ORCID Profile
0000-0003-3850-0505
Current Organisation
Argonne National Laboratory
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Electrochemistry | Inorganic Chemistry | Solid State Chemistry
Expanding Knowledge in the Chemical Sciences | Energy Storage (excl. Hydrogen) |
Publisher: The Electrochemical Society
Date: 05-2020
DOI: 10.1149/MA2020-012218MTGABS
Abstract: Nickel-rich layered oxide cathode materials are promising candidates for automotive lithium-ion batteries due to their low cost and high reversible capacity. 1 However, paired with graphite anodes these materials exhibit faster voltage and capacity fading compared to isostructural LiNi x Mn y Co z O 2 (NMC) cathodes with lower nickel content. 2 In this work we will explore the origins of capacity fade and material degradation in graphite/LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) full cells. With a focus on strategically designed electrochemical protocols (see Fig. 1), the role of several key cycling parameters ( e.g. upper cut-off voltage, time at high voltage, phase transitions) on the degradation are decoupled. The ageing processes are quantified in terms of the full cell capacity retention, impedance rise, electrode slippage, and NMC cathode deterioration. We find that most full cell capacity loss and impedance rise is caused by increasing the upper cut-off voltage to .2 V, with the impedance increase largely driven by concomitant full state-of-charge (SOC) cycling. Time spent at high voltage (voltage holds) has less impact on these parameters. These findings are supported by electron microscopy and spectroscopy experiments (SEM, high-resolution TEM, and STEM-EELS) on cycled electrodes, which show clear evidence for cycle history dependent degradation including particle cracking, shearing, and surface reconstruction. References 1. Schipper, E. M. Erickson, C. Erk, J.-Y. Shin, F. F. Chesneau, and D. Aurbach, J. Electrochem. Soc., 164, A6220, 2017. 2. Jung, M. Metzger, F. Maglia, C. Stinner, H. A. Gasteiger, J. Electrochem. Soc., 164, A1361, 2017. Figure 1
Publisher: Elsevier BV
Date: 02-2014
Publisher: Wiley
Date: 17-06-2022
Abstract: Operando electrochemical transmission electron microscopy (ec‐TEM) is a promising tool for advanced characterization of energy systems close to their operating conditions. However, reliable s le preparation for the technique is particularly challenging due to spatial constraints. Here, a novel approach of manufacturing such s les is introduced and demonstrated for industrially relevant battery powders: NMC811 and LTO (LiNi 0.8 Mn 0.1 Co 0.1 O 2 and Li 4 Ti 5 O 12 ). Aerosol‐jet printing is used to deposit microscale patterns of battery active material particles on the electrodes of commercial ec‐TEM chips. This method provides high spatial resolution (line width 30 µm) and accuracy, ease of ink preparation, flexibility of materials, and ability to manufacture complex structures (layered or mixed materials). Size selectivity of aerosol jet printing and its positive implications for ec‐TEM s le preparation are also discussed. This procedure is a promising solution to the difficult problem of micro‐battery fabrication for ec‐TEM and for other applications where high spatial resolution deposition from powders is required.
Publisher: The Electrochemical Society
Date: 2018
DOI: 10.1149/2.1271810JES
Publisher: IEEE
Date: 07-2020
Publisher: AIP Publishing
Date: 04-2022
DOI: 10.1063/5.0084105
Abstract: The lithium-ion cathode material olivine LiFePO4 (LFP) has been synthesized for the first time from natural paleozoic iron carbonate (FeCO3). The ferrous carbonate starting material consists of the mineral siderite at about 92 wt. % purity. Because FeCO3 has alent iron, the reaction with lithium dihydrogen phosphate (LiH2PO4) provides a unique method to develop iron-(II) containing LFP in an inert atmosphere. Since siderite FeCO3 is a common mineral that can be directly mined, it may, therefore, provide an inexpensive route for the production of LFP. After carbon-coating, the LFP yields a capacity in the range of 80–110 mAh g−1LFP (in one chosen specimen s le), which is lower than commercially available LiFePO4 (150–160 mAh g−1LFP). However, the tap density of LFP derived from siderite is noticeably high at 1.65 g cm−3. The material is likely to be improved with powder purification, nanosized processing, and more complete carbon-coating coverage with increased optimization.
Publisher: Elsevier BV
Date: 04-2017
Publisher: Springer Science and Business Media LLC
Date: 04-11-2015
DOI: 10.1557/JMR.2014.311
Publisher: Elsevier BV
Date: 08-2013
Publisher: The Electrochemical Society
Date: 2011
DOI: 10.1149/1.3611013
Publisher: Elsevier BV
Date: 07-2012
Publisher: Elsevier BV
Date: 10-2018
Publisher: American Chemical Society (ACS)
Date: 02-10-2018
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C7EE02995K
Abstract: A detailed investigation on the effects of Mg substitution (0 ≤ x ≤ 0.2) in high voltage P2-Na 2/3 Ni 1/3−x Mg x Mn 2/3 O 2 cathode materials for Na-ion batteries.
Publisher: Springer Science and Business Media LLC
Date: 24-03-2011
Publisher: The Electrochemical Society
Date: 2013
DOI: 10.1149/2.005309JES
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2TA04876K
Abstract: Surface reduction leads to voltage decay in extended cycling of Li - and Mn-rich layered oxides (Li 1.2 Ni 0.2 Mn 0.6 O 2 ).
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA06324C
Abstract: Tailored electrochemical protocols and characterisation methods provide a detailed account of degradation mechanisms in high energy lithium-ion batteries with nickel-rich cathodes.
Publisher: Elsevier BV
Date: 09-2011
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1TA01290H
Abstract: Over lithiated Li 1+x NMCO 2 is introduced as a dual-functional lithium source and cathode material to increase the lithium inventory and significantly improve the energy density and cycle life of lithium-ion batteries with a Si-based anode.
Publisher: American Chemical Society (ACS)
Date: 13-10-2014
DOI: 10.1021/JP506914J
Publisher: American Chemical Society (ACS)
Date: 30-08-2016
Publisher: The Electrochemical Society
Date: 12-2020
Abstract: The energy density of lithium-ion batteries can be increased by replacing the traditional graphite anode with a high capacity silicon anode. However, volume changes and interfacial instabilities cause a large irreversible capacity and a continual loss of lithium during cycling, which lead to rapid capacity loss. In this work, we add Li 5 FeO 4 (LFO) to a LiNi 0.5 Mn 0.3 Co 0.2 O 2 (NMC) cathode as a pre-lithiation additive, which increases the lithium inventory and extends the cycle life of Si-graphite/NMC full cells, and decreases the NMC particle degradation. LFO delivers a large 764 mAh g −1 LFO capacity below 4.7 V vs Li/Li + . By tuning the LFO content in Si-graphite/LFO-NMC full cells, we show higher capacity, improved retention, lower impedance, and superior rate performance compared to full cells without LFO. Post-test characterizations demonstrate that LFO inclusion in the cathode matrix leads to less NMC secondary particle segregation/cracking and a thinner surface reduced layer on the NMC particles. The beneficial effects of LFO endure after the lithium reserve has been exhausted, highlighting a lasting synergy between the lithium source and electrode active materials. This study introduces a new approach to simultaneously increase lithium inventory and reduce cathode degradation, and makes critical advances toward enabling Si anodes for lithium-ion batteries.
Publisher: American Chemical Society (ACS)
Date: 06-09-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2022
DOI: 10.1039/D2EE01754G
Abstract: Elucidating and quantifying the effects of doping on halide perovskites using lithium ion batteries.
Publisher: Springer Science and Business Media LLC
Date: 30-10-2019
DOI: 10.1038/S41467-019-12863-6
Abstract: Due to their exceptional high energy density, lithium-ion batteries are of central importance in many modern electrical devices. A serious limitation, however, is the slow charging rate used to obtain the full capacity. Thus far, there have been no ways to increase the charging rate without losses in energy density and electrochemical performance. Here we show that the charging rate of a cathode can be dramatically increased via interaction with white light. We find that a direct exposure of light to an operating LiMn 2 O 4 cathode during charging leads to a remarkable lowering of the battery charging time by a factor of two or more. This enhancement is enabled by the induction of a microsecond long-lived charge separated state, consisting of Mn 4+ (hole) plus electron. This results in more oxidized metal centers and ejected lithium ions are created under light and with voltage bias. We anticipate that this discovery could pave the way to the development of new fast recharging battery technologies.
Publisher: Elsevier BV
Date: 11-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2018
DOI: 10.1039/C8CC00456K
Abstract: A silicon-graphite blended anode is paired with a high capacity LiFePO 4 reference/counter electrode to track irreversibility and lithium inventory.
Publisher: Research Square Platform LLC
Date: 05-10-2023
Publisher: Elsevier BV
Date: 2013
Publisher: American Chemical Society (ACS)
Date: 08-03-2022
Publisher: American Chemical Society (ACS)
Date: 15-08-2017
Publisher: American Chemical Society (ACS)
Date: 22-09-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0MA00601G
Abstract: The ammonium counter ion is shown to influence the morphology, physicochemical properties and electrochemical performance of hydrothermal carbon.
Publisher: Elsevier BV
Date: 05-2020
Publisher: Springer Science and Business Media LLC
Date: 28-03-2022
DOI: 10.1038/S41467-022-29330-4
Abstract: 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 LiNi 0.8 Mn 0.1 Co 0.1 O 2 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.
Publisher: Elsevier BV
Date: 03-2018
Publisher: The Electrochemical Society
Date: 2011
DOI: 10.1149/1.3597640
Publisher: Elsevier BV
Date: 04-2021
Publisher: Wiley
Date: 28-09-2021
Abstract: Due to their ersity in the composition, lattice structures and physical/chemical properties, and various oxidation states (2+, 3+, 4+, and 5+), (V x O y ) nanomaterials have attached much attention for developing new rechargeable batteries, including lithium‐ion batteries (LIBs), sodium‐ion batteries (NIBs), zinc‐ion batteries (ZIBs), and magnesium‐ion batteries (MIBs) as well as new energy storage concepts such as light‐rechargeable batteries. However, to further improve the electrochemical performance of V x O y ‐based batteries, it is crucial to understand the various electrochemical mechanisms taking place in these materials for LIBs, NIBs, ZIBs, and MIBs. This review covers a systematical discussion of in situ and operando analysis methods carried out on V 2 O 5 , VO 2 , Li x V y O z , Na x V y O z , Zn x V y O z , and Mg x V y O z for LIBs, NIBs, ZIBs, and MIBs and the fundamental insights they have provided in the energy storage mechanisms in these batteries.
Publisher: The Electrochemical Society
Date: 2012
DOI: 10.1149/2.115206JES
Publisher: International Union of Crystallography (IUCr)
Date: 03-08-2013
DOI: 10.1107/S0021889813017846
Abstract: High-temperature in situ X-ray diffraction is used to determine the thermal expansion behaviour of manganese dioxide in air at temperatures between 298 and 673 K, the range accessible prior to material decomposition. Two manganese dioxide s les of different origins are investigated to observe the effect of synthesis conditions and resultant material properties on the thermal response. β-MnO 2 prepared by a chemical pathway is found to expand linearly over the temperature window with thermal expansion coefficients (in units of K −1 ) of α a = 9.3 (4) × 10 −6 , α c = 7.0 (2) × 10 −6 and β = 25.6 (8) × 10 −6 . Conversely, the thermal expansion of heat-treated electrolytic manganese dioxide is disjointed about 473 K in the a direction and for the overall unit-cell volume, and about 523 K in the c direction. Coefficients are therefore given (in units of K −1 ) as α a = 23 (4) × 10 −6 (298–473 K), 10 (3) × 10 −6 (473–673 K) α c = 0.2 (9) × 10 −6 (298–523 K), 10 (1) × 10 −6 (523–673 K) and β = 49 (9) × 10 −6 (298–473 K), 26 (5) × 10 −6 (473–673 K).
Publisher: American Chemical Society (ACS)
Date: 21-06-2019
Publisher: American Chemical Society (ACS)
Date: 12-10-2023
Publisher: Elsevier BV
Date: 02-2022
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3TA00912B
Abstract: Half-cell studies are widely employed to assess the performance of prospective positive electrode chemistries. In this study, we explore the failure mechanism of Li-NMC811 half-cells and propose an alternative cell chemistry for isolated, long-term positive electrode testing.
Publisher: American Chemical Society (ACS)
Date: 16-12-2021
DOI: 10.26434/CHEMRXIV-2021-XNJRT
Abstract: 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 poorly understood mechanisms. Here, we study the role of the electrolyte solvent, specifically cyclic ethylene carbonate (EC) and linear ethyl methyl carbonate (EMC), in determining the interfacial reactivity at LiNi0.33Mn0.33Co0.33O2 (NMC111) and LiNi0.8Mn0.1Co0.1O2 (NMC811). Parasitic currents are measured during high voltage holds in NMC/Li4Ti5O12 (LTO) cells, LTO avoiding parasitic currents related to anode-cathode reduction species cross-over, and are found to be higher for EC-containing vs. EC-free electrolytes with NMC811. No difference between electrolytes are observed with NMC111. On-line gas analysis reveals this to be related to lattice oxygen release, and accompanying electrolyte decomposition, which increases substantially with greater Ni content, and for EC-containing electrolytes with NMC811. This is corroborated by electrochemical impedance spectroscopy (EIS) and transmission electron microscopy (TEM) of NMC811 after the voltage hold, which show a higher interfacial impedance and a thicker oxygen-deficient rock-salt surface reconstruction layer, respectively. Combined findings from solution NMR, ICP (of electrolytes) and XPS analysis (of electrodes) reveal that higher lattice oxygen release from NMC811 in EC-containing electrolytes is coupled with more electrolyte breakdown and higher amounts of transition metal dissolution compared to EC-free electrolyte. Finally, new mechanistic insights for 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.
Publisher: The Electrochemical Society
Date: 2019
DOI: 10.1149/2.1541910JES
Publisher: American Chemical Society (ACS)
Date: 31-05-2022
DOI: 10.26434/CHEMRXIV-2022-XXTL8
Abstract: 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 similar extents 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.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1MA00020A
Abstract: The electrochemical performance of 2-dimensional hybrid perovskite electrodes for Li-ion batteries are investigated using a high-molarity electrolyte. The effect of changing the halide content and layering structure is systematically explored.
Publisher: American Chemical Society (ACS)
Date: 18-02-2022
Publisher: The Electrochemical Society
Date: 2015
DOI: 10.1149/2.1031508JES
Publisher: American Chemical Society (ACS)
Date: 06-09-2018
Publisher: Wiley
Date: 24-02-2022
Abstract: Lithium‐metal anodes (LMAs) are desirable for next‐generation rechargeable batteries because of their high energy density. However, in practical applications they are hindered by inhomogeneous and uncontrolled lithium‐dendrite deposition during cycling. Herein, we propose a dual charge storage mechanism, using freestanding carbon‐fiber paper (CFP) with carbon fillers electrode. These CFP electrodes are manufactured at an industrial scale and act both as a host for lithium (Li) intercalation and as a conductive and porous 3D scaffold for Li plating/stripping. The CFP electrode exhibits excellent long‐term cycling stability, as evidenced by Coulombic efficiencies of over 99.5 % on the 250 th cycle in CFP|Li half‐cells with a lithiation capacity of 1.5 mA h cm −2 and current density of 0.5 mA cm −2 . We also demonstrate that the CFPs are sufficiently electrically conductive to operate in small pouch cells without metal foil current collectors, further improving the energy density of the proposed electrodes.
Publisher: Elsevier BV
Date: 08-2014
Publisher: Elsevier BV
Date: 07-2014
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0EE01392G
Abstract: This paper presents a zinc-ion battery that can be recharged directly by light without the need for a solar cell, which offers a new approach to balancing the unpredictable energy surpluses and deficits associated with solar energy.
Start Date: 12-2022
End Date: 04-2026
Amount: $450,000.00
Funder: Australian Research Council
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