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1.
Chem Commun (Camb) ; 2023 Jan 24.
Artigo em Inglês | MEDLINE | ID: mdl-36691895

RESUMO

Dissolved transition metal ions can induce peak shifts in the NMR spectra of degraded battery electrolytes. Here, we exploit this staightforward, accessible method to calculate magnetic moments for dissolved Ni2+, Mn2+, Co2+, and Cu2+; subsequent analysis of dissolution from LiMn2O4, LiNiO2, and LiNi0.5Mn1.5O4 shows that the dissolved metals are exclusively divalent.

2.
Inorg Chem ; 61(48): 19203-19219, 2022 Dec 05.
Artigo em Inglês | MEDLINE | ID: mdl-36384021

RESUMO

Single-source precursors are ubiquitous in a number of areas of chemistry and material science due to their ease of use and wide range of potential applications. The development of new single-source precursors is essential in providing entries to new areas of chemistry. In this work, we synthesize nine new structurally related bimetallic metal-zirconium alkoxides, which can be used as single-source precursors to zirconia-based materials. Detailed analysis of the structures of these complexes provides important insights into the main factors influencing their aggregation. Investigation of the thermal decomposition of these species by TGA, PXRD, SEM, and EDS reveals that they can be used to produce bimetal oxides, such as Li2ZrO3, or a mixture of metal oxides, such as CuO and ZrO2. Significantly, these studies show that thermodynamically unstable forms of zirconia, such as the tetragonal phase, can be stabilized by metal doping, providing the promise for targeted deposition of zirconia materials for specific applications.

3.
J Mater Chem A Mater ; 10(41): 21941-21954, 2022 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-36353664

RESUMO

Li- and Mn-rich layered oxides (Li1.2Ni0.2Mn0.6O2) are actively pursued as high energy and sustainable alternatives to the current Li-ion battery cathodes that contain Co. However, the severe decay in discharge voltage observed in these cathodes needs to be addressed before they can find commercial applications. A few mechanisms differing in origin have been proposed to explain the voltage fade, which may be caused by differences in material composition, morphology and electrochemical testing protocols. Here, these challenges are addressed by synthesising Li1.2Ni0.2Mn0.6O2 using three different hydrothermal and solid-state approaches and studying their degradation using the same cell design and cycling protocols. The voltage fade is found to be similar under the same electrochemical testing protocols, regardless of the synthesis method. X-ray absorption near edge, extended X-ray absorption fine structure spectroscopies, and energy loss spectroscopy in a scanning transmission electron microscope indicate only minor changes in the bulk Mn oxidation state but reveal a much more reduced particle surface upon extended cycling. No spinel phase is seen via the bulk structural characterisation methods of synchrotron X-ray diffraction, 7Li magic angle spinning solid state nuclear magnetic resonance and Raman spectroscopy. Thus, the voltage fade is believed to largely result from a heavily reduced particle surface. This hypothesis is further confirmed by galvanostatic intermittent titration technique analysis, which indicates that only very small shifts in equilibrium potential take place, in contrast to the overpotential which builds up after cycling. This suggests that a major source of the voltage decay is kinetic in origin, resulting from a heavily reduced particle surface with slow Li transport.

4.
Chem Sci ; 13(37): 11083-11090, 2022 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-36320476

RESUMO

Determining the different surfaces of oxide nanocrystals is key in developing structure-property relations. In many cases, only surface geometry is considered while ignoring the influence of surroundings, such as ubiquitous water on the surface. Here we apply 17O solid-state NMR spectroscopy to explore the facet differences of morphology-controlled ceria nanocrystals considering both geometry and water adsorption. Tri-coordinated oxygen ions at the 1st layer of ceria (111), (110), and (100) facets exhibit distinct 17O NMR shifts at dry surfaces while these 17O NMR parameters vary in the presence of water, indicating its non-negligible effects on the oxide surface. Thus, the interaction between water and oxide surfaces and its impact on the chemical environment should be considered in future studies, and solid-state NMR spectroscopy is a sensitive approach for obtaining such information. The work provides new insights into elucidating the surface chemistry of oxide nanomaterials.

5.
ACS Energy Lett ; 7(10): 3524-3530, 2022 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-36277132

RESUMO

High-capacity Ni-rich layered metal oxide cathodes are highly desirable to increase the energy density of lithium-ion batteries. However, these materials suffer from poor cycling performance, which is exacerbated by increased cell voltage. We demonstrate here the detrimental effect of ethylene carbonate (EC), a core component in conventional electrolytes, when NMC811 (LiNi0.8Mn0.1Co0.1O2) is charged above 4.4 V vs Li/Li+-the onset potential for lattice oxygen release. Oxygen loss is enhanced by EC-containing electrolytes-compared to EC-free-and correlates with more electrolyte oxidation/breakdown and cathode surface degradation, which increase concurrently above 4.4 V. In contrast, NMC111 (LiNi0.33Mn0.33Co0.33O2), which does not release oxygen up to 4.6 V, shows a similar extent of degradation irrespective of the electrolyte. This work highlights the incompatibility between conventional EC-based electrolytes and Ni-rich cathodes (more generally, cathodes that release lattice oxygen such as Li-/Mn-rich and disordered rocksalt cathodes) and motivates further work on wider classes of electrolytes and additives.

6.
Chem Commun (Camb) ; 58(85): 11949-11952, 2022 Oct 25.
Artigo em Inglês | MEDLINE | ID: mdl-36205108

RESUMO

The structure of a new ZIF-8 polymorph with quartz topology (qtz) is reported. This qtz-[Zn(mIm)2] phase was obtained by mechanically amorphising crystalline ZIF-8, before heating the resultant amorphous phase to between 282 and 316 °C. The high-temperature phase structure was obtained from powder X-ray diffraction, and its thermal behaviour, CO2 gas sorption properties and dye adsorption ability were investigated.

7.
J Am Chem Soc ; 144(41): 18714-18729, 2022 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-36201656

RESUMO

Modern studies of lithium-ion battery (LIB) cathode materials employ a large range of experimental and theoretical techniques to understand the changes in bulk and local chemical and electronic structures during electrochemical cycling (charge and discharge). Despite its being rich in useful chemical information, few studies to date have used 17O NMR spectroscopy. Many LIB cathode materials contain paramagnetic ions, and their NMR spectra are dominated by hyperfine and quadrupolar interactions, giving rise to broad resonances with extensive spinning sideband manifolds. In principle, careful analysis of these spectra can reveal information about local structural distortions, magnetic exchange interactions, structural inhomogeneities (Li+ concentration gradients), and even the presence of redox-active O anions. In this Perspective, we examine the primary interactions governing 17O NMR spectroscopy of LIB cathodes and outline how 17O NMR may be used to elucidate the structure of pristine cathodes and their structural evolution on cycling, providing insight into the challenges in obtaining and interpreting the spectra. We also discuss the use of 17O NMR in the context of anionic redox and the role this technique may play in understanding the charge compensation mechanisms in high-capacity cathodes, and we provide suggestions for employing 17O NMR in future avenues of research.

8.
Nat Commun ; 13(1): 6070, 2022 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-36241622

RESUMO

The solid electrolyte interphase (SEI) that forms on Li-ion battery anodes is critical to their long-term performance, however observing SEI formation processes at the buried electrode-electrolyte interface is a significant challenge. Here we show that operando soft X-ray absorption spectroscopy in total electron yield mode can resolve the chemical evolution of the SEI during electrochemical formation in a Li-ion cell, with nm-scale interface sensitivity. O, F, and Si K-edge spectra, acquired as a function of potential, reveal when key reactions occur on high-capacity amorphous Si anodes cycled with and without fluoroethylene carbonate (FEC). The sequential formation of inorganic (LiF) and organic (-(C=O)O-) components is thereby revealed, and results in layering of the SEI. The addition of FEC leads to SEI formation at higher potentials which is implicated in the rapid healing of SEI defects and the improved cycling performance observed. Operando TEY-XAS offers new insights into the formation mechanisms of electrode-electrolyte interphases and their stability for a wide variety of electrode materials and electrolyte formulations.

9.
Adv Mater ; : e2201384, 2022 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-36063023

RESUMO

The realization of practical nonaqueous lithium-air batteries (LABs) calls for novel strategies to address their numerous theoretical and technical challenges. LiOH formation/decomposition has recently been proposed as a promising alternative route to cycling LABs via Li2 O2 . Herein, the progress in developing LiOH-based nonaqueous LABs is reviewed. Various catalytic systems, either soluble or solid-state, that can activate a LiOH-based electrochemistry are compared in detail, with emphasis in providing an updated understanding of the oxygen reduction and evolution reactions in nonaqueous media. We identify the key factors that can switch the cell chemistry between Li2 O2  and LiOH and highlight the debate around these routes, as well as rationalize potential causes for these opposing opinions. The identities of the reaction intermediates, activity of redox mediators and additives, location of reaction interfaces, causes of parasitic reactions, as well as the effect of CO2  on the LiOH electrochemistry, all play a critical role in altering the relative rates of a series of interconnected reactions and all warrant further investigation.

10.
Energy Environ Sci ; 15(8): 3416-3438, 2022 Aug 11.
Artigo em Inglês | MEDLINE | ID: mdl-36091097

RESUMO

Preventing the decomposition reactions of electrolyte solutions is essential for extending the lifetime of lithium-ion batteries. However, the exact mechanism(s) for electrolyte decomposition at the positive electrode, and particularly the soluble decomposition products that form and initiate further reactions at the negative electrode, are still largely unknown. In this work, a combination of operando gas measurements and solution NMR was used to study decomposition reactions of the electrolyte solution at NMC (LiNi x Mn y Co1-x-y O2) and LCO (LiCoO2) electrodes. A partially delithiated LFP (Li x FePO4) counter electrode was used to selectively identify the products formed through processes at the positive electrodes. Based on the detected soluble and gaseous products, two distinct routes with different onset potentials are proposed for the decomposition of the electrolyte solution at NMC electrodes. At low potentials (<80% state-of-charge, SOC), ethylene carbonate (EC) is dehydrogenated to form vinylene carbonate (VC) at the NMC surface, whereas at high potentials (>80% SOC), 1O2 released from the transition metal oxide chemically oxidises the electrolyte solvent (EC) to form CO2, CO and H2O. The formation of water via this mechanism was confirmed by reacting 17O-labelled 1O2 with EC and characterising the reaction products via 1H and 17O NMR spectroscopy. The water that is produced initiates secondary reactions, leading to the formation of the various products identified by NMR spectroscopy. Noticeably fewer decomposition products were detected in NMC/graphite cells compared to NMC/Li x FePO4 cells, which is ascribed to the consumption of water (from the reaction of 1O2 and EC) at the graphite electrode, preventing secondary decomposition reactions. The insights on electrolyte decomposition mechanisms at the positive electrode, and the consumption of decomposition products at the negative electrode contribute to understanding the origin of capacity loss in NMC/graphite cells, and are hoped to support the development of strategies to mitigate the degradation of NMC-based cells.

11.
ACS Energy Lett ; 7(8): 2745-2752, 2022 Aug 12.
Artigo em Inglês | MEDLINE | ID: mdl-35990415

RESUMO

CsPbI3 is a promising material for optoelectronics owing to its thermal robustness and favorable bandgap. However, its fabrication is challenging because its photoactive phase is thermodynamically unstable at room temperature. Adding dimethylammonium (DMA) alleviates this instability and is currently understood to result in the formation of DMA x Cs1-x PbI3 perovskite solid solutions. Here, we use NMR of the 133Cs and 13C local structural probes to show that these solid solutions are not thermodynamically stable, and their synthesis under thermodynamic control leads to a segregated mixture of yellow one-dimensional DMAPbI3 phase and δ-CsPbI3. We show that mixed-cation DMA x Cs1-x PbI3 perovskite phases only form when they are kinetically trapped by rapid antisolvent-induced crystallization. We explore the energetics of DMA incorporation into CsPbI3 using first-principles calculations and molecular dynamics simulations and find that this process is energetically unfavorable. Our results provide a complete atomic-level picture of the mechanism of DMA-induced stabilization of the black perovskite phase of CsPbI3 and shed new light on this deceptively simple material.

12.
Nat Mater ; 21(11): 1306-1313, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35970962

RESUMO

To rationalize and improve the performance of newly developed high-rate battery electrode materials, it is crucial to understand the ion intercalation and degradation mechanisms occurring during realistic battery operation. Here we apply a laboratory-based operando optical scattering microscopy method to study micrometre-sized rod-like particles of the anode material Nb14W3O44 during high-rate cycling. We directly visualize elongation of the particles, which, by comparison with ensemble X-ray diffraction, allows us to determine changes in the state of charge of individual particles. A continuous change in scattering intensity with state of charge enables the observation of non-equilibrium kinetic phase separations within individual particles. Phase field modelling (informed by pulsed-field-gradient nuclear magnetic resonance and electrochemical experiments) supports the kinetic origin of this separation, which arises from the state-of-charge dependence of the Li-ion diffusion coefficient. The non-equilibrium phase separations lead to particle cracking at high rates of delithiation, particularly in longer particles, with some of the resulting fragments becoming electrically disconnected on subsequent cycling. These results demonstrate the power of optical scattering microscopy to track rapid non-equilibrium processes that would be inaccessible with established characterization techniques.

13.
J Am Chem Soc ; 144(36): 16350-16365, 2022 Sep 14.
Artigo em Inglês | MEDLINE | ID: mdl-36040461

RESUMO

All-solid-state batteries based on non-combustible solid electrolytes are promising candidates for safe energy storage systems. In addition, they offer the opportunity to utilize metallic lithium as an anode. However, it has proven to be a challenge to design an electrolyte that combines high ionic conductivity and processability with thermodynamic stability toward lithium. Herein, we report a new highly conducting solid solution that offers a route to overcome these challenges. The Li-P-S ternary was first explored via a combination of high-throughput crystal structure predictions and solid-state synthesis (via ball milling) of the most promising compositions, specifically, phases within the Li3P-Li2S tie line. We systematically characterized the structural properties and Li-ion mobility of the resulting materials by X-ray and neutron diffraction, solid-state nuclear magnetic resonance spectroscopy (relaxometry), and electrochemical impedance spectroscopy. A Li3P-Li2S metastable solid solution was identified, with the phases adopting the fluorite (Li2S) structure with P substituting for S and the extra Li+ ions occupying the octahedral voids and contributing to the ionic transport. The analysis of the experimental data is supported by extensive quantum-chemical calculations of both structural stability, diffusivity, and activation barriers for Li+ transport. The new solid electrolytes show Li-ion conductivities in the range of established materials, while their composition guarantees thermodynamic stability toward lithium metal anodes.

14.
Nat Chem ; 14(10): 1103-1109, 2022 10.
Artigo em Inglês | MEDLINE | ID: mdl-35710986

RESUMO

Aqueous organic redox flow batteries offer a safe and potentially inexpensive solution to the problem of storing massive amounts of electricity produced from intermittent renewables. However, molecular decomposition represents a major barrier to commercialization-and although structural modifications can improve stability, it comes at the expense of synthetic cost and molecular weight. Now, utilizing 2,6-dihydroxy-anthraquinone (DHAQ) without further structural modification, we demonstrate that the regeneration of the original molecule after decomposition represents a viable route to achieve low-cost, long-lifetime aqueous organic redox flow batteries. We used in situ (online) NMR and electron paramagnetic resonance, and complementary electrochemical analyses to show that the decomposition compound 2,6-dihydroxy-anthrone (DHA) and its tautomer, 2,6-dihydroxy-anthranol (DHAL) can be recomposed to DHAQ electrochemically through two steps: oxidation of DHA(L)2- to the dimer (DHA)24- by one-electron transfer followed by oxidation of (DHA)24- to DHAQ2- by three-electron transfer per DHAQ molecule. This electrochemical regeneration process also rejuvenates the positive electrolyte-rebalancing the states of charge of both electrolytes without introducing extra ions.


Assuntos
Antralina , Mitoxantrona , Eletrólitos/química , Íons , Oxirredução
15.
J Am Chem Soc ; 144(27): 12102-12115, 2022 Jul 13.
Artigo em Inglês | MEDLINE | ID: mdl-35759794

RESUMO

Colloidal lead-halide perovskite nanocrystals (LHP NCs) have emerged over the past decade as leading candidates for efficient next-generation optoelectronic devices, but their properties and performance critically depend on how they are purified. While antisolvents are widely used for purification, a detailed understanding of how the polarity of the antisolvent influences the surface chemistry and composition of the NCs is missing in the field. Here, we fill this knowledge gap by studying the surface chemistry of purified CsPbBrxI3-x NCs as the model system, which in itself is considered a promising candidate for pure-red light-emitting diodes and top-cells for tandem photovoltaics. Interestingly, we find that as the polarity of the antisolvent increases (from methyl acetate to acetone to butanol), there is a blueshift in the photoluminescence (PL) peak of the NCs along with a decrease in PL quantum yield (PLQY). Through transmission electron microscopy and X-ray photoemission spectroscopy measurements, we find that these changes in PL properties arise from antisolvent-induced iodide removal, which leads to a change in halide composition and, thus, the bandgap. Using detailed nuclear magnetic resonance (NMR) and Fourier-transform infrared spectroscopy (FTIR) measurements along with density functional theory calculations, we propose that more polar antisolvents favor the detachment of the oleic acid and oleylamine ligands, which undergo amide condensation reactions, leading to the removal of iodide anions from the NC surface bound to these ligands. This work shows that careful selection of low-polarity antisolvents is a critical part of designing the synthesis of NCs to achieve high PLQYs with minimal defect-mediated phase segregation.

16.
Chem Mater ; 34(5): 2034-2048, 2022 Mar 08.
Artigo em Inglês | MEDLINE | ID: mdl-35557994

RESUMO

Ni-rich lithium nickel manganese cobalt (NMC) oxide cathode materials promise Li-ion batteries with increased energy density and lower cost. However, higher Ni content is accompanied by accelerated degradation and thus poor cycle lifetime, with the underlying mechanisms and their relative contributions still poorly understood. Here, we combine electrochemical analysis with surface-sensitive X-ray photoelectron and absorption spectroscopies to observe the interfacial degradation occurring in LiNi0.8Mn0.1Co0.1O2-graphite full cells over hundreds of cycles between fixed cell voltages (2.5-4.2 V). Capacity losses during the first ∼200 cycles are primarily attributable to a loss of active lithium through electrolyte reduction on the graphite anode, seen as thickening of the solid-electrolyte interphase (SEI). As a result, the cathode reaches ever-higher potentials at the end of charge, and with further cycling, a regime is entered where losses in accessible NMC capacity begin to limit cycle life. This is accompanied by accelerated transition-metal reduction at the NMC surface, thickening of the cathode electrolyte interphase, decomposition of residual lithium carbonate, and increased cell impedance. Transition-metal dissolution is also detected through increased incorporation into and thickening of the SEI, with Mn found to be initially most prevalent, while the proportion of Ni increases with cycling. The observed evolution of anode and cathode surface layers improves our understanding of the interconnected nature of the degradation occurring at each electrode and the impact on capacity retention, informing efforts to achieve a longer cycle lifetime in Ni-rich NMCs.

17.
Inorg Chem ; 61(16): 6223-6233, 2022 Apr 25.
Artigo em Inglês | MEDLINE | ID: mdl-35412823

RESUMO

The fabrication of mixed-metal oxide films holds promise for the development of practical photoelectrochemical catalyst coatings but currently presents challenges in terms of homogeneity, cost, and scalability. We report a straightforward and versatile approach to produce catalytically active zirconium-based films for electrochemical and photoelectrochemical water oxidation. The mixed-metal oxide catalyst films are derived from novel single-source precursor oxide cage compounds containing Zr with first-row transition metals such as Co, Fe, and Cu. The Zr-based film doped with Co on fluorine-doped tin oxide (FTO)-coated glass exhibits the highest electrocatalytic O2 evolution performance in an alkaline medium and an operational stability above 18 h. The deposition of this film onto a BiVO4 photoanode significantly enhances its photoelectrochemical activity toward solar water oxidation, lowering the onset potential by 0.12-0.21 V vs reversible hydrogen electrode (RHE) and improving the maximum photocurrent density by ∼50% to 2.41 mA cm-2 for the CoZr-coated BiVO4 photoanodes compared to that for bare BiVO4.

18.
Angew Chem Int Ed Engl ; 61(32): e202202133, 2022 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-35415950

RESUMO

Sodium-ion batteries (SIBs) are a promising grid-level storage technology due to the abundance and low cost of sodium. The development of new electrolytes for SIBs is imperative since it impacts battery life and capacity. Currently, sodium hexafluorophosphate (NaPF6 ) is used as the benchmark salt, but is highly hygroscopic and generates toxic HF. This work describes the synthesis of a series of sodium borate salts, with electrochemical studies revealing that Na[B(hfip)4 ]⋅DME (hfip=hexafluoroisopropyloxy, Oi PrF ) and Na[B(pp)2 ] (pp=perfluorinated pinacolato, O2 C2 (CF3 )4 ) have excellent electrochemical performance. The [B(pp)2 ]- anion also exhibits a high tolerance to air and water. Both electrolytes give more stable electrode-electrolyte interfaces than conventionally used NaPF6 , as demonstrated by impedance spectroscopy and cyclic voltammetry. Furthermore, they give greater cycling stability and comparable capacity to NaPF6 for SIBs, as shown in commercial pouch cells.

19.
Nat Commun ; 13(1): 1651, 2022 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-35347137

RESUMO

Improved analytical tools are urgently required to identify degradation and failure mechanisms in Li-ion batteries. However, understanding and ultimately avoiding these detrimental mechanisms requires continuous tracking of complex electrochemical processes in different battery components. Here, we report an operando spectroscopy method that enables monitoring the chemistry of a carbonate-based liquid electrolyte during electrochemical cycling in Li-ion batteries with a graphite anode and a LiNi0.8Mn0.1Co0.1O2 cathode. By embedding a hollow-core optical fibre probe inside a lab-scale pouch cell, we demonstrate the effective evolution of the liquid electrolyte species by background-free Raman spectroscopy. The analysis of the spectroscopy measurements reveals changes in the ratio of carbonate solvents and electrolyte additives as a function of the cell voltage and show the potential to track the lithium-ion solvation dynamics. The proposed operando methodology contributes to understanding better the current Li-ion battery limitations and paves the way for studies of the degradation mechanisms in different electrochemical energy storage systems.

20.
ACS Appl Mater Interfaces ; 14(11): 13206-13222, 2022 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-35258927

RESUMO

The chemical and electrochemical reactions at the positive electrode-electrolyte interface in Li-ion batteries are hugely influential on cycle life and safety. Ni-rich layered transition metal oxides exhibit higher interfacial reactivity than their lower Ni-content analogues, reacting via mechanisms that are poorly understood. Here, we study the pivotal role of the electrolyte solvent, specifically cyclic ethylene carbonate (EC) and linear ethyl methyl carbonate (EMC), in determining the interfacial reactivity at charged LiNi0.33Mn0.33Co0.33O2 (NMC111) and LiNi0.8Mn0.1Co0.1O2 (NMC811) cathodes by using both single-solvent model electrolytes and the mixed solvents used in commercial cells. While NMC111 exhibits similar parasitic currents with EC-containing and EC-free electrolytes during high voltage holds in NMC/Li4Ti5O12 (LTO) cells, this is not the case for NMC811. Online gas analysis reveals that the solvent-dependent reactivity for Ni-rich cathodes is related to the extent of lattice oxygen release and accompanying electrolyte decomposition, which is higher for EC-containing than EC-free electrolytes. Combined findings from electrochemical impedance spectroscopy (EIS), TEM, solution NMR, ICP, and XPS reveal that the electrolyte solvent has a profound impact on the degradation of the Ni-rich cathode and the electrolyte. Higher lattice oxygen release with EC-containing electrolytes is coupled with higher cathode interfacial impedance, a thicker oxygen-deficient rock-salt surface reconstruction layer, more electrolyte solvent and salt breakdown, and higher amounts of transition metal dissolution. These processes are suppressed in the EC-free electrolyte, highlighting the incompatibility between Ni-rich cathodes and conventional electrolyte solvents. Finally, new mechanistic insights into the chemical oxidation pathways of electrolyte solvents and, critically, the knock-on chemical and electrochemical reactions that further degrade the electrolyte and electrodes curtailing battery lifetime are provided.

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