Understanding Rechargeable Battery Function Using In Operando Neutron Powder Diffraction

Liang, Gemeng; Didier, Christophe; Guo, Zaiping; Pang, Wei Kong; Peterson, Vanessa K.

doi:10.1002/adma.201904528

Cited by 65 publications

(54 citation statements)

References 119 publications

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“…[ 5 ] Due to the similar scattering factors of Ni and Mn, the XRD patterns of the ordered and disordered phases are almost similar with minor differences. [ 23 ] Although noticeable Ni‐rich rock salt (Ni 1‐ x Li x O) phase impurity appears in the disordered phase (Figure 1g top) and visible low‐symmetry diffraction peaks (blue arrows in Figure 1g bottom) are present in the ordered phase, the XRD technique is unable to clearly distinguish the Fd

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m and P 4 3 32 structures. The independency of neutron scattering lengths from the atomic numbers and the interaction between atomic nuclei and neutrons implies that neutron powder diffraction (NPD) would be a more powerful technique for the analysis of cationic ordering in LNMO.…”

Section: Fundamentals Of High‐voltage Spinel Lnmo Cathodes: Crystal Chemistry/structure Characterization and Electrochemical Mechanismmentioning

confidence: 99%

Advances and Prospects of High‐Voltage Spinel Cathodes for Lithium‐Based Batteries

Manthiram

2021

Small Methods

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Insertion compounds have been dominating the cathodes in commercial lithium‐ion batteries. In contrast to layered oxides and polyanion compounds, the development of spinel‐structured cathodes is a little behind. Owing to a series of advantageous properties, such as high operating voltage (≈4.7 V), high capacity (≈135 mAh g−1), low environmental impact, and low fabrication cost, the high‐voltage spinel LiNi0.5Mn1.5O4 represents a high‐power cathode for advancing high‐energy‐density Li+‐ion batteries. However, the wide application and commercialization of this cathode are hampered by its poor cycling performance. Recent progress in both the fundamental understanding of the degradation mechanism and the exploration of strategies to enhance the cycling stability of high‐voltage spinel cathodes have drawn continuous attention toward this promising insertion cathode. In this review article, the structure–property correlations and the failure mode of high‐voltage spinel cathodes are first discussed. Then, the recent advances in mitigating the cycling stability issue of high‐voltage spinel cathodes are summarized, including the various approaches of structural design, doping, surface coating, and electrolyte modification. Finally, future perspectives and research directions are put forward, aiming at providing insightful information for the development of practical high‐voltage spinel cathodes.

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Section: Fundamentals Of High‐voltage Spinel Lnmo Cathodes: Crystal Chemistry/structure Characterization and Electrochemical Mechanismmentioning

confidence: 99%

Advances and Prospects of High‐Voltage Spinel Cathodes for Lithium‐Based Batteries

Manthiram

2021

Small Methods

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“…[ 9–12 ] Most carbon materials are generally favored due to their remarkable conductivity and low cost, but their capacities are relatively low (<300 mAh g −1 ). [ 13–15 ] Alloying‐type materials normally have high capacity, but they suffer from huge volume changes and pulverization during the cycling process. Organic materials usually suffer from low electric/ionic conductivity and dissolution in the electrolyte, inevitably leading to low Coulombic efficiency (CE) and poor rate capabilities.…”

Section: Introductionmentioning

confidence: 99%

Phase Engineering of Nickel Sulfides to Boost Sodium‐ and Potassium‐Ion Storage Performance

Liu

Rehman

et al. 2021

Adv Funct Materials

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Sulfides are promising anode candidates because of their relatively large theoretical discharge/charge specific capacity and pretty small volume changes, but suffers from sluggish kinetics and structural instability upon cycling. Phase engineering can be designed to overcome the weakness of the electrochemical performance of sulfide anodes. By choosing nickel sulfides (α‐NiS, β‐NiS, and NiS2) supported by reduced graphene oxide (rGO) as model systems, it is demonstrated that the nickel sulfides with different crystal structures show different performances in both sodium‐ion and potassium‐ion batteries. In particular, the α‐NiS/rGO display superior stable capacity (≈426 mAh g−1 for 500 cycles at 500 mA g−1) and exceptional rate capability (315 mAh g−1 at 2000 mA g−1). The combined density functional theory calculations and experimental studies reveal that the hexagonal structure is more conducive to ion absorption and conduction, a higher pseudocapacitive contribution, and higher mechanical ability to relieve the stress caused by the volume changes. Correspondingly, the phase engineered nickel sulfide coupled with the conducting rGO network synergistically boosts the electrochemical performance of batteries. This work sheds light on the use of phase engineering as an essential strategy for exploring materials with satisfactory electrochemical performance for sodium‐ion and potassium‐ion batteries.

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“…The room-temperature sodium-sulfur (RT Na-S) batteries as emerging energy system are arousing tremendous interest [1][2][3][4][5][6][7]. Compared to other energy devices, RT Na-S batteries are featured with high theoretical energy density (1274 Wh kg −1 ) and the abundance of sulfur and sodium resources [8][9][10][11][12][13][14][15][16]. However, two main problems are important for the development of the RT Na-S batteries in comparison with Li-S batteries [17,18].…”

Section: Introductionmentioning

confidence: 99%

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

et al. 2021

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This work reports influence of two different electrolytes, carbonate ester and ether electrolytes, on the sulfur redox reactions in room-temperature Na–S batteries. Two sulfur cathodes with different S loading ratio and status are investigated. A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio (72% S). In contrast, a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio (44% S). In carbonate ester electrolyte, only the sulfur trapped in porous structures is active via ‘solid–solid’ behavior during cycling. The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents. To improve the capacity of the sulfur-rich cathode, ether electrolyte with NaNO3 additive is explored to realize a ‘solid–liquid’ sulfur redox process and confine the shuttle effect of the dissolved polysulfides. As a result, the sulfur-rich cathode achieved high reversible capacity (483 mAh g−1), corresponding to a specific energy of 362 Wh kg−1 after 200 cycles, shedding light on the use of ether electrolyte for high-loading sulfur cathode.

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Understanding Rechargeable Battery Function Using In Operando Neutron Powder Diffraction

Cited by 65 publications

References 119 publications

Advances and Prospects of High‐Voltage Spinel Cathodes for Lithium‐Based Batteries

Advances and Prospects of High‐Voltage Spinel Cathodes for Lithium‐Based Batteries

Phase Engineering of Nickel Sulfides to Boost Sodium‐ and Potassium‐Ion Storage Performance

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

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