Understanding Transformations in Battery Materials Using in Situ and Operando Experiments: Progress and Outlook

Boebinger, Matthew G.; Lewis, John A.; Sandoval, Stephanie; McDowell, Matthew T.

doi:10.1021/acsenergylett.9b02514

Cited by 91 publications

(78 citation statements)

References 107 publications

(181 reference statements)

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“…5,6 This process, commonly referred to as Li plating, is problematic for two reasons: 1) Li is known to deposit as dendrites, which can propagate across the separator and short the cell, and 2) Li metal plating/stripping is notoriously irreversible, either due to the highly reactive nature of Li with the battery electrolyte or because a large portion of the plated Li is electronically isolated upon stripping. 7,8,9,10 Thus, evaluating the onset and extent of Li plating is crucial for enabling XFC batteries.…”

Section: Introductionmentioning

confidence: 99%

Quantification of Inactive Lithium and Solid–Electrolyte Interphase Species on Graphite Electrodes after Fast Charging

et al. 2020

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Rapid charging of Li-ion batteries is limited by lithium plating on graphite anodes, whereby Li + ions are reduced to Li metal on the graphite particle surface instead of inserting between graphitic layers. Plated Li metal not only poses a safety risk due to dendrite formation, but also contributes to capacity loss due to the low reversibility of the Li plating/stripping process. Understanding when Li plating occurs and how much Li has plated is therefore vital to remedying these issues. We demonstrate a titration technique with a minimum detection limit of 20 nmol (5×10-4 mAh) Li which is used to quantify inactive Li that remains on the graphite electrode after fast charging. Additionally, the titration is extended to quantify the total amount of solid carbonate species and lithium acetylide (Li2C2) within the solid electrolyte interphase (SEI). Finally, electrochemical modeling is combined with experimental data to determine the Li plating exchange current density (10 A/m 2) and stripping efficiency (65%) of plated Li metal on graphite. These techniques provide a highly accurate measure of Li plating onset and quantitative insight into graphite SEI evolution during fast charge.

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Section: Introductionmentioning

confidence: 99%

Quantification of Inactive Lithium and Solid–Electrolyte Interphase Species on Graphite Electrodes after Fast Charging

et al. 2020

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“…Recently, tremendous progress has been made toward the development of advanced in situ characterization techniques, each of which has unique capabilities to study specific properties or progress. [ 15 ]…”

Section: In Situ and Operando Techniques Applied To 2d Model Energy Smentioning

confidence: 99%

“…Another element of research toward improving device performance is the real‐time observation of electrochemical processes, because this approach offers insights into the underlying charge storage and degradation mechanisms, and could also allow one to monitor structural changes of the materials and their interfaces upon operation. [ 15,16 ] The technique of choice is so‐called in situ and operando characterization, where “in situ” means “at the site of the electrode at work” and “operando” implies the experiments under true operating conditions. [ 17 ] Ex situ characterization is commonly used, but, to some extent, misses key information, because it is normally used after the electrochemical processes.…”

Section: Introductionmentioning

confidence: 99%

In Situ and Operando Characterizations of 2D Materials in Electrochemical Energy Storage Devices

et al. 2021

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The urgent need of modern society for portable energy‐consuming devices has boosted the development of high‐power supercapacitors and high‐energy batteries. Major prerequisites for augmenting wider practical applications are advanced electrode materials and deeper insights into the underlying electrochemical processes. Owing to their unique physicochemical properties, 2D materials, such as graphene, transition metal carbides, nitrides, and dichalcogenides, hold special promise. Characterizing their behavior under real operating conditions (operando) or at the site of operation (in situ) without disassembling the device helps uncover essential kinetic information, which may, otherwise, be lost. By identifying both harmful and beneficial mechanisms, these in situ and operando characterization techniques allow researchers to alleviate critical issues in existing materials and develop new materials with enhanced properties. Herein, a brief introduction including the preparation and the electrochemical energy storage application of 2D materials is first presented. The main concern, thereby, is the influence of preparation methods on the resulting electrode structure and electrochemical performance. Then, the electrochemical mechanisms underlying the operation of supercapacitors and lithium batteries are discussed in detail. Finally, the perspective and future direction of applying the in situ and operando techniques to model 2D materials in revealing some important processes are highlighted.

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“…However, practically realizing high reversible capacities faces the challenges of forming/decomposing large amounts of Li2O2 while suppressing parasitic reactions 2,[4][5][6][7] . These challenges are interrelated and require understanding the interplay between chemistry and morphological evolution [8][9][10][11][12][13] .…”

Section: Andmentioning

confidence: 99%

Exclusive solution discharge in Li-O2 batteries

Prehal

Samojlov²,

Nachtnebel³

et al. 2020

Preprint

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<b>Electrodepositing insulating and insoluble Li2O2 is the key process during discharge of aprotic Li-O2 batteries and determines rate, capacity, and reversibility. Current understanding states that the partition between surface adsorbed and solvated LiO2 governs whether Li2O2 grows as surface film or particles, leading to low or high capacities, respectively. Here we show that Li2O2 forms exclusively as particles via solution mediated LiO2 disproportionation. We describe a unified O2 reduction mechanism that conclusively explains capacity limitations across the whole range of electrolytes. Low-donor-number electrolytes are shown to accelerate disproportionation rather than slowing it down. Deciding for particle morphology and achievable capacities are species mobilities, true areal rate and the rate at which associated LiO2 forms in solution. Provided that species mobilities and surface are high, this allows for high capacities even with low-donor-number electrolytes, previously considered prototypical for low capacity via surface growth. The tools for these insights include microscopy, hydrodynamic voltammetry, a numerical reaction model, and in situ small/wide angle X-ray scattering (SAXS/WAXS). Combined with sophisticated data analysis, SAXS allows retrieving rich quantitative information from complex multi-phase systems. On a wider perspective, this SAXS method is a powerful in situ metrology with atomic to sub-micron resolution to study mechanisms in complex electrochemical systems and beyond.<br></b>

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Understanding Transformations in Battery Materials Using in Situ and Operando Experiments: Progress and Outlook

Cited by 91 publications

References 107 publications

Quantification of Inactive Lithium and Solid–Electrolyte Interphase Species on Graphite Electrodes after Fast Charging

Quantification of Inactive Lithium and Solid–Electrolyte Interphase Species on Graphite Electrodes after Fast Charging

In Situ and Operando Characterizations of 2D Materials in Electrochemical Energy Storage Devices

Exclusive solution discharge in Li-O2 batteries

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