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At least 343 records · Page 19

Synthesis of new two-dimensional titanium carbonitride Ti 2 C 0.5 N 0.5 T x MXene and its performance as an electrode material for sodium-ion battery

Two-dimensional (2D) layered transition metal carbides/nitrides, called MXenes, are attractive alternative electrode materials for electrochemical energy storage. Owing to their metallic electrical conductivity and low ion diffusion barrier, MXenes are promising anode materials for sodium-ion batteries (SIBs). Herein, we report on a new 2D carbonitride MXene, viz ., Ti 2 C 0.5 N 0.5 T x (T x stands for surface terminations), and the only second carbonitride after Ti 3 CNT x so far. A new type of in situ HF (HCl/KF) etching condition was employed to synthesize multilayer Ti 2 C 0.5 N 0.5 T x powders from Ti 2 AlC 0.5 N 0.5 . Spontaneous intercalation of tetramethylammonium followed by sonication in water allowed for large-scale delamination of this new titanium carbonitride into 2D sheets. Multilayer Ti 2 C 0.5 N 0.5 T x powders showed higher specific capacities and larger electroactive surface area than those of Ti 2 CT x powders. Multilayer Ti 2 C 0.5 N 0.5 T x powders show a specific capacity of 182 mAh g -1 at 20 mA g -1 , the highest among all reported MXene electrodes as SIBs with excellent cycling stability.

25 ENERGY STORAGE↗

Spatially-resolved lithiation dynamics from operando X-ray diffraction and electrochemical modeling of lithium-ion cells

In this study, energy dispersive X-ray diffraction is used to profile the time evolution of ordered Li x C 6 phases in solid electrodes of lithium-ion cells charged at rates between 0.2 and 4.7C (where 1C corresponds to full discharge in 1 h). The methods for quantifying lithium concentration in these phases from the acquired diffraction patterns are described. Compact expressions for time-dependent concentration gradients in the solid electrodes using orthogonal polynomial expansions are presented. Experimentally, these gradients persisted in lithiated graphite electrodes even after the cells rested at open-circuit for over 9 h. A multiphase electrochemical model of graphite intercalation captured many of the observed behaviors, including the progression of phase transitions and the persistent gradients at zero current. However, the magnitude of concentration gradients in both the oxide cathode and graphite anode is underestimated by the model, even at moderate currents.

25 ENERGY STORAGE↗

Metal Sulfide Ion Exchangers: High Acid Stability of Na 2 x Mg 2 y – x Sn 4– y S 8 (NMS) and Topotactic Conversion to 2D Solid Acids with Semiconducting Character

Metal sulfide ion exchange materials (MSIEs) are of interest for nuclear waste remediation applications. Here, we report the high stability of two structurally related metal sulfide ion exchange materials, Na 2x Mg 2y–x Sn 4–y S 8 (Mg-NMS) and Na 2 SnS 3 (Na-NMS), in strongly acid media, in addition to the preparation of Na 2x Ni 2y–x Sn 4–y S 8 (Ni-NMS). Their formation progress during synthesis is studied with in-situ methods, with the target phases appearing in <15 min, reaction completion in <12 h, and high yields (75–80%). Upon contact with nitric or hydrochloric acid, these materials topotactically exchange Na + for H + , proceeding in a stepwise protonation pathway for Na 5.33 Sn 2.67 S 8 . Na-NMS is stable in 2 M HNO 3 and Mg-NMS is stable in 4 M HNO 3 for up to 4 h, while both NMS materials are stable in 6 M HCl for up to 4 days. However, the treatment of Mg-NMS and Na-NMS with 2–6 M H 2 SO 4 reveals a much slower protonation process since after 4 h of contact both NMS and HMS are present in the solution. The resultant protonated materials, H 2x Mg 2y–x Sn 4–y S 8 and H 4x [(H y Na y–1 ) 1.33x Sn 4––1.33x ]S 8 , are themselves solid acids and readily react with and intercalate a variety of organic amines, where the band gap of the resultant adduct is influenced by amine choice and can be tuned within the range of 1.88(5)–2.27(5) eV. The work function energy values for all materials were extracted from photoemission yield spectroscopy in air (PYSA) measurements and range from 5.47 (2) to 5.76 (2) eV, and the relative band alignments of the materials are discussed. DFT calculations suggest that the electronic structure of Na 2 MgSn 3 S 8 and H 2 MgSn 3 S 8 makes them indirect gap semiconductors with multi-valley band edges, with carriers confined to the [MgSn 3 S 8 ] 2– layers. Light electron effective masses indicate high electron mobilities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spontaneous Strain Buffer Enables Superior Cycling Stability in Single-Crystal Nickel-Rich NCM Cathode

The capacity degredation in layered Ni-rich LiNixCoyMnzO2 (x >= 0.8) cathode largely originated from drastic surface reactions and intergranular cracks in polycrystalline particles. Herein, we report a highly stable single- crystal LiNi0.83Co0.12Mn0.05O2 cathode material, which can deliver a high specific capacity (similar to 209 mAh g(-1) at 0.1 C, 2.8-4.3 V) and meanwhile display excellent cycling stability (>96% retention for 100 cycles and >93% for 200 cycles). By a combination of in situ X-ray diffraction and in situ pair distribution function analysis, an intermediate monoclinic distortion and irregular H3 stack are revealed in the single crystals upon charging-discharging processes. These structural changes might be driven by unique Li-intercalation kinetics in single crystals, which enables an additional strain buffer to reduce the cracks and thereby ensure the high cycling stability.

in situ synchrotron characterization↗

A review of transport models in charged porous electrodes

There is increased interest in many different processes based upon interactions between a charged solid surface and a liquid electrolyte. Energy storage in capacitive porous materials, ionic membranes, capacitive deionization (CDI) for water desalination, capacitive energy generation, removal of heavy ions from wastewater streams, and geophysical applications are some examples of these processes. Process development is driven by the production of porous materials with increasing surface area. Understanding of the physical phenomena occurring at the charged solid-electrolyte interface will significantly improve the design and development of more effective applied processes. The goal of this work is to critically review the current knowledge in the field. The focus is on concepts behind different models. We start by briefly presenting the classical electrical double layer (EDL) models in flat surfaces. Then, we discuss models for porous materials containing macro-, meso-, and micro-pores. Some of the current models for systems comprising two different pore sizes are also included. Finally, we discuss the concepts behind the most common models used for ionic transport and Faradaic processes in porous media. The latter models are used for simulation of electrosorption processes in porous media.

42 ENGINEERING↗

Revealing causes of macroscale heterogeneity in lithium ion pouch cells via synchrotron X-ray diffraction

Heterogeneous battery performance is a critical issue for maximization of cell lifetime capacity and safety. Using high energy synchrotron X-ray diffraction, the influence of charge rate, voltage limit, uneven stack pressure, and gas generation on the lithium transport properties was quantified in single-layer graphite/LiNi 0.5 Mn 0.3 Co 0.2 O 2 pouch cells. A freshly formatted cell tracked in operando during initial fast charge cycles indicated variable position-dependent performances, while lateral mapping showed a significant fast charge (6C) heterogeneity compared to slow charge (C/2). Pressure effects were non-dominant compared to charge rate. Maps of previously aged and rested cells indicate that lateral heterogeneity slowly equilibrates at rest, but regenerates upon further cycling at fast charge rate. Furthermore, an unformatted cell was mapped at charge and discharge during its first formation cycle to analyze the effect of byproduct gases on the heterogeneous lithium transport. Gas was observed as randomly interspersed “bubbles” which locally hindered lithium intercalation and caused significant heterogeneity. Electrode architectures and charging protocols that promote homogeneous intercalation are critical for predictable high-performance and long-life batteries.

25 ENERGY STORAGE↗

Formation and chemical reactivity of carbon fibers prepared by defluorination of graphite fluoride

Defluorination of graphite fluoride (CFX) by heating to temperatures of 250 to 450 C in chemically reactive environments was studied. This is a new and possibly inexpensive process to produce new carbon-based materials. For example, CF 0.68 fibers, made from P-100 carbon fibers, can be defluorinated in BrH2C-CH = CH-CH2Br (1,4-dibromo-2butene) heated to 370 C, and graphitized to produce fibers with an unusually high modulus and a graphite layer structure that is healed and cross-linked. Conversely, a sulfur-doped, visibly soft carbon fiber was produced by defluorinating CF 0.9 fibers, made from P-25, in sulfur (S) vapor at 370 C and then heating to 660 C in nitrogen (N2). Furthermore, defluorination of the CF 0.68 fibers in bromine (Br2) produced fragile, structurally damaged carbon fibers. Heating these fragile fibers to 1100 C in N2 caused further structural damage, whereas heating to 150 C in bromoform (CHBr3) and then to 1100 C in N2 healed the structural defects. The defluorination product of CFX, tentatively called activated graphite, has the composition and molecular structure of graphite, but is chemically more reactive. Activated graphite is a scavenger of manganese (Mn), and can be intercalated with magnesium (Mg). Also, it can easily collect large amounts of an alloy made from copper (Cu) and type 304 stainless steel to form a composite. Finally, there are indications that activated graphite can wet metals or ceramics, thereby forming stronger composites with them than the pristine carbon fibers can form.

Hung, Ching-Cheh↗

Assessing Impacts on Pressure Stabilization and Leasing Acreage for CO 2 Storage Utilizing Oil Migration Concepts

Favorable geological storage for CO 2 has long been pictured as large anticlines with thick sandstones, similar to oil reservoirs in the petroleum system. Unlike oil, however, stored CO 2 does not need to be recoverable, which raises the possibility of using dissolution and residual trapping to augment the capacity of buoyant traps and tap more of the bulk rock volume. The work presented builds on that idea, asking the following question: If we inject CO 2 down to a syncline – analogous to the carrier bed in the petroleum system – how would this injection mechanism impact storage capacity and plume shape, migration, and stabilization? To address this question, we built a reservoir model, based on seismic interpretation of Middle Miocene strata, offshore Galveston, Texas. 3-D seismic and well logs were used to characterize key intervals. Reservoirs chosen for modeling are progradational-aggradational sands with mud intercalation. They have a higher degree of heterogeneity than the more conventional reservoirs commonly targeted for CO 2 storage. Modeling investigated how far the CO 2 plume would migrate under two scenarios: (1) injecting CO 2 at the base of the salt withdrawal basin (syncline scenario) and (2) injecting CO 2 at the base of the structural closure, similar to a common injection well location for EOR purposes (base scenario). For each scenario, we separately simulated injection of 30 MT of CO 2 and 60 MT of CO 2 continuously for 30 years and observe the plume and pressure evolution for 100 years after the injection stops. The simulation shows that injecting the CO 2 into a syncline limits the vertical migration of CO 2 , thus making synclinal injection more secure. In the syncline scenario, the geological layer around the injection point is more heterogeneous than the layer in the base scenario; thus, the CO 2 tends to migrate laterally. Additionally, in the syncline scenario, the plume does not even reach the upper part of the anticline, allowing us to safely store an additional amount of CO 2 into the reservoir. Furthermore, the simulation also shows that in the syncline scenario, the times needed for the reservoir to reach its stabilized pressure after the end of injections are faster. To summarize, CO 2 injection at the base of a syncline could provide additional storage, increase the safety of the project from the limited vertical plume migration, and expedite plume stabilization, which could result in the decrease of monitoring frequency as the project runs, thus lowering the operating cost of the project in the long run.

58 GEOSCIENCES↗

Compositionally complex doping for zero-strain zero-cobalt layered cathodes

We report the high volatility of the price of cobalt and the geopolitical limitations of cobalt mining have made the elimination of Co a pressing need for the automotive industry. Owing to their high energy density and low-cost advantages, high-Ni and low-Co or Co-free (zero-Co) layered cathodes have become the most promising cathodes for next-generation lithium-ion batteries. However, current high-Ni cathode materials, without exception, suffer severely from their intrinsic thermal and chemo-mechanical instabilities and insufficient cycle life. Here, in this paper, by using a new compositionally complex (high-entropy) doping strategy, we successfully fabricate a high-Ni, zero-Co layered cathode that has extremely high thermal and cycling stability. Combining X-ray diffraction, transmission electron microscopy and nanotomography, we find that the cathode exhibits nearly zero volumetric change over a wide electrochemical window, resulting in greatly reduced lattice defects and local strain-induced cracks. In-situ heating experiments reveal that the thermal stability of the new cathode is significantly improved, reaching the level of the ultra-stable NMC-532. Owing to the considerably increased thermal stability and the zero volumetric change, it exhibits greatly improved capacity retention. This work, by resolving the long-standing safety and stability concerns for high-Ni, zero-Co cathode materials, offers a commercially viable cathode for safe, long-life lithium-ion batteries and a universal strategy for suppressing strain and phase transformation in intercalation electrodes.

25 ENERGY STORAGE↗

Building Artificial Layered Solids from the Bottom-up: Materials by Design to Enable New Energy Technologies

This final technical report summarizes the key accomplishments on this DOE Early Career Program award received by PI Guihua Yu at the University of Texas at Austin. The main goal of this ECP award was to develop synthetic methodologies, self-assembly approaches towards structurally controlled nanosheets-like solids from the bottom up, and to understand and characterize their chemical/physical characteristics for the design of future-generation energy devices with novel functions and properties, that will have direct implications for energy science and technologies such as energy storage and conversion, and catalysis. The project accomplished these goals by completing the following objectives: • Rational design, synthesis, and self-assembly of structurally-controlled molecular ‘nanosheets’ materials. Moving beyond conventional van der Waals two-dimensional crystals, this project enables new synthesis and processing strategies to develop ultrathin nanosheets materials, from inorganic transition-metal oxides-based, to hybrid organic-inorganic nanomaterials, with structural factors such as facet, thickness and pore structure being well controlled during synthesis or assembly processes. • Fundamental understanding and electrochemical characterization of these assembled molecular ‘nanosheets’ materials via charge/mass transport studies through electrochemical intercalation of different metal ions for next-generation energy storage, as well as electrocatalytic studies using this new material platform for understanding catalytic reaction kinetics and the roles of surface functionalization and interface interactions owing to atomic thickness, nanoscale porosity, and other structural factors.

36 MATERIALS SCIENCE↗

In Operando Calorimetric Measurements for Activated Carbon Electrodes in Ionic Liquid Electrolytes under Large Potential Windows

This study aims to investigate the effect of the potential window on heat generation in carbon-based electrical double layer capacitors (EDLCs) with ionic-liquid (IL)-based electrolytes using in operando calorimetry. The EDLCs consisted of two identical activated-carbon electrodes with either neat 1-butyl-1-methylpyrrolidinium bis(trifluoromethane-sulfonyl)imide ([Pyr 14 ][TFSI]) electrolyte or 1.0 m [Pyr 14 ][TFSI] in propylene carbonate (PC) as electrolyte. The instantaneous heat generation rate at each electrode was measured under galvanostatic cycling for different potential windows ranging from 1 to 4 V. First, the heat generation rates at the positive and negative electrodes differed significantly in neat IL owing to the differences in the ion sizes and diffusion coefficients. However, these differences were minimized when the IL was diluted in PC. Second, for EDLC in neat [Pyr 14 ][TFSI] at high potential window (4 V), a pronounced endothermic peak was observed at the beginning of the charging step at the positive electrode owing to TFSI - intercalation in the activated carbon. On the other hand, for EDLC in 1.0 m [Pyr 14 ][TFSI] in PC at potential window above 3 V, an endothermic peak was observed only at the negative electrode owing to the decomposition of PC. Third, for both neat and diluted [Pyr 14 ][TFSI] electrolytes, the irreversible heat generation rate increased with increasing potential window and exceeded Joule heating. This was attributed to the effect of potential-dependent charge redistribution resistance. Additionally, a further increase in the irreversible heat generation rate was observed for the largest potential windows owing to the degradation of the PC solvent. Finally, for both types of electrolyte, the reversible heat generation rate increased with increasing potential window because of the increase in the amount of ion adsorbed/desorbed at the electrode/electrolyte interface.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Tuning the Porous Structure in PMMA-Templated Mesoporous MoO 2 for Pseudocapacitive Li-Ion Electrodes

MoO 2 is an exciting candidate for next-generation energy storage. It can be used for fast-charging applications in nanoscale form, but its kinetic performance is often limited by insulating MoO 3 surface oxide layers. Here, we developed methods to produce polymer-templated porous MoO 2 powders where electrical conductivity was well-maintained throughout the structure, even in the presence of some surface oxidation. Porosity, pore size, and crystallite size were controlled by varying the amount and size of the colloidal templates and through calcination temperature. The electrochemical performance was correlated with nanoscale structure: samples with high porosity, medium pore sizes, and good crystallinity display optimal rate capabilities, with over 100 mAh g −1 delivered in 3 min and 93% capacity retention after 1000 cycles. Kinetic studies were performed on samples with the largest and smallest crystallite sizes to understand the charge storage mechanism. In the sample with the smallest crystallite size, 85% of the total stored charge was capacitive, compared to 60% for the largest crystallite size. Sloping voltage profiles in materials with smaller domain sizes further suggest suppression of intercalation-induced phase transitions. This work thus provides insights into the mechanisms of charge storage in nanoscale MoO 2 and design parameters for the production of fast charging materials.

25 ENERGY STORAGE↗

Highly reversible Zn anode with a practical areal capacity enabled by a sustainable electrolyte and superacid interfacial chemistry

Aqueous zinc-metal batteries are plagued by poor Zn reversibility owing to zinc dendrite and layered double hydroxide (LDH) formation. Here, we introduce a novel additive—N,N-dimethylformamidium trifluoromethanesulfonate (DOTf)—in a low-cost aqueous electrolyte that can very effectively address these issues. The initial water-assisted dissociation of DOTf into triflic superacid creates a robust nanostructured solid-electrolyte interface (SEI)—revealed by operando spectroscopy and cryomicroscopy—which excludes water and enables dense Zn deposition. We demonstrate excellent Zn plating/stripping in a Zn||Cu asymmetric cell for more than 3,500 cycles. Furthermore, near 100% CE is realized at a combined high current density of 4 mA cm -2 and an areal capacity of 4 mAh cm -2 over long-term cycling. Zn||Zn 0.25 V 2 O 5 ·nH 2 O full cells retain ~83% of their capacity after 1,000 cycles with mass-limited Zn anodes. By restricting the depth of discharge, the cathodes exhibit less proton intercalation and LDH formation with an extended lifetime of 2,000 cycles.

25 ENERGY STORAGE↗

Designing a hybrid electrode toward high energy density with a staged Li + and PF 6 - deintercalation/intercalation mechanism

Existing lithium-ion battery technology is struggling to meet our increasing requirements for high energy density, long lifetime, and low-cost energy storage. Here, a hybrid electrode design is developed by a straightforward reengineering of commercial electrode materials, which has revolutionized the “rocking chair” mechanism by unlocking the role of anions in the electrolyte. Our proof-of-concept hybrid LiFePO 4 (LFP)/graphite electrode works with a staged deintercalation/intercalation mechanism of Li + cations and PF 6 - anions in a broadened voltage range, which was thoroughly studied by ex situ X-ray diffraction, ex situ Raman spectroscopy, and operando neutron powder diffraction. Introducing graphite into the hybrid electrode accelerates its conductivity, facilitating the rapid extraction/insertion of Li + from/into the LFP phase in 2.5 to 4.0 V. This charge/discharge process, in turn, triggers the in situ formation of the cathode/electrolyte interphase (CEI) layer, reinforcing the structural integrity of the whole electrode at high voltage. Consequently, this hybrid LFP/graphite-20% electrode displays a high capacity and long-term cycling stability over 3,500 cycles at 10 C, superior to LFP and graphite cathodes. Importantly, the broadened voltage range and high capacity of the hybrid electrode enhance its energy density, which is leveraged further in a full-cell configuration.

25 ENERGY STORAGE↗

Adsorption of Mixed Micelles of Polysorbate 80 and Oleic Acid to the Air–Water Interface

The solubilization of long chain amphiphiles with limited solubility into mixed micelles composed of highly soluble surfactants plays a crucial role in modulating the stability and functionality of formulations in pharmaceutical and food systems. Subsequently, the mixed micelles adsorb from solution to the air−water surface, defining the transport mechanism of the insoluble amphiphiles to the interface. We use X-ray reflectivity to measure the composition and provide insight into the structure of these mixed monolayers, and, alongside interfacial tension measurements, we provide an understanding of how the bulk composition determines the surface composition and the dynamics of tension reduction. We use a model system consisting of an insoluble fatty acid, oleic acid (OA), and a soluble micelle-forming surfactant, polysorbate 80 (PS80). PS80 forms spherical micelles, and, above the critical micelle concentration (cmc), OA is readily solubilized inside the micelles. We show that the adsorption of PS80/OA mixed micelles to the air−water interface rapidly reduces the tension and lowers the equilibrium tension in proportion to the OA concentration. X-ray reflectivity data, fit using Parratt-slab models, quantitively demonstrates that the monolayers become enriched with OA, and we show how the OA intercalates into the PS80 monolayers.

36 MATERIALS SCIENCE↗

Electronic interactions and stability issues at the copper-graphene interface in air and in alkaline solution under electrochemical control

A micro-electrochemical cell is sealed with a polymer-free single-layer graphene (SLG) membrane to monitor the stability of Cu nanoparticles (NPs) attached to SLG, as well as the interfacial electronic interactions between Cu NPs and SLG both in air and in a mildly alkaline aqueous solution under electrochemical control. A combination of techniques, including in-situ Kelvin probe force microscopy (KPFM) and ex-situ electron microscopy, are applied. When Cu NPs are metallic at cathodic potentials, there is a relatively bias-independent offset in the SLG work function due to charge transfer at the Cu-SLG contact. When Cu NPs are oxidized at anodic potentials, on the other hand, the work function of SLG also depends on the applied bias in a quasi-linear fashion due to electrochemical gating, in addition to charge transfer at the CuOx-SLG contact. Furthermore, Cu NPs were found to oxidize and detach from SLG when kept under anodic potentials for a few hours, whereas they remain adhered to SLG at cathodic potentials. This is attributed to water intercalation at the CuO-SLG interface associated with the enhanced hydrophilicity of positively polarized graphene, as supported by the absence of Cu detachment following oxidation by galvanic corrosion in air.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Electrical and Thermal Conductivity of Woven Pristine and Intercalated Graphite Fiber-Polymer Composites

A series of woven fabric laminar composite plates and narrow strips were fabricated from a variety of pitch-based pristine and bromine intercalated graphite fibers in an attempt to determine the influence of the weave on the electrical and thermal conduction. It was found generally that these materials can be treated as if they are homogeneous plates. The rule of mixtures describes the resistivity of the composite fairly well if it is realized that only the component of the fibers normal to the equipotential surface will conduct current. When the composite is narrow with respect to the fiber weave, however, there is a marked angular dependence of the resistance which was well modeled by assuming that the current follows only along the fibers (and not across them in a transverse direction), and that the contact resistance among the fibers in the composite is negligible. The thermal conductivity of composites made from less conductive fibers more closely followed the rule of mixtures than that of the high conductivity fibers, though this is thought to be an artifact of the measurement technique. Electrical and thermal anisotropy could be induced in a particular region of the structure by weaving together high and low conductivity fibers in different directions, though this must be done throughout all of the layers of the structure as interlaminar conduction precludes having only the top layer carry the anisotropy. The anisotropy in the thermal conductivity is considerably less than either that predicted by the rule of mixtures or the electrical resistivity.

Gaier, James R.↗

Cation reordering instead of phase transitions: Origins and implications of contrasting lithiation mechanisms in 1D ζ- and 2D α-V 2 O 5

Substantial improvements in cycle life, rate performance, accessible voltage, and reversible capacity are required to realize the promise of Li-ion batteries in full measure. Here, we have examined insertion electrodes of the same composition (V 2 O 5 ) prepared according to the same electrode specifications and comprising particles with similar dimensions and geometries that differ only in terms of their atomic connectivity and crystal structure, specifically two-dimensional (2D) layered α-V 2 O 5 that crystallizes in an orthorhombic space group and one-dimensional (1D) tunnel-structured ζ-V 2 O 5 crystallized in a monoclinic space group. By using particles of similar dimensions, we have disentangled the role of specific structural motifs and atomistic diffusion pathways in affecting electrochemical performance by mapping the dynamical evolution of lithiation-induced structural modifications using ex situ scanning transmission X-ray microscopy, operando synchrotron X-ray diffraction measurements, and phase-field modeling. We find the operation of sharply divergent mechanisms to accommodate increasing concentrations of Li-ions: a series of distortive phase transformations that result in puckering and expansion of interlayer spacing in layered α-V 2 O 5 , as compared with cation reordering along interstitial sites in tunnel-structured ζ-V 2 O 5 . By alleviating distortive phase transformations, the ζ-V 2 O 5 cathode shows reduced voltage hysteresis, increased Li-ion diffusivity, alleviation of stress gradients, and improved capacity retention. The findings demonstrate that alternative lithiation mechanisms can be accessed in metastable compounds by dint of their reconfigured atomic connectivity and can unlock substantially improved electrochemical performance not accessible in the thermodynamically stable phase.

25 ENERGY STORAGE↗