Continuous transition from double-layer to Faradaic charge storage in confined electrolytes

Fleischmann, Simon; Zhang, Yuan; Wang, Xuepeng; Cummings, Peter T.; Wu, Jianzhong; Simon, Patrice; Gogotsi, Yury; Presser, Volker; Augustyn, Veronica

doi:10.1038/s41560-022-00993-z

Cited by 208 publications

(153 citation statements)

References 58 publications

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“…S7 and S8 †). 80 The obtained reduction and oxidation peaks from cyclic voltammetry agree with the galvanostatic discharge and charge proles tested at different specic currents in a voltage range between 0.1 and 2.0 V vs. Na + /Na as shown in Fig. 6A and B.…”

Section: Electrochemical Characterizationsupporting

confidence: 75%

Design of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries

Arnold

Gentile

et al. 2022

J. Mater. Chem. A

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Section: Electrochemical Characterizationsupporting

confidence: 75%

Design of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries

Arnold

Gentile

et al. 2022

J. Mater. Chem. A

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“…The study of Li plating/stripping kinetics on the investigated substrates was carried out through electrochemical approaches, where the powders of HMOs were coated on Cu foils to form the working electrodes [Supplementary Figure 3]. The voltage profiles of the initial Li electroplating were first assessed, where the Li nucleation overpotential can be revealed as the difference between the voltage dip and plateau [26] . At a current density of 1 mA cm -2 , a high Li nucleation overpotential of ~180 mV was achieved on bare Cu, which can result in unevenly distributed Li nuclei, followed by dendrite growth [Figure 3A].…”

Section: Resultsmentioning

confidence: 99%

Constructing stable lithium metal anodes using a lithium adsorbent with a high Mn3+/Mn4+ ratio

Zhao¹,

Liu²,

Li³

et al. 2022

Energy Mater

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Lithium (Li) metal batteries (LMBs) have emerged as the most prospective candidates for post-Li-ion batteries. However, the practical deployment of LMBs is frustrated by the notorious Li dendrite growth on hostless Li metal anodes. Herein, a protonated Li manganese (Mn) oxide with a high Mn3+/Mn4+ ratio is used as a Li adsorbent for constructing highly stable Li metal anodes. In addition to the Mn3+ sites with high Li affinity that afford an ultralow Li nucleation overpotential, the decrease in the average Mnn+ oxidation state also induces a disordered adsorbent structure via the Jahn-Teller effect, resulting in improved Li transfer kinetics with a significantly reduced Li electroplating overpotential. Based on the mutually improved Li diffusion and adsorption kinetics, the Li adsorbent is used as a versatile host to enable dendrite-free and stable Li metal anodes in LMBs. Consequently, a modified Li||LiNi0.8Mn0.1Co0.1O2 (NMC811) coin cell with a high NMC811 loading of 4.3 mAh cm-2 delivers a high Coulombic efficiency of 99.85% over 200 cycles and the modified Li||NMC811 pouch cell also achieves a remarkable improvement in electrochemical performance. This work demonstrates a novel approach for the preparation of highly efficient Li protection structures for safe LMBs with long lifespans.

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“…There is debate about the fundamental nature of these responses, [52,[54][55][56][57][58][59][60][61] including rigorous theoretical arguments that the first camp is attributed principally to EDLC [60] and a separate suggestion of a continuum between Faradaic and EDLC. [62] If indeed charge storage were dominated by EDLC, then the term pseudocapacitance [60] would be inaccurate. T-Nb 2 O 5 was the first material described as exhibiting intercalation pseudocapacitance.…”

Section: Rapid Intercalation Materials and Pseudocapacitancementioning

confidence: 99%

Understanding Rapid Intercalation Materials One Parameter at a Time

Bergh

Stefik

2022

Adv Funct Materials

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Demand for fast, energy‐dense storage drives the research into nanoscale intercalation materials. Nanomaterials accelerate kinetics and can modify reaction path thermodynamics, intercalant solubility, and reversibility. The discovery of intercalation pseudocapacitance has opened questions about their fundamental operating principles. For example, are their capacitor‐like current responses caused by storing energy in special near‐surface regions or rather is this response due to normal intercalation limited by a slower faradaic surface‐reaction? This review highlights emerging methods combining tailored nanomaterials with the process of elimination to disambiguate cause‐and‐effect at the nanoscale. This method is applied to multiple intercalation pseudocapacitive materials showing that the timescales exhibiting surface‐limited kinetics depended on the total intercalation length scale. These trends are inconsistent with the near‐surface perspective. A revised current‐model without assuming special near‐surface storage fits experimental data better across wide timescales. This model, combined with tailored nanomaterials and the process of elimination, can isolate material‐specific effects such as how amorphization/defect‐tailoring modifies both insertion and diffusion kinetics. Avenues for both faster intercalation pseudocapacitance and increased energy density are discussed. A relaxation time argument is suggested to explain the continuum between battery‐like and pseudocapacitive behaviors. Future directions include synthetic methods emphasizing tailored defects and analytical methods that minimize assumptions.

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Continuous transition from double-layer to Faradaic charge storage in confined electrolytes

Cited by 208 publications

References 58 publications

Design of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries

Design of high-performance antimony/MXene hybrid electrodes for sodium-ion batteries

Constructing stable lithium metal anodes using a lithium adsorbent with a high Mn3+/Mn4+ ratio

Understanding Rapid Intercalation Materials One Parameter at a Time

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