findings reveal a new coupled abiotic-biotic pathway for the transformation of metacinnabar-bound Hg(II) to Hg(0), while expanding the sulfide substrates available for neutrophilic chemosynthetic bacteria to Hg-laden sulfides. Lastly, they also point to mineral-hosted Hg as an underappreciated source of gaseous elemental Hg to the environment.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

The Effect of Bicarbonate on Autunite Dissolution in the Presence of Shewanella oneidensis under Oxygen Restricted Conditions - 16429

Uranium is a key contaminant at many U.S. Department of Energy sites that served a leading role in the nation's defense for over 50 years. Uranium contamination of soil and groundwater is of great environmental concern due to the toxicological properties of the uranyl species. In an effort to decrease the concentration of soluble uranium, tripolyphosphate injections were identified as a feasible remediation strategy for sequestering uranium in situ in contaminated groundwater at the Hanford Site (WA). The introduction of sodium tripolyphosphate into uranium-bearing porous media results in the formation of uranyl phosphate minerals (autunite) of general formula (X{sub 1-2}[(UO{sub 2})(PO{sub 4})]{sub 2-1}.nH{sub 2}O), where X is a monovalent or divalent cation. The stability of the uranyl phosphate minerals in the subsurface is a critical factor since it determines the long-term effectiveness of the sodium tripolyphosphate injection as a remediation strategy. The behavior of uranium and its mobility in the subsurface are affected by various factors such as the chemistry of pore water, groundwater and soil minerals, the presence of complex-forming ligands, and micro-organisms that thrive under these conditions. Bicarbonate presence in the aqueous phase facilitates uranium desorption from soil and sediments and promotes the release of U(VI) into the aqueous phase, thus increasing uranium mobility in natural waters. In neutral or basic pH conditions, uranium can readily complex with a wide variety of ligands such as carbonate and form soluble uranyl-carbonato complexes such as UO{sub 2}(CO{sub 3}){sub 2}{sup 2-} and UO{sub 2}(CO{sub 3}){sub 3}{sup 4-}. Bicarbonate complexes have been identified in contaminated pore water at the Hanford Site. Furthermore, the presence of bacteria can significantly affect uranium mobility since bacteria may bio-enhance the release of U (VI) from uranyl-phosphate minerals, thus liberating uranium in the aqueous phase in an effort to obtain phosphorous, a vital nutrient for their metabolism. The Columbia River at the site exhibits large stage variations, causing fluctuations in the water table. These water table fluctuations and multiple rise-and-fall cycles in the river created an oxic-anoxic interface in this region. Previous assessments of Hanford sediment samples collected from this area noted a decline in cultivable aerobic bacteria and suggested the presence of facultative anaerobic bacteria. Shewanella oneidensis MR1 is a common bacterial group in soils and Shewanella species have been found in the Hanford soil. Shewanella oneidensis is a facultative anaerobic species which also belongs to a group known as dissimilatory metal-reducing bacteria (DMRB), due to their ability to reduce metals as a part of their metabolic pathway. Therefore, understanding the role of Shewanella is a critical factor affecting the outcome of environmental remediation. The objective of this research was to demonstrate the significance of bacteria-uranium interactions and investigate the effect of bicarbonate in the aqueous phase on Ca-autunite dissolution in the oxygen-restricted conditions. Sterile 100-mL glass mixed bioreactors with weighed amounts of ground Ca-autunite particles were used for initial experimentation. These autunite-containing bioreactors were injected with bacterial cells after the autunite equilibrated with the media solution amended with 0 mM, 3 mM 5 mM and 10 mM concentrations of bicarbonate. Additional abiotic samples were prepared without bacterial inoculation to provide a control for the biotic samples. The concentration of U(VI) determined in the aqueous phase was in direct correlation to the concentration of bicarbonate present in the solution. It was noted that an increase in bicarbonate concentration led to higher U(VI) concentration in the aqueous phase. A sharp decrease in U(VI) concentration was observed in the bicarbonate-free samples, probably due to a microbe mediated reduction of U(VI) to U(IV). In the case of samples amended with 3 mM bicarbonate, a slight, yet significant, decrease in U(VI) was also observed compared to the abiotic control. However, compared to the abiotic controls, there was no change in U(VI) levels in the aqueous phase as a result of bacterial inoculation for the samples amended with 5 and 10 mM bicarbonate for a period of time as long as 50 days. These results imply that the uranyl-carbonate complexes (UO{sub 2}(CO{sub 3}){sub 2}{sup 2-} and UO{sub 2}(CO{sub 3}){sub 3}{sup 4-}) that are present in carbonate-rich environments might be interfering with the microbial reduction in the oxygen- restricted conditions; however, this conclusion requires further investigation. Finally, the data indicate that release of U, P and Ca from autunite was non-stoichiometric. In conclusion, the high stability of uranyl-phosphate complexes makes them a strong candidate for the remediation efforts to sequester uranium in the subsurface. Nevertheless, in a bicarbonate-rich environment, Ca-autunite has a high probability of dissolution and the presence of metal-reducing bacteria does not seem to impede this process in the presence of higher bicarbonate concentrations under oxygen restricted conditions. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2015

Synchronization of dissolution and precipitation fronts during infiltration‐driven replacement in porous rocks

Abstract Coupled dissolution‐precipitation reactions, where two minerals share a common ion, occur frequently in geological replacement; the reactions are driven by an inflow of precipitating secondary ions and an outflow of dissolved primary ions. Although crystallization pressure is frequently invoked to explain volume‐preserving replacement, it cannot be operative if the chemical reactions lead to a loss of mineral volume; here the host rock that should confine the precipitating mineral is dissolving faster than the grains are growing. In this paper we propose two chemical mechanisms by which a rapid dissolution front and a slower precipitation front can be synchronized, and volume‐for‐volume replacement preserved. We analyze these mechanisms within the framework of reactive transport theory and show that morphological features observed in calcite replacement can be correlated with predictions of the models.

Kondratiuk, Paweł↗
DOE OSTI2021

Reducing Antisolvent Use in the STRAP Process by Enabling a Temperature–Controlled Polymer Dissolution and Precipitation for the Recycling of Multilayer Plastic Films

The recently reported processing strategy called solvent-targeted recovery and precipitation (STRAP) enables deconstruction of multilayer plastic packaging films into their constituent resins by selective dissolution. It uses a series of solvent washes that are guided by thermodynamic calculations of polymer solubility. In this work, the use of antisolvents in the STRAP process was reduced and solvent mixtures were considered to enable the temperature-controlled dissolution and precipitation of the target polymers in multilayer films. This was considered as a means to further improve the STRAP process and its estimated costs. Two STRAP approaches were compared based on different polymer precipitation techniques: precipitation by the addition of an antisolvent (STRAP-A) and precipitation by decreasing the solvent temperature (STRAP-B). Both approaches were able to separate the constituent polymers in a post-industrial film composed primarily of polyethylene (PE), ethylene vinyl alcohol (EVOH), and polyethylene terephthalate (PET) with near 100 % material efficiency. Technoeconomic analysis indicates that the minimum selling price (MSP) of the recycled resins with STRAP-B is 21.0 % lower than that achieved with STRAP-A. This provides evidence that thermally driven polymer precipitation is an option to reduce the use of antisolvents, making the STRAP process more economically and environmentally attractive. A third process, STRAP-C, was demonstrated with another post-industrial multilayer film of a different composition. Here, the results demonstrate that this process can also recover polymers at similar costs to those of virgin resins, indicating that the STRAP technology is flexible and can remain economically competitive as the plastic feed complexity is increased.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗