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Toggling Calcium Plating Activity and Reversibility through Modulation of Ca²⁺ Speciation in Borohydride-based Electrolytes.

ABSTRACT: Learning how to tailor Ca²⁺ speciation and electroactivity is of central importance to engineer next-generation battery electrolytes. Using an exemplar dual-salt electrolyte, Ca(BH₄)₂ + Ca(TFSI)₂ in THF, this work examines how to modulate a critical parameter proposed to govern electroactivity, the BH₄ ^-/Ca²⁺ ratio. Introduction of a more-dissociating source of Ca²⁺ via Ca(TFSI)₂ drives re-speciation of strongly ion-paired Ca(BH₄)₂, confirmed by ionic conductivity, Raman spectroscopy, and reaction microcalorimetry measurements, generating larger populations of charged species and enhancing plating currents. Ca plating is possible when [Ca(TFSI)₂] < [Ca(BH₄)₂] and thus BH₄ ^-/Ca²⁺ >1, but a dramatic shut-down of plating activity occurs when [Ca(TFSI)₂] > [Ca(BH₄)₂] (BH₄ ^-/Ca²⁺ <1), directly evidencing the significance of coordination-shell chemistry on plating activity. Ca(BH₄)₂ + TBABH₄ in THF, which enables enrichment of BH₄ ^- concentrations compared to Ca²⁺, is also examined; ionic conductivity and plating currents also increase compared to Ca(BH₄)₂/THF, with the latter related in part to a decrease in solution resistance. These findings delineate future directions to modulate Ca²⁺ coordination towards achieving both high plating activity and reversibility.

SUBMITTER: Melemed AM

PROVIDER: S-EPMC8792997 | biostudies-literature | 2022 Jan

REPOSITORIES: biostudies-literature

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Toggling Calcium Plating Activity and Reversibility through Modulation of Ca2+ Speciation in Borohydride-based Electrolytes.

Melemed Aaron M AM Skiba Dhyllan A DA Gallant Betar M BM

The journal of physical chemistry. C, Nanomaterials and interfaces 20220105 2

Learning how to tailor Ca2+ speciation and electroactivity is of central importance to engineer next-generation battery electrolytes. Using an exemplar dual-salt electrolyte, Ca(BH4)2 + Ca(TFSI)2 in THF, this work examines how to modulate a critical parameter proposed to govern electroactivity, the BH4 -/Ca2+ ratio. Introduction of a more-dissociating source of Ca2+ via Ca(TFSI)2 drives re-speciati ...[more]

PMID: 35096216

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Project description:The nutritional status of dairy cows and the metabolism of specific nutrients are critical regulators of immune cell function. Around the time of parturition, mobilization of body lipid and muscle helps compensate for the decrease in nutrient intake and the increased requirements of the mammary gland for lactation. An end-result of these processes is the marked increase in circulating concentrations of fatty acids (FA), which are a major risk factor for immune dysfunction. In food animal species such as dairy cows, any disturbance in nutritional or immunological homeostasis leads to deleterious feedback loops that can further risk health, efficiency of nutrient use, and compromise availability of safe and nutritious dairy foods for humans. Despite substantial progress with respect to regulation of innate immunity, such knowledge for adaptive immunity is scarce. To help bridge this gap in knowledge, we sought to study the role of calcium release-activated calcium modulator ORAI1 activation in T cells systemic immune function in vivo. CD4+ T cells were isolated from peripheral blood of dairy cows diagnosed as healthy or with ketosis, a common metabolic disorder of FA metabolism. Results revealed that levels of intracellular Ca2+ and reactive oxygen species (ROS) along with the abundance of store-operated Ca2+ entry (SOCE) moiety increased during ketosis. Further, plasma concentrations of inflammatory cytokines were elevated, the balance of Th17/Treg cells was disrupted, mitochondrial function impaired, and the abundance of mitophagy-related proteins in CD4+ T cells altered during ketosis. Molecular characterization of the direct effects of FA was evaluated in CD4+ T cells isolated from the spleen of 1-day-old calves. Enhanced supply of FA increased intracellular Ca2+ and ROS concentrations, upregulated the abundance of proteins associated with mitochondrial dynamics and ORAI1. Intermediates of mitophagy accumulated and the balance of Th17/Treg cells also was affected by the supply of FA. These negative effects were attenuated by silencing or inhibition of ORAI1 in CD4+ T cells. Together, data indicated that physiological states that lead to increases in systemic concentrations of FA could impact adaptive immunity negatively through ORAI1 regulated intracellular Ca2+, ROS balance, and increased effector functions of Th17 cells.

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Toggling Calcium Plating Activity and Reversibility through Modulation of Ca²⁺ Speciation in Borohydride-based Electrolytes.

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Toggling Calcium Plating Activity and Reversibility through Modulation of Ca<sup>2+</sup> Speciation in Borohydride-based Electrolytes.

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Toggling Calcium Plating Activity and Reversibility through Modulation of Ca2+ Speciation in Borohydride-based Electrolytes.

Publications

Toggling Calcium Plating Activity and Reversibility through Modulation of Ca&lt;sup&gt;2+&lt;/sup&gt; Speciation in Borohydride-based Electrolytes.

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OmicsDI is part of the ELIXIR infrastructure

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Toggling Calcium Plating Activity and Reversibility through Modulation of Ca²⁺ Speciation in Borohydride-based Electrolytes.

Toggling Calcium Plating Activity and Reversibility through Modulation of Ca<sup>2+</sup> Speciation in Borohydride-based Electrolytes.