Cathode degradation is a key factor that limits the lifetime of Li-ion batteries. To identify functional coatings that can suppress this degradation, we present a high-throughput density functional theory based framework which consists of reaction models that describe thermodynamic and electrochemical stabilities, and acid-scavenging capabilities of materials. Screening more than 130,000 oxygen-bearing materials, we suggest physical and hydrofluoric-acid barrier coatings such as WO3, LiAl5O8 and ZrP2O7 and hydrofluoric-acid scavengers such as Sc2O3, Li2CaGeO4, LiBO2, Li3NbO4, Mg3(BO3)2 and Li2MgSiO4. Using a design strategy to find the thermodynamically optimal coatings for a cathode, we further present optimal hydrofluoric-acid scavengers such as Li2SrSiO4, Li2CaSiO4 and CaIn2O4 for the layered LiCoO2, and Li2GeO3, Li4NiTeO6 and Li2MnO3 for the spinel LiMn2O4 cathodes. These coating materials have the potential to prolong the cycle-life of Li-ion batteries and surpass the performance of common coatings based on conventional materials such as Al2O3, ZnO, MgO or ZrO2.

A series of nonanuclear lanthanide oxo-hydroxo complexes of the general formula [Ln(9)(mu(4)-O)(2)(mu(3)-OH)(8)(mu-BA)(8)(BA)(8)](-)[HN(CH(2)CH(3))(3)](+).(CH(3)OH)(2)(CHCl(3)) (BA = benzoylacetone; Ln = Sm, 1; Eu, 2; Gd, 3; Dy, 4; Er, 5) were prepared by the reaction of hydrous lanthanide trichlorides with benzoylacetone in the presence of triethylamine in methanol and recrystallized from chloroform/methanol (1:10) at room temperature. These five compounds are isomorphous. Crystal data for 1: cubic, Pn3n; T = 180 K; a = 33.8652(4) A; V = 38838.4(8) A(3); Z = 6; D(calcd) = 1.125 g cm(-)(3); R1 = 3.37%. Crystal data for 2: cubic, Pn3n; T = 180 K; a = 33.8252(8) A; V = 38700.9(16) A(3); Z = 6; D(calcd) = 1.133 g cm(-)(3); R1 = 4.97%. Crystal data for 3: cubic, Pn3n; T = 180 K; a = 33.7061(6) A; V = 38293.5(12) A(3); Z = 6; D(calcd) = 1.157 g cm(-)(3); R1 = 5.13%. Crystal data for 4: cubic, Pn3n; T = 180 K; a = 33.5900(7) A; V = 37899.2(14) A(3); Z = 6; D(calcd) = 1.182 g cm(-)(3); R1 = 4.03%. Crystal data for 5: cubic, Pn3n; T = 180 K; a = 33.5054(8) A; V = 37613.6(16) A(3); Z = 6; D(calcd) = 1.202 g cm(-)(3); R1 = 4.86%. The core of the anionic cluster comprises two vertex-sharing square-pyramidal [Ln(5)(mu(4)-O)(mu(3)-OH)(4)](9+) units. The compounds were characterized by elemental analysis, IR, fast atom bombardment mass spectra, thermogravimetry, and differential scanning calorimetry. The thermal analysis indicated that the nonanuclear species were stable up to 150 degrees C. Luminescence spectra of 2 and magnetic properties of 1-5 were also studied.

Material design of new Li-rich Li2(MI,MII)O3 layered oxides for high-energy-density lithium-ion batteries via multi-faceted high-throughput density function theory calculations.

Materials with synchronous capabilities of color change and actuation have prospects for application in biomimetic dual-stealth camouflage and artificial intelligence. However, color/shape dual-responsive devices involve stimuli that are difficult to control such as gas, light or magnetism, and the devices show poor coordination. Here, a flexible composite film with electrochromic/actuating (238° bending angle) dual-responsive phenomena, excellent reversibility, high synchronization, and fast response speed (< 5 s) utilizes a single active component, W18O49 nanowires. From in situ synchrotron X-ray diffraction, first principles calculations/numerical simulations, and a series of control experiments, the actuating mechanism for macroscopic deformation is elucidated as pseudocapacitance-based reversible lattice contraction/recovery of W18O49 nanowires (i.e. nanostructure change at the atomic level) during lithium ion intercalation/de-intercalation. In addition, we demonstrate the W18O49 nanowires in a solid-state ionic polymer-metal composite actuator that operates stably in air with a significant pseudocapacitive actuation.

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Embedding a lithiated cobalt oxide spinel (LiCoO, or LiCoO) component or a nickel-substituted LiCoNi O analogue in structurally integrated cathodes such as xLiMnO·(1- x)LiM'O (M' = Ni/Co/Mn) has been recently proposed as an approach to advance the performance of lithium-ion batteries. Here, we first revisit the phase stability and electrochemical performance of LiCoO synthesized at different temperatures using density functional theory calculations. Consistent with previous studies, we find that the occurrence of low- and high-temperature structures (i.e., cubic lithiated spinel LT-LiCoO; or LiCoO ( Fd3̅ m) vs trigonal-layered HT-LiCoO ( R3̅ m), respectively) can be explained by a small difference in the free energy between these two compounds. Additionally, the observed voltage profile of a Li/LiCoO cell for both cubic and trigonal phases of LiCoO, as well as the migration barrier for lithium diffusion from an octahedral (O) site to a tetrahedral site (T) in Fd3̅ m LT-LiCoO, has been calculated to help understand the complex electrochemical charge/discharge processes. A search of LiCo MO lithiated spinel (M = Ni or Mn) structures and compositions is conducted to extend the exploration of the chemical space of Li-Co-Mn-Ni-O electrode materials. We predict a new lithiated spinel material, LiNiCoO ( Fd3̅ m), with a composition close to that of commercial, layered LiNiCoAlO, which may have the potential for exploitation in structurally integrated, layered spinel cathodes for next-generation lithium-ion batteries.

Article impact statement: Conservation triage is not necessary for species conservation. Adequate resources exist; even species with small populations can recover.

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