Electrochemical Potential of the Metal Organic Framework MIL-101(Fe) as Cathode Material in Li-Ion Batteries

Keshavarz, Fatemeh; Kadek, Marius; Barbiellini, B.; Bansil, Arun

doi:10.3390/condmat6020022

Cited by 11 publications

(8 citation statements)

References 58 publications

(84 reference statements)

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“…This intercalation model suggests hydration of Li by the structural FOD water molecules. Reversible and irreversible structural changes induced by Li intercalation have also been reported for other Fe-containing electrodes [38,39].…”

Section: Intercalation Mechanismmentioning

confidence: 54%

Anodic Activity of Hydrated and Anhydrous Iron (II) Oxalate in Li-Ion Batteries

et al. 2022

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We discuss the applicability of the naturally occurring compound Ferrous Oxalate Dihydrate (FOD) (FeC2O4·2H2O) as an anode material in Li-ion batteries. Using first-principles modeling, we evaluate the electrochemical activity of FOD and demonstrate how its structural water content affects the intercalation reaction and contributes to its performance. We show that both Li0 and Li+ intercalation in FOD yields similar results. Our analysis indicates that fully dehydrated ferrous oxalate is a more promising anodic material with higher electrochemical stability: it carries 20% higher theoretical Li storage capacity and a lower voltage (0.68 V at the PBE/cc-pVDZ level), compared to its hydrated (2.29 V) or partially hydrated (1.43 V) counterparts.

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Section: Intercalation Mechanismmentioning

confidence: 54%

Anodic Activity of Hydrated and Anhydrous Iron (II) Oxalate in Li-Ion Batteries

et al. 2022

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“…DFT-based simulations are also able to provide precious information regarding the effect of the local atomic environment and structural deformations on the electrochemical redox potentials [17]. This is well illustrated further by a computational study of the electrochemical potentials in a metal-organic framework used as cathode for Li-ion batteries [25]. In addition, DFT-based methods are used to explain the experimentally measured conductivity and capacity of anode materials, such as in high-capacity Na-ion batteries [26].…”

Section: Advanced Battery Characterisationmentioning

confidence: 88%

Study of Rechargeable Batteries Using Advanced Spectroscopic and Computational Techniques

2021

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Improving the efficiency and longevity of energy storage systems based on Li- and Na-ion rechargeable batteries presents a major challenge. The main problems are essentially capacity loss and limited cyclability. These effects are due to a hierarchy of factors spanning various length and time scales, interconnected in a complex manner. As a consequence, and in spite of several decades of research, a proper understanding of the ageing process has remained somewhat elusive. In recent years, however, combinations of advanced spectroscopy techniques and first-principles simulations have been applied with success to tackle this problem. In this Special Issue, we are pleased to present a selection of articles that, by precisely applying these methods, unravel key aspects of the reduction–oxidation reaction and intercalation processes. Furthermore, the approaches presented provide improvements to standard diagnostic and characterisation techniques, enabling the detection of possible Li-ion flow bottlenecks causing the degradation of capacity and cyclability.

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“…To calibrate the computational level, we evaluated the density functionals that have been commonly used in modeling of MOFs, including PBE, PBE0, HSE06, M06 variations, and ωB97-XD along with various basis sets. , PBE and PBE0 are generally good choices for organometallic complexes . HSE06 is a rather expensive functional but it gives more accurate band gap values .…”

Section: Methodsmentioning

confidence: 99%

“…Such a fragment-based approach has been widely used − and presents some limitations and some perspective implications. The main limitation refers to the fact that some properties of MOFs are collective results of the MN and OL cooperative effects and periodic simulations would be needed to address those.…”

Section: Introductionmentioning

confidence: 99%

“…This does not mean that small-cluster-based models and isolated fragments are never reliable. The fragment-based method would be reliable when the SBUs are well separated, the active site is the MN and the MOF’s stability only depends on the MN. ,, That is why cluster-based methods are still in use as a key to mechanistic insight into many MOF applications (for example, see refs − ). The second limitation is that some MOF properties require highly advanced quantum mechanical treatments in addition to periodicity.…”

Section: Introductionmentioning

confidence: 99%

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Dissecting the Water Uptake Behavior of Metal–Organic Frameworks Using Their Isolated Linkers and Metal Nodes

Keshavarz

2023

Chem. Mater.

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Metal−organic frameworks (MOFs) have been a center of interest because of their highly diverse structural and physicochemical properties. The study of many MOFs requires periodic calculations. However, isolated models have also been employed in first-principles calculations to study their mechanisms and energy profiles. Following the water adsorption properties of MOF building units, this study determines how far isolated models of MOFs can reproduce experimental observations and where they fail. According to our DFT simulations of water adsorption by 70 common metal nodes and over 110 organic linkers, the isolated models provide some opportunities and limitations. They indicate the water adsorption mechanism and energy of the individual MOF components. They give clues about the water stability of the metal nodes and the degradation pathways. Also, they predict an overall trend for the maximum water uptake capacity. However, they cannot always give an accurate insight into MOF's water adsorption enthalpies, their water harvesting efficiency, their water uptake capacities under varying conditions, and a complete picture of the water uptake mechanism inside MOF pores.

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Electrochemical Potential of the Metal Organic Framework MIL-101(Fe) as Cathode Material in Li-Ion Batteries

Cited by 11 publications

References 58 publications

Anodic Activity of Hydrated and Anhydrous Iron (II) Oxalate in Li-Ion Batteries

Anodic Activity of Hydrated and Anhydrous Iron (II) Oxalate in Li-Ion Batteries

Study of Rechargeable Batteries Using Advanced Spectroscopic and Computational Techniques

Dissecting the Water Uptake Behavior of Metal–Organic Frameworks Using Their Isolated Linkers and Metal Nodes

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