Cation Anion Research Articles

Chemical Reduction of Iodine Impurities and Defects with Potassium Formate for Efficient and Stable Perovskite Solar Cells

AbstractThe performance of perovskite solar cells (PSCs) is negatively affected by iodine (I2) impurities generated from the oxidation of iodide ions in the perovskite precursor powder, solution, and perovskite films. In this study, the use of potassium formate (HCOOK) as a reductant to minimize the presence of detrimental I2 impurities is presented. It is demonstrated that HCOOK can effectively reduce I2 back to I− in the precursor solution as well as in the devices under external conditions. Furthermore, the introduced formate anion (HCOO−) and alkali metal cation (K+) can reduce the defect density within the perovskite film by modulating perovskite growth and passivating electronic defects, significantly prolonging the carrier lifetime and reducing the J–V hysteresis. Consequently, the maximum efficiency of the HCOOK‐doped planar n–i–p PSCs reaches 23.8%. After 1000 h of operation at maximum power point tracking under continuous 1 sun illumination, the corresponding encapsulated devices retain 94% of their initial efficiency.

Probing the Origin of Viscosity of Liquid Electrolytes for Lithium Batteries

AbstractViscosity is an extremely important property for ion transport and wettability of electrolytes. Easy access to viscosity values and a deep understanding of this property remain challenging yet critical to evaluating the electrolyte performance and tailoring electrolyte recipes with targeted properties. We proposed a screened overlapping method to efficiently compute the viscosity of lithium battery electrolytes by molecular dynamics simulations. The origin of electrolyte viscosity was further comprehensively probed. The viscosity of solvents exhibits a positive correlation with the binding energy between molecules, indicating viscosity is directly correlated to intermolecular interactions. Salts in electrolytes enlarge the viscosity significantly with increasing concentrations while diluents serve as the viscosity reducer, which is attributed to the varied binding strength from cation–anion and cation–solvent associations. This work develops an accurate and efficient method for computing the electrolyte viscosity and affords deep insight into viscosity at the molecular level, which exhibits the huge potential to accelerate advanced electrolyte design for next‐generation rechargeable batteries.

Loosely bonded dual-functionalized ionic liquid-based phase change solvent for energy-saving CO2 capture

A phase change solvent based on a novel loosely bonded dual-functionalized ionic liquids (ILs) containing diethylenetriamine (DETA) and 1-methylimidazole (1-MI), namely [DETA][1-MI], was developed. The strong anion–cation interactions in an ILs inhibited the CO2–ILs interaction and decrease the absorption capacity of the ILs. The weak interaction of [DETA][1-MI] retained most of the absorption capacity of DETA and 1-MI (up to 2.06 mol CO2/mol ILs). When simulated flue gas was fed into the [DETA][1-MI] + dimethylformamide (DMF) + H2O phase change solvent, the CO2-rich phase had a CO2 concentration of up to 6.51 mol CO2/L and a volume ratio of 42.2%. Moreover, a regeneration efficiency of > 90% was maintained even after three regeneration cycles at 393 K. The corresponding regeneration heat (1.40 GJ/ton CO2) was only 36.8% of 30 wt% monoethanolamine (MEA, 3.80 GJ/ton CO2). To the best of our knowledge, it’s well below the reported regeneration energy of amine-based absorbents. In addition, the corrosion rates of the rich and lean phases were only 0.58% and 0.51% of those of the saturated MEA solution, indicating that the corrosivity of [DETA][1-MI] + DMF + H2O was negligible. Moreover, [1-MI]− was observed to promote the formation of m-DETACOO− and HCO3−/CO32−, further enhancing the CO2 absorption capacity. Therefore, the proposed [DETA][1-MI] + DMF + H2O was verified to be a promising absorbent with favorable absorption properties, a low corrosion rate, high cyclic stability, and superior energy efficiency for CO2 capture.

Authentic Sn═B-Double Bonds in Polar Stannaborene Derivatives.

We report on the synthesis of an authentic Sn═B-moiety realized in a stannaborenyl anion and stannaborenium cation. Starting with an oxidative addition of boron tribromide to a stannylene-phosphine Lewis pair [o-C6H4(Ar*BrSn-BBr2-PPh2)] (2a) [Ar* = C6H3(2,6-Trip)2, Trip = 2,4,6-C6H2iPr3] was synthesized. Reduction of 2a with magnesium yields the Grignard-type stannaborene [o-C6H4(Ar*Sn═B{PPh2}MgBr{thf})]2 (3)2 featuring a Sn═B double bond and a B-Mg interaction. Following an alternative protocol, hydride substitution at 2a yields the tinhydride [o-C6H4(Ar*HSn-BBr2-PPh2)] (4a). HBr elimination of 4a in reaction with MeNHC (MeNHC = 1,3,4,5-tetramethylimidazol-2-ylidene) gives the carbene and phosphine stabilized stannyl-borylene [o-C6H4(Ar*BrSn-B{PPh2}{MeNHC})] (5) after simultaneous bromide transfer from boron to tin. In reaction of 5 with Li[Al(OC{CF3}3)4] or Na[BArF4] in a mixture of o-DFB/benzene a stannaborene [o-C6H4(Ar*Sn═B{PPh2}{MeNHC})]+ [6] stabilized by the respective weakly coordinating anion was isolated (ArF = C6H3-3,5-(CF3)2, o-DFB = o-difluorobenzene). The phosphine and NHC-supported stannaborenium cation 6 adds ammonia at room temperature under splitting of a N-H bond and formation of Sn-NH2 and B-H bonds to give [o-C6H4(Ar*{H2N}Sn-BH{PPh2}{MeNHC})]+ (7).

Controlled crystallization and surface engineering of mixed-halide γ-CsPbI2Br inorganic perovskites via guanidinium iodide additive in air-processed perovskite solar cells

In this report, we demonstrate enlarged grain size (up to ∼3 μm) in ambient-stable black γ-phase CsPbI2Br thin films through the regulated addition of guanidinium iodide (GAI) as an effective volatile additive. Nuclear magnetic resonance (NMR) and X-ray photoelectron spectroscopy (XPS) measurements indicate the complete sublimation of GAI following annealing, with no inclusion inside the final γ-CsPbI2Br perovskite lattice. GAI is found to participate by retarding the cation–anion reaction via the Cs+ and GA+ cation-exchange process. We find that inorganic perovskite solar cells (IPSCs) devices made from (CsPbI2Br)0.925 + 0.075 GAI and a phenyltrimethylammonium chloride (PTACl) passivation retain a solar-friendly band-gap of 1.91 eV and excellent device performance, with the best open-circuit voltage reaching as high as 1.34 V, with highly reproducible and stable photo conversion efficiencies of 16.88% (for 0.09 cm2) and 15.60% (large area 1 cm2) under ambient conditions. Photostability analysis further demonstrated negligible efficiency loss over 1000 h under continuous one-sun equivalent illumination, indicating GAI additive as a promising approach toward ambient stable, all-inorganic high-efficiency solar cells.

Treatment of strong alkaline wastewater from neutral leaching of EAF dust by precipitation and ion exchange

Neutral leaching or water washing is used for Cl− and partially Ca2+ ion removal in order to save the leaching reagents for the next steps in hydrometallurgical treatment of electric arc furnace dust. This pre-treatment of the material leads to the generation of strong alkaline (pH = 11.9–12.7) leachate (wastewater), which underlies precipitation of Ca and other accompanying metals. This work presents results from the study of various economically differing (cost and time) techniques for elimination of these disadvantageous phenomena. The aim of the experimental study was to obtain water suitable for reuse in the leaching or for discharge into a recipient in accordance with valid legislation. The experiments were focused on the removal of precipitates, or metals which create the precipitates, and pH decreasing. Our results indicate that five-minute agitation of 4 g solid NaHCO3 and 1 L of neutral leachate and subsequent ion exchange in the sequence of strong-acid cation and strong-base anion exchange treatment led to the acquisition of water without creation of precipitates, with pH below 8.5 and conductivity approx. 0.03 mS. The removal of Cl− ions was not complete.

Simultaneously Achieved Defect Passivation and Crystallization Modulation by a Multifunctional Pseudohalogen Salt for Efficient and Stable Perovskite Solar Cells

The accumulation of defects and ion migration at the surfaces and grain boundaries of perovskite impedes the improvement of performance and stability in perovskite solar cells. Therefore, developing strategies to reduce trap‐assisted nonradiative recombination and suppress ion migration in perovskite films is urgently needed. Herein, a multifunctional pseudohalogen salt additive, (benzotriazol‐1‐yloxy) dipyrrolidinocarbenium hexafluorophosphate (denoted as BDPF6), composed of a benzotriazole derivative cation and hexafluorophosphate anion, is incorporated into the perovskite precursor solution. The anion vacancies of perovskite films are filled by , whereas the cation and anion in BDPF6 form ionic and coordination bonds with the perovskites. The BDPF6 additive promotes the crystallization of perovskite films with large grain size, reducing defect densities, prolonging carrier lifetimes, and inhibiting ion migration. Thus, the power conversion efficiency (PCE) of the BDPF6‐modified device remarkably improves from 20.36% to 22.68%. The unencapsulated BDPF6‐modified device maintains 97% of its initial PCE after 1,400 h of exposure to an ambient environment with a relative humidity of 10–20%, whereas the control device maintains only 85% of its initial PCE. Similarly, the BDPF6‐modified device maintains 78% of its original PCE after aging at 60 °C for 1,400 h, whereas the control device only maintains 55%.

Resin and loading condition screening for effective and robust byproducts removal by anion exchange chromatography: A case study

In downstream processing of protein therapeutics, ion exchange (IEX) chromatography is a powerful tool for removing byproducts whose isoelectric point (pI) is appreciably different from that of the product. Although in theory for a given case cation exchange (CEX) and anion exchange (AEX) chromatography should be equally effective for separation, in reality they may show different effectiveness. In the current work, with a case study, we demonstrated that AEX is more effective than CEX chromatography at removing the associated byproducts. In addition, we screened AEX resins and loading conditions to achieve best separation. Finally, we demonstrated that effective separation was achieved with the selected resin/condition, and chromatography performance was comparable between runs conducted at low and high load densities, suggesting that the developed process was relatively robust. The procedure described in this work can be used as a general approach for selecting resin and loading condition that allow for effective and robust removal of byproduct that binds weaker than the product to the selected type of column.

4-carboxyanilinium phosphite: A structural, vibrational, thermal and computational study

A new organo- phosphite adduct, 4-carboxyanilinium dihydrogen phosphite (4-CAPI) was synthesized and characterized by single-crystal X-ray diffraction, FTIR and DSC. 4-CAPI crystallises in the Triclinic space group, P-1, Z = 4, with two 4-CA cations and two H2PO3− anions in an asymmetric unit. In 4-CAPI crystal the organic layer containing 4-CA cations and the inorganic layer containing phosphite anions are connected through a three-dimensional network of strong charge-assisted N–H⋯O and C–OH⋯O hydrogen bonds. The cations, 4-CA exists as a cyclic acid dimer. The infrared vibrational frequencies of 4-CAPI were assigned and the spectral features of 4-CAPI obtained suggest presence of a stronger NH⋯O and C–OH⋯O hydrogen bond interactions thus corroborating with the x-ray result. The intermolecular interaction topology of 4-CAPI has been quantitatively analyzed using the computational tool of energy framework analysis, A very high values of interaction energies are found for the hydrogen bonded anion–cation pairs. The major contribution is from electrostatic interaction.

Structural stabilizing action of terbium cation and phosphate anion to layered transition-metal oxide cathodes

The capacity decay and safety issues of layered cathodes caused by structural deterioration upon deeply delithiated state, have impeded the further large-scale commercial-used of layered transition-metal cathodes in advanced lithium-ion batteries. In this work, the terbium cation and phosphate anion are doped homogeneously into LiCoO2 and LiNi0.83Co0.11Mn0.06O2 cathodes via the facile solid phase reaction method. We found that the lattice oxygen can be stabilized by the introduction of the Tb element, leading to the mitigation of structural degradation. More impressively, the PO43− polyanion possesses a benign binding affinity for Li-ions, further accelerating Li-ion transportation. Theoretically, the incorporation of the Tb element into the crystal lattice can alleviate oxygen redox activity in the high delithiation state. Thus, the introduction of an appropriate content of anion and cation dopants synergistically modulates the robust layered structure to suppress structural collapse during cycling. Consequently, the Tb element and PO43− polyanion co-doped LiNi0.83Co0.11Mn0.06O2 (a capacity of 179.3 mAh g−1 after 100 cycles with capacity retention of 96%) and LiCoO2 (169.4 mAh g−1 after 400 cycles and with capacity retention of 95%) illustrate prominent cycling stability. This study proposes a feasible and powerful strategy for enhancing the structural stability and cycling durability of high-voltage LiCoO2 and nickel-rich ternary layered cathode materials.

Unraveling local structures of Salt-in-Water and Water-in-Salt electrolytes via ab initio molecular dynamics

Water-in-salt electrolytes (WiSE) are attractive for electrochemical energy storage applications owing to their wide electrochemical stability windows and inherent safety. The high concentration of salts is widely known to suppress the decomposition of water, which otherwise limits the stability of conventional aqueous salt-in-water electrolytes (SiWE). Nevertheless, the microstructural features of WiSE that lead to this enhanced stability have not yet been fully elucidated. In this work, ab initio molecular dynamics simulations were performed to study the energetic, structural, and spectroscopic properties of LiTFSI SiWE and WiSE solutions. A detailed mapping of water-water and water-anion hydrogen bonding and cation–anion electrostatic interactions is reported for both electrolytes. Structural features are presented in terms of both radial and spatial distribution functions. Analysis of IR and vibrational power spectra reveal key differences in the intermolecular interactions in SiWE and WiSE that arise from modified solvation shell structures. The results obtained herein reveal the most important structural and spectroscopic differences between the electrolytes in normal and superconcentrated concentrations.

Blue Light Irradiated Metal-, Oxidant-, and Base-Free Cross-Dehydrogenative Coupling of C(sp2)-H and N-H Bonds: Amination of Naphthoquinones with Amines.

Herein, we report a blue-light-driven amination of C(sp2)-H bond of naphthoquinones and quinones with the N-H bond of primary and secondary amines for the synthesis of 2-amino-naphthoquinones and 2-amino-quinones. The coupling of naphthoquinones with a wide array of aliphatic, aromatic, chiral, primary, and secondary amines having electron donating (-CH3, -OCH3, -SCH3), withdrawing (-F, -Cl, -Br, -I), and CO2H, -OH, -NH2 groups with acidic protons selectively occurred to afford C-N coupled 2-amino-naphthoquinones in 60-99% yields and hydrogen gas as a byproduct in methanol solvent without using any additional reagents, additives, and oxidant under the blue light irradiation. Mechanistic insight by DFT computation, controlled experiments, kinetic isotopic effect, and substitution effect of the substrates suggest that the reaction proceeds by radical pathway in which naphthoquinone forms a highly oxidizing naphthoquinonyl biradical upon irradiation of blue light (457 nm). Consequently, electron transfer from electron-rich amine to an oxidizing naphthoquinonyl biradical leads to a naphthoquinonyl radical anion and aminyl radical cation, followed by proton transfer and delocalization leading to a carbon-centered naphthoquinonyl radical. The cross-coupling of naphthoquinonyl carbon-centered and aminyl nitrogen radicals forms a C-N bond, with subsequent elimination of hydrogen gas (which was also confirmed by GC-TCD), affording 2-amino-1,4-naphthoquinone under metal-, reagent-, base-, and oxidant-free conditions.

Wetting Behavior and Support Interactions in Imidazolium-Based Supported Ionic Liquid Phase Materials─A Systematic Study by Solid-State Nuclear Magnetic Resonance Spectroscopy

Supported ionic liquid phase (SILP) catalysts are an extremely promising class of materials that combine advantageous concepts from both homogeneous and heterogeneous catalysis. Optimized SILP catalysts should exhibit a thin, homogeneous, and continuous film of the ionic liquid (IL) to avoid pore blocking and to ensure a good accessibility of the catalyst. Yet, the interactions between the IL and the support, which determine the formation of such a film, are still poorly understood. We investigate here in a systematic way the deposition of three imidazolium-based ILs on silica supports with different surface areas and morphologies using 1H magic angle spinning solid-state nuclear magnetic resonance spectroscopy. We demonstrate that the point of complete surface wetting can be determined by the disappearance of the 1H resonance of isolated silanol groups and that this point depends both on the textural properties of the support material and the chemical properties of the IL. 1H chemical shifts also provide valuable insight into hydrogen bonding interactions within the IL and between the IL and the support. They indicate cleavage of the anion–cation hydrogen bonds upon IL deposition and the formation of new hydrogen bonds with the silica surface.

Preparation of paramagnetic ferroferric oxide-calcined layered double hydroxide core–shell adsorbent for selective removal of anionic pollutants

Adsorption is one of the most common methods of pollution treatment. The selectivity for pollutants and recyclability of adsorbents are crucial to reduce the treatment cost. Layered double hydroxide (LDH) materials are one type of adsorbent with poor recyclability. Prussian blue (PB) is a sturdy and inexpensive metal–organic framework material that can be used as the precursor for synthesizing paramagnetic ferroferric oxide (Fe3O4). It is intriguing to build some reusable adsorbents with magnetic separation by integrating LDH and PB. In this work, paramagnetic Fe3O4-calcined LDH (Fe3O4@cLDH) core–shell adsorbent was designed and prepared by the calcination of PB-ZnAl layered double hydroxide (PB@LDH) core–shell precursor, which exhibits high anionic dyes selectivity in wastewater solutions. The paramagnetism and adsorption capability of Fe3O4@cLDH come from the Fe3O4 core and calcined ZnAl-LDH shell, respectively. Fe3O4@cLDH shows an adsorption capacity of 230 mg g−1 for acid orange and a high selectivity for anionic dyes in cation–anion mixed dye solutions. The regeneration process indicates that the high selectivity for anions is related to the specific hydration recovery process of ZnAl-LDH. The synergistic effect of the paramagnetic Fe3O4 core and calcined ZnAl-LDH shell makes Fe3O4@cLDH an excellent magnetic separation adsorbent with high selectivity to anions.

Thermophysical properties and ionic conductivity of new imidazolium-based protic ionic liquids

This research aimed to develop new low-cost proton-conducting electrolytes for fuel cells operating above 100 °C. Thus, two room temperature protic ionic liquids (PILs), imidazolium dibutyl phosphate (IM-DBP) and imidazolium bis(2-ethylhexyl)phosphate) (IM-BEHP) were prepared by neutralization of corresponding dialkyl phosphate with imidazole. The cation–anion ion pairs of the synthesized PILs were optimized within the density functional theory (DFT) approach utilizing the Becke three-parameter exchange–correlation-functional (B3LYP). It was found that hydrogen bonds are formed mainly between the N–H and C2-H hydrogen atoms of the imidazolium cation and the oxygen atoms of the dialkyl phosphate anion. According to thermal characterization, imidazolium dialkyl phosphates have glass transition temperatures around −60 °C and thermal degradation points (i.e. 5% weight loss) of 190 °C (IM-DBP) and 229 °C (IM-BEHP). The rheological studies indicate that the viscosity of IM-BEHP at room temperature is four times higher compared to IM-DBP. A significant decrease in the viscosity was observed for both PILs while increasing the temperature from 22 to 60 °C. The ionic conductivity of PILs was studied by electrochemical impedance spectroscopy in wide frequency (10−1 – 106 Hz) and temperature (25 – 180 °C) ranges. At room temperature, the conductivity of IM-DBP is much higher than that of IM-BEHP (4.5·10−3 S/cm versus 9.3·10−5 S/cm). However, above 140 °C the conductivity of both PILs reached the level of 10−2 S/cm. The activation energy Ea calculated from the slope of the Arrhenius plot of ionic conductivity is 19 kJ/mol for IM-DBP and 39 kJ/mol for IM-BEHP. The relationship between the molar conductivity and the fluidity was described using the Walden rule. The Walden lines for both PILs are close to the “ideal” KCl line that indicates the presence of almost completely dissociated ions. Overall, the obtained results show the availability of imidazolium dialkyl phosphates as proton conducting electrolytes for medium temperature fuel cell applications.

Influence of ionic liquid characteristics on the performance of ternary solid polymer electrolytes with poly(vinylidene fluoride-co-hexafluoropropylene) and zeolite

Solid polymer electrolytes (SPEs) are the necessary step towards solid-state lithium-ion batteries (LIBs). Their function as separator and electrolyte allows to increase the safety of energy storage devices by the elimination of the liquid components. In this work, three-component SPEs based on poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) as host polymer, clinoptilolite zeolite, and different ionic liquids (ILs) (1-ethyl-3-methylimidazolium thiocyanate ([EMIM][SCN]), 1-butyl-3-methylimidazolium thiocyanate ([BMIM][SCN]), 1-ethyl-3-methylimidazolium dicyanamide ([EMIM][NCN2]) and 1-butyl-3-methylimidazolium dicyanamide ([BMIM][NCN2]) were produced and characterized. The influence of the nature of the IL anion and cation on the morphology, degree of crystallinity, mechanical properties, ionic conductivity, and battery cycling performance were studied. It is demonstrated that the [SCN]- anion is the most suitable if SPE applications are envisaged. The ionic conductivity depends on the IL type. At room temperature, a maximum value of 1.3 × 10−5 S cm−1 was obtained for the SPE doped with [BMIM][NCN2]. Regarding battery performance, the best value of discharge capacity was observed for the SPE based on [BMIM][SCN], which for an initial discharge capacity of 135 mAh.g−1 yielded a capacity loss below 30% after 30 cycles at room temperature. Thus, it is concluded that proper selection of the IL (cation chain length and anion size) allows tailoring battery performance of solid-state batteries based on three-component SPEs.

Exploring the thermo-stability and optical characteristics of (Morpholine)2SbCl5 crystal with a non-centrosymmetric structure

Currently combining the transition-metal cation and organic amine anion is a useful strategy to design novel optical materials. In the work, (Morpholine)2SbCl5 with non-centrosymmetric structure has been synthesized by introducing Sb3+ cation with lone-pair electron into heterocyclic amine morpholine, and the single crystals were also obtained by solvent evaporation method. The colorless crystals of (Morpholine)2SbCl5 show the suitable thermal stability up to about 195 °C. In particular, the power SHG response of (Morpholine)2SbCl5 exhibits an intensity of approximately 0.28 × KDP. Further optical properties reveal that the absorption cutoff edge is about 394 nm corresponding to the band gap 3.00 eV, and the PL spectrum display yellow emission at 570 nm. All results indicate that (Morpholine)2SbCl5 is a multifunctional material in the areas of photoluminescence and nonlinear optics.

Chemical separation and measurement of platinum activation products

A method has been developed to purify and measure platinum radioisotopes in the presence of fission products and environmental constituents. The method uses a combination of cation exchange and anion exchange chromatography and selective precipitation steps to remove other radioisotopes from the sample. The addition of stable platinum carrier allows for a gravimetric determination of the chemical yield of the procedure. Overall, the method is fast, simple, and potentially applicable for rapid turnaround of unknown samples. Using this method, multiple platinum radioisotopes were measured in two different irradiation experiments. The measured ratios of the platinum radioisotopes clearly reflect the neutron spectrum of the irradiation, suggesting that platinum radioisotopes could be valuable signatures in nuclear forensic analyses.

Theoretical Study on CO<sub>2</sub>/SO<sub>2</sub> Absorption Using <i>N</i>- Alkylethylenediaminium Protic Ionic Liquid

The protic ionic liquids (PILs) comprising with N-2-ethylhexylethylenediaminium cation (HEtHex+) and bis (trifluoromethanesulfonate) imide anion (TFSA-) forming [HEtHex][TFSA] which has two amines in the polar group and available to absorbs acid gases such as CO2 and SO2. In order to study the CO2/SO2 absorption mechanism of [HEtHex][TFSA], the stable configurations of [HEtHex][TFSA]-nCO2 (n=1, 2, 3, 4) and [HEtHex][TFSA]-nSO2 (n=1, 2, 4, 6) are investigated using the density functional theory at the M06-2X/6-311G (d, p) level, then the interaction energy, molecular vibration frequency, second-order perturbation energy, electron density and Laplace value are calculated and analysed for the most stable configurations. The results show that N–H...O type weak or medium hydrogen bonding are mainly formed between [HEtHex][TFSA] and CO2/SO2 molecules. The hydrogen bonding interaction is stronger for [HEtHex][TFSA]-nSO2 comparing with [HEtHex][TFSA]-nCO2 and increases with increasing the number of CO2/SO2 molecules.

Structural and Dynamic Characterization of Li–Ionic Liquid Electrolyte Solutions for Application in Li-Ion Batteries: A Molecular Dynamics Approach

Pyrrolidinium-based (Pyr) ionic liquids (ILs) have been proposed as electrolyte components in lithium-ion batteries (LiBs), mainly due to their higher electrochemical stability and wider electrochemical window. Since they are not naturally electroactive, in order to allow their use in LiBs, it is necessary to mix the ionic liquids with lithium salts (Li). Li–PF6, Li–BF4, and Li–TFSI are among the lithium salts more frequently used in LiBs, and each anion, namely PF6 (hexafluorophosphate), BF4 (tetrafluoroborate), and TFSI (bis(trifluoromethanesulfonyl)azanide), has its own solvation characteristics and interaction profile with the pyrrolidinium ions. The size of Pyr cations, the anion size and symmetry, and cation–anion combinations influence the Li-ion solvation properties. In this work, we used molecular dynamics calculations to achieve a comprehensive view of the role of each cation–anion combination and of different fractions of lithium in the solutions to assess their relative advantage for Li-ion battery applications, by comparing the solvation and structural properties of the systems. This is the most-comprehensive work so far to consider pyrrolidinium-based ILs with different anions and different amounts of Li: from it, we can systematically determine the role of each constituent and its concentration on the structural and dynamic properties of the electrolyte solutions.