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Article ; Online: Enabling selective zinc-ion intercalation by a eutectic electrolyte for practical anodeless zinc batteries.

Li, Chang / Kingsbury, Ryan / Thind, Arashdeep Singh / Shyamsunder, Abhinandan / Fister, Timothy T / Klie, Robert F / Persson, Kristin A / Nazar, Linda F

Nature communications

2023 Volume 14, Issue 1, Page(s) 3067

Abstract: Two major challenges hinder the advance of aqueous zinc metal batteries for sustainable stationary storage: (1) achieving predominant Zn-ion (de)intercalation at the oxide cathode by suppressing adventitious proton co-intercalation and dissolution, and ( ... ...

Abstract	Two major challenges hinder the advance of aqueous zinc metal batteries for sustainable stationary storage: (1) achieving predominant Zn-ion (de)intercalation at the oxide cathode by suppressing adventitious proton co-intercalation and dissolution, and (2) simultaneously overcoming Zn dendrite growth at the anode that triggers parasitic electrolyte reactions. Here, we reveal the competition between Zn
Language	English
Publishing date	2023-05-27
Publishing country	England
Document type	Journal Article
ZDB-ID	2553671-0
ISSN	2041-1723 ; 2041-1723
ISSN (online)	2041-1723
ISSN	2041-1723
DOI	10.1038/s41467-023-38460-2
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article: Unconventional Charge Transport in MgCr₂O₄ and Implications for Battery Intercalation Hosts

Johnson, Ian D. / Mistry, Aashutosh N. / Yin, Liang / Murphy, Megan / Wolfman, Mark / Fister, Timothy T. / Lapidus, Saul H. / Cabana, Jordi / Srinivasan, Venkat / Ingram, Brian J.

Journal of the American Chemical Society. 2022 July 27, v. 144, no. 31

2022

Abstract: Ion transport in solid-state cathode materials prescribes a fundamental limit to the rates batteries can operate; therefore, an accurate understanding of ion transport is a critical missing piece to enable new battery technologies, such as magnesium ... ...

Abstract	Ion transport in solid-state cathode materials prescribes a fundamental limit to the rates batteries can operate; therefore, an accurate understanding of ion transport is a critical missing piece to enable new battery technologies, such as magnesium batteries. Based on our conventional understanding of lithium-ion materials, MgCr₂O₄ is a promising magnesium-ion cathode material given its high capacity, high voltage against an Mg anode, and acceptable computed diffusion barriers. Electrochemical examinations of MgCr₂O₄, however, reveal significant energetic limitations. Motivated by these disparate observations; herein, we examine long-range ion transport by electrically polarizing dense pellets of MgCr₂O₄. Our conventional understanding of ion transport in battery cathode materials, e.g., Nernst–Einstein conduction, cannot explain the measured response since it neglects frictional interactions between mobile species and their nonideal free energies. We propose an extended theory that incorporates these interactions and reduces to the Nernst–Einstein conduction under dilute conditions. This theory describes the measured response, and we report the first study of long-range ion transport behavior in MgCr₂O₄. We conclusively show that the Mg chemical diffusivity is comparable to lithium-ion electrode materials, whereas the total conductivity is rate-limiting. Given these differences, energy storage in MgCr₂O₄ is limited by particle-scale voltage drops, unlike lithium-ion particles that are limited by concentration gradients. Future materials design efforts should consider the interspecies interactions described in this extended theory, particularly with respect to multivalent-ion systems and their resultant effects on continuum transport properties.
Keywords	anodes ; batteries ; cathodes ; diffusivity ; electric potential difference ; electrochemistry ; magnesium
Language	English
Dates of publication	2022-0727
Size	p. 14121-14131.
Publishing place	American Chemical Society
Document type	Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.2c03491
Database	NAL-Catalogue (AGRICOLA)

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Article: Understanding the Solid-State Electrode–Electrolyte Interface of a Model System Using First-Principles Statistical Mechanics and Thin-Film X-ray Characterization

Howard, Jason D. / Evmenenko, Guennadi / Kim, Jae Jin / Warburton, Robert E. / Patel, Shane / Fister, Timothy T. / Buchholz, D. Bruce / Greeley, Jeffrey / Curtiss, Larry A. / Fenter, Paul

ACS applied materials & interfaces. 2022 Jan. 28, v. 14, no. 5

2022

Abstract: Intermixing of atomic species at the electrode–electrolyte boundaries can impact the properties of the interfaces in solid-state batteries. Herein, this work uses first-principles statistical mechanics along with experimental characterization to ... ...

Abstract	Intermixing of atomic species at the electrode–electrolyte boundaries can impact the properties of the interfaces in solid-state batteries. Herein, this work uses first-principles statistical mechanics along with experimental characterization to understand intermixing at the electrode–electrolyte interface. For the model presented in this work, lithium manganese oxide (LiMn₂O₄, LMO) and lithium lanthanum titanate (Li₃ₓLa₂/₃–ₓTiO₃, LLTO) are employed as the cathode and electrolyte, respectively. The results of the computational work show that Ti–Mn intermixing at the interface is significant at synthesis temperatures. The experimental results in this work find that, at some critical temperatures between 600 and 700 °C for material preparation, the interface of LLTO–LMO becomes blurred. Calculations predict that the interface is unstable with regard to Ti–Mn intermixing starting at 0 K, suggesting that the critical temperature found in the experiment is related to kinetics. The work overall suggests that, in designing a solid-state battery, the fundamental reactions such as intermixing need to be considered.
Keywords	X-radiation ; batteries ; cathodes ; electrolytes ; lanthanum ; lithium ; manganese monoxide ; mechanics ; models ; temperature
Language	English
Dates of publication	2022-0128
Size	p. 7428-7439.
Publishing place	American Chemical Society
Document type	Article
ISSN	1944-8252
DOI	10.1021/acsami.1c20988
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Article ; Online: The evolution of solvation symmetry and composition in Zn halide aqueous solutions from dilute to extreme concentrations.

Dhakal, Diwash / Driscoll, Darren M / Govind, Niranjan / Stack, Andrew G / Rampal, Nikhil / Schenter, Gregory / Mundy, Christopher J / Fister, Timothy T / Fulton, John L / Balasubramanian, Mahalingam / Seidler, Gerald T

Physical chemistry chemical physics : PCCP

2023 Volume 25, Issue 34, Page(s) 22650–22661

Abstract: The emergence of cation-anion species, or contact ion pairs, is fundamental to understanding the physical properties of aqueous solutions when moving from the ideal, low-concentration limit to the manifestly non-ideal limits of very high solute ... ...

Abstract	The emergence of cation-anion species, or contact ion pairs, is fundamental to understanding the physical properties of aqueous solutions when moving from the ideal, low-concentration limit to the manifestly non-ideal limits of very high solute concentration or constituent ion activity. We focus here on Zn halide solutions both as a model system and also as an exemplar of the applications spanning from (i) electrical energy storage
Language	English
Publishing date	2023-08-30
Publishing country	England
Document type	Journal Article
ZDB-ID	1476244-4
ISSN	1463-9084 ; 1463-9076
ISSN (online)	1463-9084
ISSN	1463-9076
DOI	10.1039/d3cp01559a
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Article: Dual functionality of over-lithiated NMC for high energy silicon-based lithium-ion batteries

Dose, Wesley M / Kim, Soojeong / Liu, Qian / Trask, Stephen E / Dunlop, Alison R / Ren, Yang / Zhang, Zhengcheng / Fister, Timothy T / Johnson, Christopher S

Journal of materials chemistry A. 2021 June 1, v. 9, no. 21

2021

Abstract: Owing to their high specific capacity and suitably low operating potential, silicon-based anodes are an attractive alternative to graphite in next-generation lithium-ion batteries. However, silicon anodes suffer from low initial coulombic efficiency and ... ...

Abstract	Owing to their high specific capacity and suitably low operating potential, silicon-based anodes are an attractive alternative to graphite in next-generation lithium-ion batteries. However, silicon anodes suffer from low initial coulombic efficiency and fast capacity decay, limiting their widespread application. Pre-lithiation strategies are highly appealing to compensate for irreversible active lithium loss and to boost the cell energy density. In this work, we maximize the cell energy density by direct pre-lithiation of the NMC (LiNi₀.₅Mn₀.₃Co₀.₂O₂) cathode to Li₁₊ₓNMCO₂ without introducing inactive deadweight to either electrode. First, we demonstrate that Li₁₊ₓNMCO₂ can be synthesized chemically, via reaction between NMC and lithium napthalide, and electrochemically. The NMC cathode is tolerant of a one-time over-lithiation up to 60 mA h gNMC⁻¹, giving capacity retention on par with untreated NMC in half cell electrochemical cycling. Using synchrotron X-ray absorption spectroscopy (ex situ) and diffraction (in situ), we demonstrate that higher amounts of over-lithiation lead to local structure distortion – driven by transition metal reduction to Jahn–Teller active Mn³⁺ and Co²⁺ – as well as bulk structural hysteresis during over-lithiation and layer “buckling” that increases the amount of lithium extracted from the structure in the charged state. The Li₁₊ₓNMCO₂ with low-to-moderate over-lithiation capacity (23, 46, and 70 mA h gNMC⁻¹) is proven to be a highly effective dual-purpose lithium source and cathode material in full cell tests with a commercially relevant Si–graphite anode. These cells show higher capacity, superior cycle life, and improved coulombic efficiencies when compared to those with stoichiometric NMC cathodes. This study introduces a new and simple method to pre-lithiate layered transition metal oxide cathodes, opening up new possibilities for the development of high energy density lithium-ion batteries with next-generation anodes.
Keywords	X-ray absorption spectroscopy ; anodes ; cathodes ; electrochemistry ; energy ; energy density ; graphene ; hysteresis ; lithium ; silicon ; stoichiometry
Language	English
Dates of publication	2021-0601
Size	p. 12818-12829.
Publishing place	The Royal Society of Chemistry
Document type	Article
Note	NAL-AP-2-clean
ZDB-ID	2702232-8
ISSN	2050-7496 ; 2050-7488
ISSN (online)	2050-7496
ISSN	2050-7488
DOI	10.1039/d1ta01290h
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Article: Effect of Antisolvent Additives in Aqueous Zinc Sulfate Electrolytes for Zinc Metal Anodes: The Case of Acetonitrile.

Ilic, Stefan / Counihan, Michael J / Lavan, Sydney N / Yang, Yingjie / Jiang, Yinke / Dhakal, Diwash / Mars, Julian / Antonio, Emma N / Kitsu Iglesias, Luis / Fister, Timothy T / Zhang, Yong / Maginn, Edward J / Toney, Michael F / Klie, Robert F / Connell, Justin G / Tepavcevic, Sanja

ACS energy letters

2023 Volume 9, Issue 1, Page(s) 201–208

Abstract: Aqueous zinc-ion batteries (ZIBs) employing zinc metal anodes are gaining traction as batteries for moderate to long duration energy storage at scale. However, corrosion of the zinc metal anode through reaction with water limits battery efficiency. Much ... ...

Abstract	Aqueous zinc-ion batteries (ZIBs) employing zinc metal anodes are gaining traction as batteries for moderate to long duration energy storage at scale. However, corrosion of the zinc metal anode through reaction with water limits battery efficiency. Much research in the past few years has focused on additives that decrease hydrogen evolution, but the precise mechanisms by which this takes place are often understudied and remain unclear. In this work, we study the role of an acetonitrile antisolvent additive in improving the performance of aqueous ZnSO
Language	English
Publishing date	2023-12-20
Publishing country	United States
Document type	Journal Article
ISSN	2380-8195
ISSN	2380-8195
DOI	10.1021/acsenergylett.3c02504
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Article ; Online: Microwave-Assisted Synthesis of NaCoPO

Gutierrez, Arturo / Kim, Soojeong / Fister, Timothy T / Johnson, Christopher S

ACS applied materials & interfaces

2017 Volume 9, Issue 5, Page(s) 4391–4396

Abstract: Transition metal-containing polyanion compounds are attractive for use as cathode materials in sodium-ion batteries (SIB) because they possess elevated higher intrinsic electrochemical potentials versus oxide analogs given the same ... ...

Abstract	Transition metal-containing polyanion compounds are attractive for use as cathode materials in sodium-ion batteries (SIB) because they possess elevated higher intrinsic electrochemical potentials versus oxide analogs given the same M
Language	English
Publishing date	2017-02-08
Publishing country	United States
Document type	Journal Article
ISSN	1944-8252
ISSN (online)	1944-8252
DOI	10.1021/acsami.6b14341
Database	MEDical Literature Analysis and Retrieval System OnLINE

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Article ; Online: Investigation of Ca Insertion into α-MoO

Kim, Sanghyeon / Yin, Liang / Bak, Seong-Min / Fister, Timothy T / Park, Haesun / Parajuli, Prakash / Gim, Jihyeon / Yang, Zhenzhen / Klie, Robert F / Zapol, Peter / Du, Yonghua / Lapidus, Saul H / Vaughey, John T

Nano letters

2022 Volume 22, Issue 6, Page(s) 2228–2235

Abstract: Calcium-ion batteries (CIBs) are a promising alternative to lithium-ion batteries (LIBs) due to the low redox potential of calcium metal and high abundance of calcium compounds. Due to its layered structure, α- ... ...

Abstract	Calcium-ion batteries (CIBs) are a promising alternative to lithium-ion batteries (LIBs) due to the low redox potential of calcium metal and high abundance of calcium compounds. Due to its layered structure, α-MoO
MeSH term(s)	Calcium ; Electrodes ; Ions ; Lithium/chemistry ; Nanoparticles
Chemical Substances	Ions ; Lithium (9FN79X2M3F) ; Calcium (SY7Q814VUP)
Language	English
Publishing date	2022-03-02
Publishing country	United States
Document type	Journal Article ; Research Support, U.S. Gov't, Non-P.H.S.
ISSN	1530-6992
ISSN (online)	1530-6992
DOI	10.1021/acs.nanolett.1c04157
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Article ; Online: Structural Changes during the Conversion Reaction of Tungsten Oxide Electrodes with Tailored, Mesoscale Porosity.

Kim, Jae Jin / Zhou, Chun / Mane, Anil U / Suh, Hyo Seon / Kim, Soojeong / Shi, Bing / Fenter, Paul / Elam, Jeffrey W / Nealey, Paul F / Lee, Byeongdu / Fister, Timothy T

ACS nano

2022 Volume 16, Issue 4, Page(s) 5384–5392

Abstract: In-plane tungsten oxide nanostructures, including hexagonally patterned cylinders and holes in a matrix, were ... ...

Abstract	In-plane tungsten oxide nanostructures, including hexagonally patterned cylinders and holes in a matrix, were fabricated
Language	English
Publishing date	2022-03-31
Publishing country	United States
Document type	Journal Article
ISSN	1936-086X
ISSN (online)	1936-086X
DOI	10.1021/acsnano.1c08599
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Article ; Online: Unconventional Charge Transport in MgCr

Johnson, Ian D / Mistry, Aashutosh N / Yin, Liang / Murphy, Megan / Wolfman, Mark / Fister, Timothy T / Lapidus, Saul H / Cabana, Jordi / Srinivasan, Venkat / Ingram, Brian J

Journal of the American Chemical Society

2022 Volume 144, Issue 31, Page(s) 14121–14131

Abstract	Ion transport in solid-state cathode materials prescribes a fundamental limit to the rates batteries can operate; therefore, an accurate understanding of ion transport is a critical missing piece to enable new battery technologies, such as magnesium batteries. Based on our conventional understanding of lithium-ion materials, MgCr
Language	English
Publishing date	2022-07-27
Publishing country	United States
Document type	Journal Article
ZDB-ID	3155-0
ISSN	1520-5126 ; 0002-7863
ISSN (online)	1520-5126
ISSN	0002-7863
DOI	10.1021/jacs.2c03491
Database	MEDical Literature Analysis and Retrieval System OnLINE

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