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At least 523 records · Page 29

Can Charge Transfer Across C─H⋅⋅⋅O Hydrogen Bonds Stabilize Oil Droplets in Water?

Oil-water emulsions resist aggregation due to the presence of negative charges at their surface that leads to mutual repulsion between droplets, but the molecular origin of oil charge is currently under debate. Although much evidence has suggested that ionic species must accumulate at the interface, an alternative perspective attributes the negative charge on the oil droplet to charge transfer of electron density from water to oil molecules. Although the charge transfer mechanism is consistent with the correct sign of oil charge, it is just as important to provide good estimates of the charge magnitude to explain emulsion stability and electrophoresis experiments. Here, we show using energy decomposition analysis that the amount of net flow of charge from water to oil is negligibly small due to nearly equal forward and backward charge transfer through weak oil-water interactions, such that oil droplets would be unstable and coalesce, contrary to experiment. The lack of charge transfer also explains why vibrational sum frequency scattering reports a blue shift in the oil C-H frequency when forming emulsions with water, which arises from Pauli repulsion due to localized confinement at the interface. Finally, unlike ions, neither charge transfer nor dynamic polarization can produce a finite conductivity needed to couple to electric fields that would explain electrophoretic mobility.

Zhao, Ruoqi↗

Mechanisms of adhesion degradation at the photovoltiac module's cell metallization-encapsulant interface

Adhesion measurements and chemical characterization of the encapsulant/silver metallization interface of a photovoltaic (PV) module through temperature, humidity, and voltage bias exposures were conducted. Results demonstrate two independent degradation mechanisms: (a) with voltage bias, the ionic conduction of Na + ions through the encapsulant results in the formation of sodium silicate at the silver metallization surface, thereby weakening that interface and (b) with moisture ingress, dissociation of the silane bonding to silver in the silver oxide similarly weakens this interface resulting in significantly lower debond energies.

14 SOLAR ENERGY↗

From classical to quantum dynamics of atomic and ionic species interacting with graphene and its analogue

Graphene and its analogues offer a broad range of application opportunities for (opto)-electronics, sensing, catalysis, phase separation, energy conversion and storage, etc. Engineering graphene properties often relies on its controllable functionalization, defect formation and patterning, and reactive gas etching. In this chapter, we survey the dynamics of graphene using classical and quantum-classical dynamics methods. We discuss the reactivity, scattering, and transmission of atomic and ionic species including Ar cluster ion, H/D, and H+/D+ on graphene flakes of various sizes, focusing on the atomic-scale motion and energy dissipation pathways involved in forming and breaking covalent bonding. Discussions on the nuclear quantum effects of light species, the effects of isotopic substitution, and the methodologies for such modeling are also included.

Garashchuk, Sofiya V.↗

Chemical design of electronic and magnetic energy scales of tetravalent praseodymium materials

Lanthanides in the trivalent oxidation state are typically described using an ionic picture that leads to localized magnetic moments. The hierarchical energy scales associated with trivalent lanthanides produce desirable properties for e.g., molecular magnetism, quantum materials, and quantum transduction. Here, we show that this traditional ionic paradigm breaks down for praseodymium in the tetravalent oxidation state. Synthetic, spectroscopic, and theoretical tools deployed on several solid-state Pr 4+ -oxides uncover the unusual participation of 4f orbitals in bonding and the anomalous hybridization of the 4f 1 configuration with ligand valence electrons, analogous to transition metals. The competition between crystal-field and spin-orbit-coupling interactions fundamentally transforms the spin-orbital magnetism of Pr 4+ , which departs from the J eff = 1/2 limit and resembles that of high-valent actinides. Our results show that Pr 4+ ions are in a class on their own, where the hierarchy of single-ion energy scales can be tailored to explore new correlated phenomena in quantum materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interfacial structure of SrZr x Ti 1-x O 3 films on Ge

The interfacial structure of SrZr x Ti 1-x O 3 films grown on semiconducting Ge substrates is investigated here by synchrotron X-ray diffraction and first-principles density functional theory. By systematically tuning the Zr content x, the effects of bonding at the interface and epitaxial strain on the physical structure of the film can be distinguished. The interfacial perovskite layers are found to be polarized as a result of cation-anion ionic displacements perpendicular to the perovskite/semiconductor interface. We find a correlation between the observed buckling and valence band offsets at the SrZr x Ti 1-x O 3 /Ge interface. The trends in the theoretical valence band offsets as a function of Zr content for the polar structures are in agreement with reported X-ray photoelectron spectroscopy measurements. Finally, these results have important implications for the integration of functional oxide materials with established semiconductor based technologies.

36 MATERIALS SCIENCE↗

New Class of Flow Batteries for Terrestrial and Aerospace Energy Storage Applications

Future sustainable energy generation technologies such as photovoltaic and wind farms require advanced energy storage systems on a massive scale to make the alternate (green) energy options practical. The daunting requirements of such large-scale energy systems such as long operating and cycle life, safety, and low cost are not adequately met by state-of-the-art energy storage technologies such as vanadium flow cells, lead-acid, and zinc-bromine batteries. Much attention is being paid to redox batteries specifically to the vanadium redox battery (VRB) due to their simplicity, low cost, and good life characteristics compared to other related battery technologies. NASA is currently seeking high-specific- energy and long-cycle-life rechargeable batteries in the 10-to-100-kW range to support future human exploration missions, such as planetary habitats, human rovers, etc. The flow batteries described above are excellent candidates for these applications, as well as other applications that propose to use regenerative fuel cells. A new flow cell technology is proposed based on coupling two novel electrodes in the form of solvated electron systems (SES) between an alkali (or alkaline earth) metal and poly aromatic hydrocarbons (PAH), separated by an ionically conducting separator. The cell reaction involves the formation of such SES with a PAH of high voltage in the cathode, while the alkali (or alkaline earth metal) is reduced from such an MPAH complex in the anode half-cell. During recharge, the reactions are reversed in both electrodes. In other words, the alkali (alkaline earth) metal ion simply shuttles from one M-PAH complex (SES) to another, which are separated by a metal-ion conducting solid or polymer electrolyte separator. As an example, the concept was demonstrated with Li-naphthalene//Li DDQ (DDQ is 2,3-Dichloro-5,6-dicyano- 1,4-benzoquinone) separated by lithium super ion conductor, either ceramic or polymer (solid polymer or gel polymer) electrolytes. The reactants are Li-naphthalene dissolved in tetrahydrofuran (THF) with a lithium salt of 1M LiBF4 (lithium tetra fluoroborate) in the anode compartment, and DDQ again dissolved in THF and also containing 1M LiBF4 salt in the cathode half-cell. The solid electrolyte separator used in the first set of experiments is a ceramic solid electrolyte, available from a commercial source. The open circuit voltage of the cells is close to 3.0 V, as expected from the individual half-cell voltages of Li-naphthalene and Li-DDQ. Upon discharge, the cell shows steady discharge voltage of 2.7 V, which confirms that the electrochemical processes do involve lithium ion shuttling from the anodic compartment to the cathode half-cell. The reversibility or rechargeability is demonstrated by charging the partially discharged cells (i.e., with lithium present in the DDQ half). Once again, a steady voltage close to 3.0 V was observed during charge, indicating that the system is quite reversible. In the subsequent concept-demonstration studies, the ceramic electrolyte has been replaced with a gel polymer electrolyte, e.g., PVDF-HFP (poly vinylene difluoride hexafluoropropene) gel, which has several advantages such as high ionic conductivity (almost comparable to liquid electrolyte and about 2 orders of magnitude better than the ceramic equivalent), lower cost, and possibly higher chemical stability at the anode. In addition, it can be bonded to the electrode by thermal fusion to form membrane electrode assemblies (MEAs), as is done in fuel cells.

Bugga, Ratnakumar V.↗

Development of Ultrafiltration Membrane-Separation Technology for Energy-Efficient Water Treatment and Desalination Process

The growing scarcity of fresh water is a major political and economic challenge in the 21st century. Compared to thermal-based distillation technique of water production, pressure driven membrane-based water purification process, such as ultrafiltration (UF), nanofiltration (NF) and reverse osmosis (RO), can offer more energy-efficient and environmentally friendly solution to clean water production. Potential applications also include removal of hazardous chemicals (i.e., arsenic, pesticides, organics) from water. Although those membrane-separation technologies have been used to produce drinking water from seawater (desalination) and non-traditional water (i.e., municipal wastewater and brackish groundwater) over the last decades, they still have problems in order to be applied in large-scale operations. Currently, a major huddle of membrane-based water purification technology for large-scale commercialization is membrane fouling and its resulting increases in pressure and energy cost of filtration process. Membrane cleaning methods, which can restore the membrane properties to some degree, usually cause irreversible damage to the membranes. Considering that electricity for creating of pressure constitutes a majority of cost (~50%) in membrane-based water purification process, the development of new nano-porous membranes that are more resistant to degradation and less subject to fouling is highly desired. Styrene-ethylene/butylene-styrene (SEBS) block copolymer is one of the best known block copolymers that induces well defined morphologies. Due to the polarity difference of aromatic styrene unit and saturated ethylene/butylene unit, these two polymer chains self-assemble each other and form different phase-separated morphologies depending on the ratios of two polymer chain lengths. Because the surface of SEBS is hydrophobic which easily causes fouling of membrane, incorporation of ionic group (e,g, sulfonate) to the polymer is necessary to reduces fouling. Recently, sulfonated SEBS became commercially available and has been extensively explored for membrane-mediated water purification technology. The sulfonated block copolymer creates a well developed nano-sale phase-separated morphologies composed of hydrophilic domains (sulfonated polystyrene) and hydrophobic domains (polyethylene/polybutylene). The hydrophilic domains determines transport properties (water transport, salt and/or ion rejection, etc) and the hydrophobic domains provides mechanical stability of the membrane. Unfortunately, a high degree of sulfonation of SEBS induces excessive swelling and deterioration of mechanical stability of the membrane. In an effort to develop robust polymeric membrane materials for water purification technology, phosphonic acid-functionalized SEBS membranes are investigated during this report period. In compare to sulfonated polymers, the corresponding phosphonated polymers are known to swell less because of the formation of extensive hydrogen bonding networks between phosphonates. In addition to the expected better mechanical stability, phosphonated polymers has another advantage over sulfonated polymers for the use water purification membrane; each phosphonate can accommodate two ions while each sulfonate accommodates only one ion. Membrane properties (ion type, ionic density, etc) of new membranes will be studied and their separation performance will be evaluated in water purification and desalination process. Through systematic study of the relationship of chemical structure–surface property–membrane performance, we aim to better understand the nature of membrane fouling and develop more fouling-resistant water purification membranes. The basic understanding of this relationship will lead to the development of advanced membrane materials which can offer a solution to environmentally sustainable production of fresh water.

36 MATERIALS SCIENCE↗

Energetic and Electronic Properties of AcX and LaX (X = O and F)

The bonding and spectroscopic properties of LaX and AcX (X = O and F) diatomic molecules were studied by highlevel ab initio CCSD(T) and SO-CASPT2 electronic structure calculations. Bond dissociation energies (BDEs) were calculated at the Feller−Peterson−Dixon (FPD) level. Potential energy curves and spectroscopic constants for the lowest-lying spin−orbit Ω states were obtained at the SO-CASPT2/aQ-DK level. A dense manifold of excited states was described for the monofluorides with the ground states well separated from the excited states. The spectroscopic parameters were in good agreement with those reported experimentally for LaO and LaF. For the diatomic molecules containing actinides, no experimental data of these parameters was found, but the results were consistent with other high-level calculations. The BDEs calculated at the FPD level were 791.3 (LaO), 705.2 (AcO), 650.0 (LaF), and 678.6 (AcF) kJ/ mol. The NBO analysis showed that the monofluorides are essentially ionic, which explains why the BDE(AcF) is higher than BDE(LaF); for the monoxides, covalent contributions involving the d orbitals of the metal and the p orbitals of the oxygen are stronger for LaO than AcO, which explains the higher BDE for LaO. Finally, the bond orders are predicted to be 2 for LaF and AcF, 3 for AcO, and higher than 3 for LaO.

Basis sets↗

Thermodynamic Water Activity Explains the Unusual Electrochemical Stability of Aqueous Deep Eutectic Solvents

The presence of water in nonaqueous deep eutectic solvent (DES) electrolytes has been debated in recent years, with efforts ranging from its complete removal to willful addition. It was shown that controlled amounts of water can be beneficial, as it not only enhances the physicochemical properties of these electrolytes but also has no significant detrimental effects on their electrochemical stability. Despite these advantages, there is still limited understanding of how water interacts with DES systems at the molecular level. This study examines the water activity in ethylene glycol and glycerol, as well as their binary mixtures with choline chloride to form the DESs ethaline and glyceline, respectively. In this work, we show that the high electrochemical stability of glyceline is related to its lower water activity compared to ethaline and can be attributed to the robust H-bonding network formed by the three hydroxyl groups of glycerol. Its 3D H-bond network effectively integrates water molecules within its solvent structure, reducing degradation and maintaining stability at higher water contents. The deviations from the ideal Raoult's law behavior are reflected in the water activity and activity coefficients, which highlight the intricate H-bond interactions within DES-water mixtures. Water acts like a lubricant within the more viscous DES mixtures without being detrimental to their electrochemical performance. The presented results emphasize the necessity of customizing DES-water compositions to enhance their performance as electrolytes, especially in flow battery applications where electrochemical stability, ionic conductivity, and fluidity are of utmost importance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Structural Effects on Solubility and Crystallinity in Polyamide Ionomers

Although polyamides have been an industrial staple for decades, their solubility and processability remain limited due to the strong hydrogen bonding between amide groups. Here, we report a family of polyamides in which aryl rings, alkyl spacers, sulfonate groups, and amide linkages are regularly spaced along the polymer backbone, allowing us to probe the structural elements that affect processability. We accessed these polymers through a synthetic route based on an expanded diamine monomer and characterized them through a range of physical and spectroscopic techniques. Our results show that the combination of sulfonate groups with increased amide content results in highly soluble polymers, which can dissolve in polar solvents such as water, methanol, and N,N-dimethylformamide. Infrared spectroscopy on the solid polymers shows that the aliphatic amides engage in hydrogen bonding with the sulfonate groups, thus inhibiting ion aggregation, crystallization, and microphase separation. These findings expand the avenue to sulfonate-containing polyamide chemistry and provide design rules for the synthesis of more processable ionic polyamides.

amides↗

Ion–Molecule Complex Dissociation and Formation Dynamics in LiCl Aqueous Solutions from 2D IR Spectroscopy

Ion–molecule complex dynamics as well as water dynamics in concentrated lithium chloride (LiCl) solutions are examined using ultrafast two-dimensional infrared (2D IR) spectroscopy with the CN stretching mode of methyl thiocyanate (MeSCN) as the vibrational probe. In pure water, MeSCN has a narrow symmetric absorption line shape. 2D IR spectral diffusion measurements of the CN stretch give the identical time dependence of water dynamics, as previously observed using the OD stretch of HOD in H 2 O. In concentrated LiCl solutions, the IR absorption spectrum of MeSCN displays two distinct peaks, one corresponding to water H-bonded to the N lone pair of MeSCN (W) and the other corresponding to Li + associated with the N (L). These two species are in equilibrium, and switching of the CN bonding partner from Li + to H 2 O and vice versa was observed and explicated with 2D IR chemical exchange spectroscopy. The MeSCN·Li + complex dissociation time constant, τ LW , and the MeSCN·H 2 O dissociation time constant, τ WL , were determined. The observed τ LW chemical exchange dissociation time constant changes from 60 to 40 ps as the LiCl concentration decreases from ~10.7 to ~7.7 M, mainly due to the increase of the water concentration as the LiCl concentration is reduced. The observed time constants are independent of the model for the chemical reaction. With the assumption of a simple chemical equation, MeSCN·Li + + H 2 O ⇌ MeSCN·H 2 O + Li + , the equilibrium equation rate constants were obtained from the observed chemical exchange time constants. It was determined that the equilibrium rate constants barely change even though the viscosity changes by a factor of 2 and the ionic strength changes by a factor of 1.4. Extrapolation to dilute LiCl solution estimates the τ LW to be ~30 ps. The orientational relaxation (anisotropy decay) of both the W and L complexes was measured using polarization selective 2D IR experiments. The lithium-bonded species undergoes orientational relaxation ~3 times slower than the water-bonded species in each LiCl solution studied. In conclusion, the difference demonstrates the distinct interactions with the medium experienced by the neutral and charged species in the concentrated salt solutions.

14 SOLAR ENERGY↗

Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries

The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li ion batteries. Several lithium chloride SEs, Li 3 MCl 6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and good chemical stability. This study systematically investigated 17 Li 3 MCl 6 SEs to identify novel and promising lithium chloride SEs. Calculation results revealed that 12 Li 3 MCl 6 (M = Bi, Dy, Er, Ho, In, Lu, Sc, Sm, Tb, TI, Tm, and Y) were stable phase with a wide electrochemical stability window and excellent chemical stability against cathode materials and moisture. Li-ion transport properties were examined using bond valence site energy (BVSE) and ab initio molecular dynamics (AIMD) calculation. Li 3 MCl 6 showed the lower migration energy barrier in monoclinic structures, while orthorhombic and trigonal structures exhibited higher energy barriers due to the sluggish diffusion along the two-dimensional path based on the BVSE model. AIMD results confirmed the slower ion migration along the 2D path, exhibiting lower ionic diffusivity and higher activation energy in orthorhombic and trigonal structures. For the further increase of ionic conductivity in monoclinic structures, Li-ion vacancy was formed by the substitution of M 3+ with Zr 4+ . Zr-substituted phase (Li 2.5 M 0.5 Zr 0.5 Cl 6 , M = In, Sc) exhibited up to a fourfold increase in ionic conductivity. This finding suggested that the optimization of Li vacancy in the Li 3 MCl 6 SEs could lead to superionic Li 3 MCl 6 SEs.

25 ENERGY STORAGE↗

Solvation Thermodynamics of Solutes in Water and Ionic Liquids Using the Multiscale Solvation-Layer Interface Condition Continuum Model

We report molecular assembly processes are generally driven by thermodynamic properties in solutions. Atomistic modeling can be very helpful in designing and understanding complex systems, except that bulk solvent is very inefficient to treat explicitly as discrete molecules. The SLIC/CDC multiscale model combines continuum solvent electrostatics based on the solvent layer interface condition (SLIC) with statistical thermodynamic models for hydrogen bonding and nonpolar modes: cavity formation, dispersion interactions, combinatorial mixing (CDC). The SLIC/CDC model predicts Gibbs energies of solvation for a database of 500 solutes in water with average accuracy better than 1 kcal/mol both for experimental measurements and for explicit-solvent molecular dynamics simulations. The separate SLIC/CDC energy mode values agree quantitatively with those computed from explicit-solvent molecular dynamics. The SLIC/SASA multiscale model combines the SLIC continuum electrostatic model with the solvent accessible surface area (SASA) nonpolar energy mode. The SLIC/SASA model predicts Gibbs energies of solvation with better than 1.4 kcal/mol average accuracy in aqueous systems and better than 1.6 kcal/mol average accuracy in ionic liquids. Both models predict solvation entropies, and are the first implicit-solvation models capable of predicting solvation heat capacities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Role of composition, bond covalency, and short-range order in the disordering of stannate pyrochlores by swift heavy ion irradiation

A 2 Sn 2 O 7 (A = Nd, SM, Gd, Er, Yb, and Y) materials with the pyrochlore structure were irradiated with 2.2 GeV Au ions to systematically investigate disordering of this system in response to dense electronic excitation. Structural modifications were characterized, over multiple length scales, by transmission electron microscopy, x-ray diffraction, and Raman spectroscopy. Transformations to amorphous and disordered phases were observed, with disordering dominating the structural response of materials with small A -site cation ionic radii. Both the disordered and amorphous phases were found to possess weberite-type local ordering, differing only in that the disordered phase exhibits a long-range, modulated arrangement of weberite-type structural units into an average defect-fluorite structure, while the amorphous phase remains fully aperiodic. Comparison with the behavior of titanate and zirconate pyrochlores showed minimal influence of the high covalency of the Sn-O bond on this phase behavior. Finally, an analytical model of damage accumulation was developed to account for simultaneous amorphization and recrystallization of the disordered phase during irradiation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Exploring low-temperature dehydrogenation at ionic Cu sites in beta zeolite to enable alkane recycle in dimethyl ether homologation

Cu-based catalysts containing targeted functionalities including metallic Cu, oxidized Cu, ionic Cu, and Bronsted acid sites were synthesized and evaluated for isobutane dehydrogenation. Hydrogen productivities, combined with operando X-ray absorption spectroscopy, indicated that Cu(I) sites in Cu/BEA catalysts activate C-H bonds in isobutane. Computational analysis revealed that isobutane dehydrogenation at a Cu(I) site proceeds through a two-step mechanism with a maximum energy barrier of 159 kJ/mol. Furthermore, these results demonstrate that light alkanes can be reactivated on Cu/BEA, which may enable re-entry of these species into the chain-growth cycle of dimethyl ether homologation, thereby increasing gasoline-range (C 5+ ) hydrocarbon yield.

09 BIOMASS FUELS↗

A dual cryogenic ion trap spectrometer for the formation and characterization of solvated ionic clusters

A new experimental approach is presented in which two separate cryogenic ion traps are used to reproducibly form weakly bound solvent clusters around electrosprayed ions and messenger-tag them for single-photon infrared photodissociation spectroscopy. This approach thus enables the vibrational characterization of ionic clusters comprised of a solvent network around large and non-volatile ions. We demonstrate the capabilities of the instrument by clustering water, methanol, and acetone around a protonated glycylglycine peptide. For water, cluster sizes with greater than twenty solvent molecules around a single ion are readily formed. We further demonstrate that similar water clusters can be formed around ions having a shielded charge center or those that do not readily form hydrogen bonds. Finally, infrared photodissociation spectra of D{sub 2}-tagged GlyGlyH{sup +} ⋅ (H{sub 2}O){sub 1−4} are presented. They display well-resolved spectral features and comparisons with calculations reveal detailed information on the solvation structures of this prototypical peptide.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Pauling’s rules for oxide-based minerals: A re-examination based on quantum mechanical constraints and modern applications of bond-valence theory to Earth materials

Since their introduction in 1929, Pauling’s five rules have been used by scientists from many disciplines to rationalize and predict stable arrangements of atoms and coordination polyhedra in crystalline solids; amorphous materials such as silicate glasses and melts; nanomaterials, poorly crystalline solids; aqueous cation and anion complexes; and sorption complexes at mineral-aqueous solution interfaces. The predictive power of these simple yet powerful rules was challenged recently by George et al. (2020), who performed a statistical analysis of the performance of Pauling’s five rules for about 5000 oxide crystal structures. They concluded that only 13% of the oxides satisfy the last four rules simultaneously and that the second rule has the most exceptions. They also found that Pauling’s first rule is satisfied for only 66% of the coordination environments tested and concluded that no simple rule linking ionic radius to coordination environment will be predictive due to the variable quality of univalent radii. We address these concerns and discuss quantum mechanical calculations that complement Pauling’s rules, particularly his first (radius sum and radius ratio rule) and second (electrostatic valence rule) rules. We also present a more realistic view of the bonded radii of atoms, derived by determining the local minimum in the electron density distribution measured along trajectories between bonded atoms known as bond paths, i.e., the bond critical point (rc). Electron density at the bond critical point is a quantum mechanical observable that correlates well with Pauling bond strength. Moreover, a metal atom in a polyhedron has as many bonded radii as it has bonded interactions, resulting in metal and O atoms that may not be spherical. O atoms, for example, are not spherical in many oxide-based crystal structures. Instead, the electron density of a bonded oxygen is often highly distorted or polarized, with its bonded radius decreasing systematically from ~1.38 Å when bonded to highly electropositive atoms like sodium to 0.64 Å when bonded to highly electronegative atoms like nitrogen. Bonded radii determined for metal atoms match the Shannon (1976) radii for more electropositive atoms, but the match decreases systematically as the electronegativities of the M atoms increase. As a result, significant departures from the radius ratio rule in the analysis by George et al. (2020) is not surprising. We offer a modified, more fundamental version of Pauling’s first rule and demonstrate that the second rule has a one-to-one connection between the electron density accumulated between the bonded atoms at the bond critical point and the Pauling bond strength of the bonded interaction. Pauling’s second rule implicitly assumes that bond strength is invariant with bond length for a given pair of bonded atoms. Many studies have since shown that this is not the case, and Brown and Shannon (1973) developed an equation and a set of parameters to describe the relation between bond length and bond strength, now redefined as bond valence to avoid confusion with Pauling bond-strength. Brown (1980) used the valence-sum rule, together with the path rule and the valence-matching principle, as the three axioms of bond-valence theory (BVT), a powerful method for understanding many otherwise elusive aspects of crystals and also their participation in dynamic processes. We show how a priori bond-valence calculations can predict unstrained bond-lengths and how bond-valence mapping can locate low-Z atoms in a crystal structure (e.g., Li) or examine possible diffusion pathways for atoms through crystal structures. In addition, we briefly discuss Pauling’s third, fourth, and fifth rules, the first two of which concern the sharing of polyhedron elements (edges and faces) and the common instability associated with structures in which a polyhedron shares an edge or face with another polyhedron and contains high-valence cations. The olivine [α-(MgxFe1–x)2SiO4] crystal structure is used to illustrate the distortions from hexagonal close-packing of O atoms caused by metal-metal repulsion across shared polyhedron edges. We conclude by discussing several applications of BVT to Earth materials, including the use of BVT to: (1) locate H+ ions in crystal structures, including the location of protons in the crystal structures of nominally anhydrous minerals in Earth’s mantle; (2) determine how strongly bonded (usually anionic) structural units interact with weakly bonded (usually cationic) interstitial complexes in complex uranyl-oxide and uranyl-oxysalt minerals using the valence-matching principle; (3) calculate Lewis acid strengths of cations and Lewis base strengths of anions; (4) determine how (H2O) groups can function as bond-valence transformers by dividing one bond into two bonds of half the bond valence; (5) help characterize products of sorption reactions of aqueous cations (e.g., Co2+ and Pb2+) and oxyanions [e.g., selenate (Se6+O4)2- and selenite (Se4+O3)2-] at mineral-aqueous solution interfaces and the important role of protons in these reactions; and (6) help characterize the local coordination environments of highly charged cations (e.g., Zr4+, Ti4+, U4+, U5+, and U6+) in silicate glasses and melts.

Geochemistry & Geophysics↗

Design of Sodium Chalcohalide Solid Electrolytes with Mixed Anions for All‐Solid‐State Sodium‐Ion Batteries

Solid-state sodium-ion batteries (SSNIBs) have emerged as a promising alternative to lithium-ion systems for grid-scale energy storage, owing to sodium's abundance and the improved safety of solid-state designs. Among various solid-state electrolytes (SSEs), halide-based Na + SSEs offer high electrochemical stability but are limited by low ionic conductivity and poor thermal stability. Herein, a novel class of sodium hafnium chalcohalide SSEs is reported with a dual-anion (S 2− /Cl − ) framework, with a high ionic conductivity of 4.5 × 10 −4 S cm −1 . The incorporation of sulfur enhances Na⁺ mobility by reducing the migration barrier through increased anion polarizability and expanded diffusion pathways. Additionally, S 2− contributes to stronger interatomic bonding, leading to higher cohesive energy density, improved thermal stability, and mechanical robustness. These SSEs exhibit minimal sulfur oxidation and excellent chemical/electrochemical interface stability with different cathode materials, such as O3-layered NaNi 1/3 Fe 1/3 Mn 1/3 O 2 , P2/O3 layered Na 0.85 Mn 0.5 Ni 0.4 Fe 0.1 O 2 , and Na 3 V 2 (PO 4 ) 3 cathodes. As a result, SSNIBs with P2/O3 layered Na 0.85 Mn 0.5 Ni 0.4 Fe 0.1 O 2 employing the sodium hafnium chalcohalide SSEs demonstrate outstanding cycling performance, achieving a capacity retention of 88.5% after 200 cycles at 0.1 C. This study establishes a new design strategy for high-performance SSEs, demonstrating that mixed-anion frameworks offer a viable route to overcome the intrinsic limitations of single-anion electrolytes in next-generation SSNIBs.

DFT calculation↗