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2. Temperature-Dependent Dynamic Disproportionation in LiNiO$_2$

Author

Poletayev, Andrey D., Green, Robert J., Swallow, Jack E. N., An, Lijin, Jones, Leanne, Harris, Grant, Bencok, Peter, Sutarto, Ronny, Cottom, Jonathon P., Morgan, Benjamin J., House, Robert A., Weatherup, Robert S., and Islam, M. Saiful

Subjects
Condensed Matter - Materials Science
Abstract

Nickelate materials offer diverse functionalities for energy and computing applications. Lithium nickel oxide (LiNiO$_2$) is an archetypal layered nickelate, but the electronic structure of this correlated material is not yet fully understood. Here we investigate the temperature-dependent speciation and spin dynamics of Ni ions in LiNiO$_2$. Our ab initio simulations predict that Ni ions disproportionate into three states, which dynamically interconvert and whose populations vary with temperature. These predictions are verified using x-ray absorption spectroscopy, x-ray magnetic circular dichroism, and resonant inelastic x-ray scattering at the Ni L$_{3,2}$-edge. Charge-transfer multiplet calculations consistent with disproportionation reproduce all experimental features. Together, our experimental and computational results support a model of dynamic disproportionation that explains diverse physical observations of LiNiO$_2$, including magnetometry, thermally activated electronic conduction, diffractometry, core-level spectroscopies, and the stability of ubiquitous antisite defects. This unified understanding of the fundamental material properties of LiNiO$_2$ is important for applications of nickelate materials as battery cathodes, catalysts, and superconductors., Comment: 30 pages, 16 figures

Published
2022

3. Factors affecting capacity and voltage fading in disordered rocksalt cathodes for lithium-ion batteries

Author

Pi, Liquan, Björklund, Erik, Rees, Gregory J., Song, Weixin, Gong, Chen, Marie, John-Joseph, Gao, Xiangwen, Pu, Shengda D., Juelsholt, Mikkel, Chater, Philip A., Park, Joohyuk, Kim, Min Gyu, Choi, Jaewon, Agrestini, Stefano, Garcia-Fernandez, Mirian, Zhou, Ke-Jin, Robertson, Alex W., Weatherup, Robert S., House, Robert A., and Bruce, Peter G.

Published
2025
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7. Not So Fast Fifth Circuit - Louisiana Supreme Court Reaffirms Statutory Prohibition On Insurance Policy Arbitration Clauses

Author

House, Robert

Subjects
Louisiana. Supreme Court -- Powers and duties, Commercial arbitration agreements -- Cases -- Laws, regulations and rules, Insurance policies -- Cases -- Laws, regulations and rules, Company legal issue, Government regulation, Business, international
Abstract

On October 25, 2024, the Louisiana Supreme Court issued its opinion in Police Jury of Calcasieu Parish v. Indian Harbor Insurance Co., et al., No. 2024-CQ-00449, answering three questions regarding [...]

Published
2024

8. Low- and Very Low-Dose Bevacizumab for Retinopathy of Prematurity: Reactivations, Additional Treatments, and 12-Month Outcomes

Author

Freedman, Sharon F., Prakalapakorn, Sasapin G., Wallace, David K., Jones, Sarah K., Barman, Navajyoti R., House, Robert J., Nasrazadani, David A., Crouch, Eric, Crouch, Earl R., Jr., Ventura, Gaylord G., Yang, Michael B., Dosunmu, Eniolami O., Gray, Michael E., Motley, William W., Castleberry, Katherine, Cobb, Patricia, Hirsch, Patricia, Reed, Melissa, Sandoval, Monica A., Vallabh, Neil, Rogers, David L., Bremer, Don.L., Golden, Richard P., Jordan, Catherine O., McGregor, Mary Lou, Reem, Rachel E., Schreckengost, Amanda N., Maletic, Sara A., Miller, Rachel T., Bhatt, Amit R., Coats, David K., Romany, Gihan, Demmy, Ann B., Kong, Lingkun X., Hartnett, Mary E., Dries, David C., Hoffman, Robert O., Allman, Susan, Farnsworth, Katie J., Hart, Barbara, Ordonez, Kelliann, Hutchinson, Amy K., Hubbard, George B., III, Rao, Prethy, Robinson, Joshua E., Brower, Judy L., Haider, Kathryn M., Boente, Charline S., Smith, Heather A., Hynes, Elizabeth A., Whitaker, Michele E., VanderVeen, Deborah K., Mantagos, Jason S., Wu, Carolyn, Goldstein, Samantha, Winter, Tamar, Yoon, Grace X., Siatkowski, R. Michael, Collinge, Janine E., Satnes, Kelli J., Blunt, Michelle H., Repka, Michael X., Kraus, Courtney, Shepard, Jennifer A., Kraker, Raymond T., Beck, Roy W., Austin, Darrell S., Boyle, Nicole M., Chandler, Danielle L., Connelly, Patricia L., Conner, Courtney L., Donahue, Quayleen, Fimbel, Brooke P., Henderson, Robert J., Hercinovic, Amra, Hoepner, James E., Kaplon, Joseph D., Li, Zhuokai, Melia, B. Michele, Ortiz, Gillaine, Robinson, Julianne L., Stutz, Kathleen M., Sutherland, Desirae R., Toro, David O., Woodard, Victoria C., Wu, Rui, Cotter, Susan A., Holmes, Jonathan M., Birch, Eileen E., Chen, Angela M., Christiansen, Stephen P., Crouch, Eric R., III, Enyedi, Laura B., Erzurum, S. Ayse, Everett, Donald F., Good, William V., Jenewein, Erin C., Lee, Katherine A., London, Richard, Manh, Vivian M., Manny, Ruth E., Morrell, Beth A., Morrison, David G., Petersen, David B., Pineles, Stacy L., Ranaivo, Hantamalala Ralay, Roberts, Tawna L., Ruark, Scott T., Schweinler, Bonita R., Silver, Jayne L., Suh, Donny W., Summers, Allison I., Verderber, Lisa C., Weise, Katherine K., Diener-West, Marie, Baker, John D., Davis, Barry, Phelps, Dale L., Poff, Stephen W., Saunders, Richard A., Tychsen, Lawrence, Crouch, Eric R., Hubbard, G. Baker, VanderVeen, Deborah, and Cheung, Nathan L.

Published
2022
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9. The Pediatric Optic Neuritis Prospective Outcomes Study: Two-Year Results

Author

Borchert, Mark S., Chang, Melinda Y., Contractor, Dilshad, Zolfaghari, Emily J., Vyas, Aarti, Yuen, Tiffany, Shah, Veeral S., Paysse, Evelyn A., Romany, Gihan, Peragallo, Jason H., Brower, Judy L., Raghuram, Aparna, Heidary, Gena, Al Wattar, Bilal, Chinn, Ryan, Kothari, Srishti, Siatkowski, R. Michael, Collinge, Janine E., Lim, Maria E., Brewer, Alisha N., Doughty, Annette M., Icks, Sonny W., Almeida, Shannon, de Alba Campomanes, Alejandra, Banwait, Premilla, Graves, Jennifer S., Hajkazemshirazi, Leila, Bastea-Forte, Yizhuo, Arjona, Jennifer K., Chen, Jeremy, Cooper, Karen, Ghadban, Rafif, Chung, Sophia M., Cruz, Oscar A., Khanna, Sangeeta, Christenson, Traci A., Breeding, Lisa L., Govreau, Dawn M., Wallis, Beth A., Geddie, Brooke E., Conley, Julie A., Wolinski, Elisabeth T., Davis, Patricia L., Rudaitis, Indre M., Twite, Jacqueline, Bloomquist, Carrie S., Laboy, Sarah R., Twite, Jackie M., Pineles, Stacy L., Doan, Michelle V., Bernardo, Marianne J., Brodsky, Michael C., Chen, John J., Holmes, Jonathan M., Wernimont, Suzanne M., Czaplewski, Lindsay L., Eastman, Stacy L., Keehn, Moriah A., Priebe, Debbie M., Bremer, Don L., Golden, Richard P., Jordan, Catherine O., McGregor, Mary Lou, Reem, Rachel E., Rogers, David L., Schreckengost, Amanda N., Maletic, Sara A., Dairi, Mays A., Enyedi, Laura B., Jones, Sarah K., Barman, Navajyoti R., House, Robert J., Nasrazadani, David A., Gratton, Sean M., Marsh, Justin D., Dent, Rebecca J., Bond, Lezlie L., Soske, Lori L., Sudhakar, Padmaja, Willen, Christi M., Taylor, Deborah, Moliterno, Nathaniel Q., Nsoesie, Michael, Vally, Shaista, Phillips, Paul H., Lowery, Robert S., Colon, Beth, Stotts, Nancy L., To, Kelly D., McClelland, Collin M., Areaux, Raymond G., Holleschau, Ann M., Merrill, Kim S., Ospina, Luis H., Superstein, Rosanne, Thibeault, Maryse, Gagnon, Helene, Donahue, Sean P., Ruark, Scott T., Fraine, Lisa A., Sprouse, Petrice A., Biernacki, Ronald J., Liu, Grant T., Avery, Robert A., Forbes, Brian J., Jivraj, Imran, Kohli, Anita A., Richter, Meg M., Baumritter, Agnieshka, Mitchell, Ellen B., Nischal, Ken K., Runkel, Lauren M., Blaha, Bianca, Churchfield, Whitney, Fulwylie, Christina, Ko, Melissa W., Mejico, Luis J., Iqbal, Muhammad, Attanasio, Catherine E., Deb, Lena F., Goodrich, Courtney B., Hartwell, Alisha M., Moore, Jennifer A., Bohra, Lisa, Apkarian, Alexandra O., Gianfermi, Elena M., Roarty, John D., Rotberg, Leemor B., Perzyk, Susan N., Kraker, Raymond T., Beck, Roy W., Austin, Darrell S., Boyle, Nicole M., Chandler, Danielle L., Connelly, Patricia L., Conner, Courtney L., Dean, Trevano W., Donahue, Quayleen, Fimbel, Brooke P., Henderson, Robert J., Hercinovic, Amra, Hoepner, James E., Kaplon, Joseph D., Li, Zhuokai, Ortiz, Gillaine, Robinson, Julianne L., Stutz, Kathleen M., Toro, David O., Woodard, Victoria C., Wu, Rui, Repka, Michael X., Balcer, Laura, Kupersmith, Mark, Lazar, Elizabeth L., Waldman, Amy, Wallace, David K., Cotter, Susan A., Birch, Eileen E., Chen, Angela M., Christiansen, Stephen P., Erzurum, S. Ayse, Everett, Donald F., Freedman, Sharon F., Good, William V., Lee, Katherine A., London, Richard, Manh, Vivian M., Manny, Ruth E., Morrison, David G., Schweinler, Bonita R., Silver, Jayne L., Verderber, Lisa C., Weise, Katherine K., Green, Ari, Diener-West, Marie, Baker, John D., Davis, Barry, Phelps, Dale L., Poff, Stephen W., Saunders, Richard A., Tychsen, Lawrence, and Waldman, Amy T.

Published
2022
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10. Optimisation of a P3 phase with superior high voltage reversibility.

Author

Linnell, Stephanie F., Choi, Yong-Seok, Liao, Yingling, Pateli, Ioanna M., Naden, Aaron B., Irvine, John T. S., House, Robert A., Scanlon, David O., and Armstrong, A. Robert

Abstract

Activation of oxygen anion redox represents an effective method of increasing the specific capacity as well as raising the operating voltage of layered sodium transition metal oxides. However, these reactions are often accompanied by irreversible structural transformations and detrimental side-reactions between the electrolyte and electrode interface which accelerate degradation, thereby impeding their practical application. To optimise the oxygen anion reversibility for practical use and compare the effects of dopants, we investigated Zn- and Ti-substitution both separately and combined in P3-structure Na0.7Mn0.75Ni0.25O2, assisted by DFT calculations. The Zn-substituted materials, Na0.7Mn0.65Ni0.25Zn0.1O2 and Na0.7Mn0.58Ni0.25Zn0.07Ti0.1O2 present superior cycling stability over the high voltage range 3.8–4.3 V and enhanced rate capability, delivering a reversible capacity of ∼80 mA h g−1 at 500 mA g−1 over the voltage window 2.2–4.3 V compared with 58.6 mA h g−1 for the parent-phase. The improved electrochemical performance of the Zn-substituted materials is attributed to suppression of the P3 to O′3 phase transformation revealed by X-ray diffraction and the lower electronegativity and filled d-band of Zn. The presence of TiO6 octahedra in the Ti-substituted materials relieves structural distortions/TM ordering, also improving the cycling stability. With Zn/Ti co-substitution these advantages may be combined, as demonstrated by the superior electrochemical performance observed for Na0.7Mn0.58Ni0.25Zn0.07Ti0.1O2. [ABSTRACT FROM AUTHOR]

Published
2025
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13. A combination of two human neutralizing antibodies prevents SARS-CoV-2 infection in cynomolgus macaques

Author

Cobb, Ronald R., Nkolola, Joseph, Gilchuk, Pavlo, Chandrashekar, Abishek, Yu, Jingyou, House, Robert V., Earnhart, Christopher G., Dorsey, Nicole M., Hopkins, Svetlana A., Snow, Doris M., Chen, Rita E., VanBlargan, Laura A., Hechenblaickner, Manuel, Hoppe, Brian, Collins, Laura, Tomic, Milan T., Nonet, Genevieve H., Hackett, Kyal, Slaughter, James C., Lewis, Mark G., Andersen, Hanne, Cook, Anthony, Diamond, Michael S., Carnahan, Robert H., Barouch, Dan H., and Crowe, James E., Jr.

Published
2022
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16. Reversible Electron–Holes on O in P2‐type Na0.67Li0.1Ni0.3Mn0.6O2.

Author

Marie, John‐Joseph, Jenkins, Max, Chen, Jun, Rees, Gregory, Cellorio, Veronica, Choi, Jaewon, Agrestini, Stefano, Garcia‐Fernandez, Mirian, Zhou, Ke‐Jin, House, Robert A., and Bruce, Peter G.

Subjects
ENERGY density, HIGH voltages, TRANSITION metals, CATHODES, HONEYCOMB structures
Abstract

Achieving reversible O‐redox through the formation of electron–holes on O could hold the key to a new generation of high energy density Na‐ion cathodes. However, to date, it has only been demonstrated in a small handful of cathode materials and none of these materials exploit the dual benefit of high voltage transition metal redox and O‐redox, instead relying on Mn3+/4+ capacity close to 2 V vs Na+/Na. Here, a new Na‐ion cathode exhibiting electron–holes on O is demonstrated, P2‐type Na0.67Li0.1Ni0.3Mn0.6O2, which also utilizes the high voltage Ni3+/4+ redox couple to deliver the highest reported energy density among this class of compound. By employing a low Li content and avoiding honeycomb ordering within the transition metal layer, it is possible to stabilize the hole states, and the high voltage plateau is preserved in Na0.67Li0.1Ni0.3Mn0.6O2 over cycling. [ABSTRACT FROM AUTHOR]

Published
2024
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17. Mg-rich disordered rocksalt oxide cathodes for Mg-ion batteries.

Author

Quan, Yuan, Ji, Dingqiao, Yuan, Yi, Xu, Hang, Qi, Rui, De Sousa Coutinho, Sofia, Riedel, Sibylle, Zhao-Karger, Zhirong, Song, Lijiang, Robertson, Alexander W., Bruce, Peter G., and House, Robert A.

Abstract

The discovery of new transition metal (TM) oxide cathodes which can act as intercalation hosts for Mg2+ ions is critical for the development of high energy density Mg-ion batteries. In Li-ion batteries, disordered rocksalts with sufficiently high Li+ charge carrier ion concentration, i.e. Li : TM >1.1, can support fast Li+ diffusion and therefore deliver high capacities (∼300 mA h g−1) and rate performance. Here, we investigate a range of simple Mg-rich disordered rocksalt cathodes, Mg2TMO3 (TM = Mn, Ni, Co), which possess similar charge carrier ion concentrations and similar ratios between the ion size and interstitial tetrahedron height to Li-rich disordered rocksalts. However, even with high carbon loadings, elevated cycling temperatures and reduced particle and crystallite size, no significant Mg2+ deintercalation was observed, indicating that conventional design rules established for Li-rich DRS cannot be simply translated to Mg-rich systems. Despite the lack of activity in Mg-rich oxides, we demonstrate that Mg2+ intercalation into close-packed cubic disordered rocksalts, such as Li2−xMnO2F (x = 1), is possible, opening possible routes to activating Mg-rich systems. [ABSTRACT FROM AUTHOR]

Published
2024
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18. Epidemiologische Situation ausgewählter zoonotischer Parasiten bei wildlebenden Karnivoren in Sachsen-Anhalt

Author

Universität Leipzig, House, Robert Valerio, Universität Leipzig, and House, Robert Valerio

Abstract

Einleitung: Wildtiere stellen eine Quelle zoonotischer Erreger dar. Insbesondere Mesokarnivoren, kleine bis mittelgroße Karnivoren, wie z. B. Füchse, Marderhunde, Waschbären, Dachse und Marder, spielen eine besondere Rolle bei Eintrag, Erhalt und Übertragung parasitärer Zoonosen auf Haustiere und den Menschen. Ziele der Untersuchung: Das Ziel der Arbeit bestand darin, Vorkommen und Prävalenz relevanter zoonotischer Parasiten bei wildlebenden Karnivoren zu definieren und eventuell vorhandene Areale mit einem erhöhten „relativen geografischen Risiko“ als Näherungswert für das Infektionsrisiko des Menschen zu berechnen. Im Sinne des One-Health-Ansatzes wurde das vorhandene Risiko sowie Risikominderungsmaßnahmen unter Betrachtung der Erreger, der Wirte und der Umwelt interpretiert. Tiere, Material und Methoden: In den Jahren 2016 und 2017 wurden im Rahmen des Surveillanceprogramms zur Aufrechterhaltung des Status „Tollwutfreie Region“ 1.206 Wildkarnivoren, darunter 926 Füchse, 213 Waschbären, 38 Marderhunde und 29 andere Karnivoren (Dachs, Marder, Steinmarder), eingesendet. Dabei wurden die Untersuchungen bei den in Mitteleuropa für den jeweiligen Parasiten relevantesten Endwirten durchgeführt. Konkret wurde auf Echinococcus multilocularis (Füchse und Marderhunde, n= 864), Baylisascaris procyonis (Waschbären, n= 197), Alaria alata (Füchse und Marderhunde, n= 864), Trichinella spp., Thelazia callipaeda und Sarcoptes scabiei (alle Karnivoren, n= 1.206) untersucht. Zudem wurde im Jahr 2018 eine Stichprobe von 150 Füchsen auf Giardia spp. untersucht. Für alle nachgewiesenen Erreger wurde die adjustierte Prävalenz berechnet. Zur Beantwortung der Frage, ob Anhäufungen positiver Nachweise durch die zugrundeliegende Populationsdichte zu erklären waren, wurden unter Nutzung der Pakete „sparr“, „sm“ und „maptools“ in der Software R eine Kernelglättung mit berechnetem, konstanten Glättungsparameter durchgeführt und darüber hinaus Toleranzkonturen ermittelt. Dadurch konnten Areale, Introduction: Wild animals are a source of zoonotic pathogens. Especially mesocarnivores, small- or mid-sized carnivores, i.e. foxes, raccoon dogs, raccoons, badgers and martens, play a relevant role in the introduction, maintenance and transmission of parasitic zoonoses to humans or domestic animals. Aims of the Study: Aim of this study was to define the presence and prevalence of relevant zoonotic parasites in wild carnivores and to detect areas with an increased “spatial relative risk” as proxy for the risk of human infection. The risk and risk reducing measures were interpreted under consideration of the pathogens, the hosts and the environment as requested by a One-Health approach. Animals, Material and Methods: In the years 2016 and 2017, 1.206 wild carnivores, therefrom 926 foxes, 213 raccoons, 38 raccoon dogs and 29 other carnivores (badgers and martens), of the surveillance program against rabies were examined. The study was carried out on the final hosts that are most relevant for the respective parasite in Central Europe. Overall, Echinococcus multilocularis (foxes and raccoon dogs, n=864), Baylisascaris procyonis (raccoons, n=197), Alaria alata (foxes and raccoon dogs, n=864), Trichinella spp., Thelazia callipaeda and Sarcoptes scabiei (all carnivores, n=1.206) were examined. In 2018, a sample of 150 foxes was examined for Giardia spp.. The adjusted prevalence was calculated. In order to answer the question whether the accumulation of positive detections could be explained by the underlying population density, a kernel smoothing with a calculated, constant smoothing parameter was performed using the packages 'sparr', 'sm' and 'maptools' in the software R and tolerance contours were also determined. This made it possible to define areas with an increased risk of infection of the final hosts. Results: Following adjusted Prevalences could be calculated: Echinococcus multilocularis 27.71 % (adjust. CI 95 %: 24.94 %–30.49 %); Baylisascaris procyonis 32.49 % (

Published
2024

19. Epidemiologische Situation ausgewählter zoonotischer Parasiten bei wildlebenden Karnivoren in Sachsen-Anhalt

Author

House, Robert Valerio and House, Robert Valerio

Abstract

Einleitung: Wildtiere stellen eine Quelle zoonotischer Erreger dar. Insbesondere Mesokarnivoren, kleine bis mittelgroße Karnivoren, wie z. B. Füchse, Marderhunde, Waschbären, Dachse und Marder, spielen eine besondere Rolle bei Eintrag, Erhalt und Übertragung parasitärer Zoonosen auf Haustiere und den Menschen. Ziele der Untersuchung: Das Ziel der Arbeit bestand darin, Vorkommen und Prävalenz relevanter zoonotischer Parasiten bei wildlebenden Karnivoren zu definieren und eventuell vorhandene Areale mit einem erhöhten „relativen geografischen Risiko“ als Näherungswert für das Infektionsrisiko des Menschen zu berechnen. Im Sinne des One-Health-Ansatzes wurde das vorhandene Risiko sowie Risikominderungsmaßnahmen unter Betrachtung der Erreger, der Wirte und der Umwelt interpretiert. Tiere, Material und Methoden: In den Jahren 2016 und 2017 wurden im Rahmen des Surveillanceprogramms zur Aufrechterhaltung des Status „Tollwutfreie Region“ 1.206 Wildkarnivoren, darunter 926 Füchse, 213 Waschbären, 38 Marderhunde und 29 andere Karnivoren (Dachs, Marder, Steinmarder), eingesendet. Dabei wurden die Untersuchungen bei den in Mitteleuropa für den jeweiligen Parasiten relevantesten Endwirten durchgeführt. Konkret wurde auf Echinococcus multilocularis (Füchse und Marderhunde, n= 864), Baylisascaris procyonis (Waschbären, n= 197), Alaria alata (Füchse und Marderhunde, n= 864), Trichinella spp., Thelazia callipaeda und Sarcoptes scabiei (alle Karnivoren, n= 1.206) untersucht. Zudem wurde im Jahr 2018 eine Stichprobe von 150 Füchsen auf Giardia spp. untersucht. Für alle nachgewiesenen Erreger wurde die adjustierte Prävalenz berechnet. Zur Beantwortung der Frage, ob Anhäufungen positiver Nachweise durch die zugrundeliegende Populationsdichte zu erklären waren, wurden unter Nutzung der Pakete „sparr“, „sm“ und „maptools“ in der Software R eine Kernelglättung mit berechnetem, konstanten Glättungsparameter durchgeführt und darüber hinaus Toleranzkonturen ermittelt. Dadurch konnten Areale, Introduction: Wild animals are a source of zoonotic pathogens. Especially mesocarnivores, small- or mid-sized carnivores, i.e. foxes, raccoon dogs, raccoons, badgers and martens, play a relevant role in the introduction, maintenance and transmission of parasitic zoonoses to humans or domestic animals. Aims of the Study: Aim of this study was to define the presence and prevalence of relevant zoonotic parasites in wild carnivores and to detect areas with an increased “spatial relative risk” as proxy for the risk of human infection. The risk and risk reducing measures were interpreted under consideration of the pathogens, the hosts and the environment as requested by a One-Health approach. Animals, Material and Methods: In the years 2016 and 2017, 1.206 wild carnivores, therefrom 926 foxes, 213 raccoons, 38 raccoon dogs and 29 other carnivores (badgers and martens), of the surveillance program against rabies were examined. The study was carried out on the final hosts that are most relevant for the respective parasite in Central Europe. Overall, Echinococcus multilocularis (foxes and raccoon dogs, n=864), Baylisascaris procyonis (raccoons, n=197), Alaria alata (foxes and raccoon dogs, n=864), Trichinella spp., Thelazia callipaeda and Sarcoptes scabiei (all carnivores, n=1.206) were examined. In 2018, a sample of 150 foxes was examined for Giardia spp.. The adjusted prevalence was calculated. In order to answer the question whether the accumulation of positive detections could be explained by the underlying population density, a kernel smoothing with a calculated, constant smoothing parameter was performed using the packages 'sparr', 'sm' and 'maptools' in the software R and tolerance contours were also determined. This made it possible to define areas with an increased risk of infection of the final hosts. Results: Following adjusted Prevalences could be calculated: Echinococcus multilocularis 27.71 % (adjust. CI 95 %: 24.94 %–30.49 %); Baylisascaris procyonis 32.49 % (

Published
2024

20. Vibrationally-resolved RIXS reveals OH-group formation in oxygen redox active Li-ion battery cathodes

Author

Hirsbrunner, Moritz, Mikheenkova, Anastasiia, Törnblom, Pontus, House, Robert A., Zhang, Wenliang, Asmara, Teguh C., Wei, Yuan, Schmitt, Thorsten, Rensmo, Håkan, Mukherjee, Soham, Hahlin, Maria, Duda, Laurent C., Hirsbrunner, Moritz, Mikheenkova, Anastasiia, Törnblom, Pontus, House, Robert A., Zhang, Wenliang, Asmara, Teguh C., Wei, Yuan, Schmitt, Thorsten, Rensmo, Håkan, Mukherjee, Soham, Hahlin, Maria, and Duda, Laurent C.

Abstract

Vibrationally-resolved resonant inelastic X-ray scattering (VR-RIXS) at the O K-edge is emerging as a powerful tool for identifying embedded molecules in lithium-ion battery cathodes. Here, we investigate two known oxygen redox-active cathode materials: the commercial LixNi0.90Co0.05Al0.05O2 (NCA) used in electric vehicles and the high-capacity cathode material Li1.2Ni0.13Co0.13Mn0.54O2 (LRNMC) for next-generation Li-ion batteries. We report the detection of a novel vibrational RIXS signature for Li-ion battery cathodes appearing in the O K pre-peak above 533 eV that we attribute to OH-groups. We discuss likely locations and pathways for OH-group formation and accumulation throughout the active cathode material. Initial-cycle behaviour for LRNMC shows that OH-signal strength correlates with the cathodes state of charge, though reversibility is incomplete. The OH-group RIXS signal strength in long-term cycled NCA is retained. Thus, VR-RIXS offers a path for gaining new insights to oxygen reactions in battery materials., Authors in the list of papers of Anastasiia Mikheenkova's thesis: Moritz Hirsbrunner, Anastasiia Mikheenkova, Pontus Törnblom, Robert A. House, Thorsten Schmitt, Håkan Rensmo, Soham Mukherjee, Maria Halin, Laurent Duda

Published
2024
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21. Distinguishing Bulk Redox from Near-Surface Degradation in Lithium Nickel Oxide Cathodes

Author

Weatherup, Robert, primary, An, Lijin, additional, Swallow, Jack, additional, Cong, Peixi, additional, Zhang, Ruomu, additional, Poletayev, Andrey, additional, Björklund, Erik, additional, Didwal, Pravin, additional, Fraser, Michael, additional, Jones, Leanne, additional, Phelan, Conor, additional, Ramesh, Namrata, additional, Harris, Grant, additional, Sahle, Christoph, additional, Ferrer, Pilar, additional, Grinter, David, additional, Bencok, Peter, additional, Hayama, Shusaku, additional, Islam, M. Saiful, additional, House, Robert, additional, Nellist, Peter, additional, Green, Robert, additional, and Nicholls, Rebecca, additional

Published
2024
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22. Does trapped O2 form in the bulk of LiNiO2 during charging?

Author

Juelsholt, Mikkel, primary, Chen, Jun, additional, Pérez-Osorio, Miguel A., additional, Rees, Gregory Jon, additional, De Sousa Coutinho, Sofia, additional, Maynard-Casely, Helen Elizabeth, additional, Liu, Jue, additional, Everett, Michelle, additional, Agrestini, Stefano, additional, Garcia-Fernandez, Mirian, additional, Zhou, Ke-Jin, additional, House, Robert, additional, and Bruce, Peter G., additional

Published
2024
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24. Visualization of Tetrahedral Li in the Alkali Layers of Li-Rich Layered Metal Oxides

Author

Song, Weixin, Pérez-Osorio, Miguel A., Chen, Jun, Ding, Zhiyuan, Marie, John-Joseph, Juelsholt, Mikkel, House, Robert A., Bruce, Peter G., and Nellist, Peter D.

Abstract

Understanding Li+ion diffusion pathways in Li-rich layered transition metal (TM) oxides is crucial for understanding the sluggish kinetics in anionic O2–redox. Although Li diffusion within the alkali layers undergoes a low-barrier octahedral–tetrahedral–octahedral pathway, it is less clear how Li diffuses in and out of the TM layers, particularly given the complex structural rearrangements that take place during the oxidation of O2–. Here, we develop simultaneous electron ptychography and annular dark field imaging methods to unlock the Li migration pathways in Li1.2Ni0.13Mn0.54Co0.13O2associated with structural changes in the charge–discharge cycle. At the end of TM oxidation and before the high-voltage O oxidation plateau, we show that the Li migrating out of the TM layers occupies the alkali-layer tetrahedral sites on opposite sides of the TM layers, forming Li–Li dumbbell configurations, consistent with the density functional theory calculations. Also occurring are the TM migration and phase transition from O3 to O1 stacking, leading to unstable tetrahedral Li and the absence of Li contrast in imaging. Upon further Li deintercalation to 4.8 V, most of the tetrahedral Li are removed. After discharging to 2 V, we did not identify the reformation of tetrahedral Li but observed permanently migrated TMs at the alkali-layer sites, disfavoring the Li occupying the tetrahedral sites for diffusion. Our findings suggest a landscape of Li diffusion pathways in Li-rich layered oxides and strategies for minimizing the disruption of Li diffusion.

Published
2024
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28. Chemical Origins of a Fast-Charge Performance in Disordered Carbon Anodes

Author

Ahn, Sunyhik, primary, Lagnoni, Marco, additional, Yuan, Yi, additional, Ogarev, Anton, additional, Vavrinyuk, Elena, additional, Voynov, George, additional, Barrett, Eleanor, additional, Pelli, Alexander, additional, Atrashchenko, Alexander, additional, Platonov, Alexei, additional, Gurevich, Sergey, additional, Gorokhov, Maksim, additional, Rupasov, Dmitry, additional, Robertson, Alex W., additional, House, Robert A., additional, Johnson, Lee R., additional, Bertei, Antonio, additional, and Chernyshov, Denis V., additional

Published
2023
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29. Trapped O2and the origin of voltage fade in layered Li-rich cathodes

Author

Marie, John-Joseph, House, Robert A., Rees, Gregory J., Robertson, Alex W., Jenkins, Max, Chen, Jun, Agrestini, Stefano, Garcia-Fernandez, Mirian, Zhou, Ke-Jin, and Bruce, Peter G.

Abstract

Oxygen redox cathodes, such as Li1.2Ni0.13Co0.13Mn0.54O2, deliver higher energy densities than those based on transition metal redox alone. However, they commonly exhibit voltage fade, a gradually diminishing discharge voltage on extended cycling. Recent research has shown that, on the first charge, oxidation of O2−ions forms O2molecules trapped in nano-sized voids within the structure, which can be fully reduced to O2−on the subsequent discharge. Here we show that the loss of O-redox capacity on cycling and therefore voltage fade arises from a combination of a reduction in the reversibility of the O2−/O2redox process and O2loss. The closed voids that trap O2grow on cycling, rendering more of the trapped O2electrochemically inactive. The size and density of voids leads to cracking of the particles and open voids at the surfaces, releasing O2. Our findings implicate the thermodynamic driving force to form O2as the root cause of transition metal migration, void formation and consequently voltage fade in Li-rich cathodes.

Published
2024
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30. The Pediatric Optic Neuritis Prospective Outcomes Study

Author

Pineles, Stacy L., primary, Henderson, Robert J., additional, Repka, Michael X., additional, Heidary, Gena, additional, Liu, Grant T., additional, Waldman, Amy T., additional, Borchert, Mark S., additional, Khanna, Sangeeta, additional, Graves, Jennifer S., additional, Collinge, Janine E., additional, Conley, Julie A., additional, Davis, Patricia L., additional, Kraker, Raymond T., additional, Cotter, Susan A., additional, Holmes, Jonathan M., additional, Chang, Melinda Y., additional, Contractor, Dilshad, additional, Zolfaghari, Emily J., additional, Vyas, Aarti, additional, Yuen, Tiffany, additional, Shah, Veeral S., additional, Paysse, Evelyn A., additional, Romany, Gihan, additional, Peragallo, Jason H., additional, Brower, Judy L., additional, Raghuram, Aparna, additional, Al Wattar, Bilal, additional, Chinn, Ryan, additional, Kothari, Srishti, additional, Siatkowski, R. Michael, additional, Lim, Maria E., additional, Brewer, Alisha N., additional, Doughty, Annette M., additional, Icks, Sonny W., additional, Almeida, Shannon, additional, de Alba Campomanes, Alejandra, additional, Banwait, Premilla, additional, Hajkazemshirazi, Leila, additional, Bastea-Forte, Yizhuo, additional, Arjona, Jennifer K., additional, Chen, Jeremy, additional, Cooper, Karen, additional, Ghadban, Rafif, additional, Chung, Sophia M., additional, Cruz, Oscar A., additional, Christenson, Traci A., additional, Breeding, Lisa L., additional, Govreau, Dawn M., additional, Wallis, Beth A., additional, Geddie, Brooke E., additional, Wolinski, Elisabeth T., additional, Rudaitis, Indre M., additional, Twite, Jacqueline, additional, Bloomquist, Carrie S., additional, Laboy, Sarah R., additional, Twite, Jackie M., additional, Pineles, Stacy L., additional, Doan, Michelle V., additional, Bernardo, Marianne J., additional, Brodsky, Michael C., additional, Chen, John J., additional, Wernimont, Suzanne M., additional, Czaplewski, Lindsay L., additional, Eastman, Stacy L., additional, Keehn, Moriah A., additional, Priebe, Debbie M., additional, Bremer, Don L., additional, Golden, Richard P., additional, Jordan, Catherine O., additional, McGregor, Mary Lou, additional, Reem, Rachel E., additional, Rogers, David L., additional, Schreckengost, Amanda N., additional, Maletic, Sara A., additional, Dairi, Mays A., additional, Enyedi, Laura B., additional, Jones, Sarah K., additional, Barman, Navajyoti R., additional, House, Robert J., additional, Nasrazadani, David A., additional, Gratton, Sean M., additional, Marsh, Justin D., additional, Dent, Rebecca J., additional, Bond, Lezlie L., additional, Soske, Lori L., additional, Sudhakar, Padmaja, additional, Willen, Christi M., additional, Taylor, Deborah, additional, Moliterno, Nathaniel Q., additional, Nsoesie, Michael, additional, Vally, Shaista, additional, Phillips, Paul H., additional, Lowery, Robert S., additional, Colon, Beth, additional, Stotts, Nancy L., additional, To, Kelly D., additional, McClelland, Collin M., additional, Areaux, Raymond G., additional, Holleschau, Ann M., additional, Merrill, Kim S., additional, Ospina, Luis H., additional, Superstein, Rosanne, additional, Thibeault, Maryse, additional, Gagnon, Helene, additional, Donahue, Sean P., additional, Ruark, Scott T., additional, Fraine, Lisa A., additional, Sprouse, Petrice A., additional, Biernacki, Ronald J., additional, Avery, Robert A., additional, Forbes, Brian J., additional, Jivraj, Imran, additional, Kohli, Anita A., additional, Richter, Meg M., additional, Baumritter, Agnieshka, additional, Mitchell, Ellen B., additional, Nischal, Ken K., additional, Runkel, Lauren M., additional, Blaha, Bianca, additional, Churchfield, Whitney, additional, Fulwylie, Christina, additional, Ko, Melissa W., additional, Mejico, Luis J., additional, Iqbal, Muhammad, additional, Attanasio, Catherine E., additional, Deb, Lena F., additional, Goodrich, Courtney B., additional, Hartwell, Alisha M., additional, Moore, Jennifer A., additional, Bohra, Lisa, additional, Apkarian, Alexandra O., additional, Gianfermi, Elena M., additional, Roarty, John D., additional, Rotberg, Leemor B., additional, Perzyk, Susan N., additional, Beck, Roy W., additional, Austin, Darrell S., additional, Boyle, Nicole M., additional, Chandler, Danielle L., additional, Connelly, Patricia L., additional, Conner, Courtney L., additional, Dean, Trevano W., additional, Donahue, Quayleen, additional, Fimbel, Brooke P., additional, Hercinovic, Amra, additional, Hoepner, James E., additional, Kaplon, Joseph D., additional, Li, Zhuokai, additional, Ortiz, Gillaine, additional, Robinson, Julianne L., additional, Stutz, Kathleen M., additional, Toro, David O., additional, Woodard, Victoria C., additional, Wu, Rui, additional, Balcer, Laura, additional, Kupersmith, Mark, additional, Lazar, Elizabeth L., additional, Waldman, Amy, additional, Wallace, David K., additional, Birch, Eileen E., additional, Chen, Angela M., additional, Christiansen, Stephen P., additional, Erzurum, S. Ayse, additional, Everett, Donald F., additional, Freedman, Sharon F., additional, Good, William V., additional, Lee, Katherine A., additional, London, Richard, additional, Manh, Vivian M., additional, Manny, Ruth E., additional, Morrison, David G., additional, Schweinler, Bonita R., additional, Silver, Jayne L., additional, Verderber, Lisa C., additional, Weise, Katherine K., additional, Green, Ari, additional, Diener-West, Marie, additional, Baker, John D., additional, Davis, Barry, additional, Phelps, Dale L., additional, Poff, Stephen W., additional, Saunders, Richard A., additional, and Tychsen, Lawrence, additional

Published
2022
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32. Unravelling the Chemical and Structural Evolution of Mn and Ti in Disordered Rocksalt Oxyfluoride Cathode Materials Using OperandoX-ray Absorption Spectroscopy

Author

Shirazi Moghadam, Yasaman, Hu, Yang, El Kharbachi, Abdel, Belin, Stéphanie, Diemant, Thomas, Chen, Jun, House, Robert A., Bruce, Peter G., and Fichtner, Maximilian

Abstract

Li-rich disordered rocksalt (DRS) cathode materials with naturally abundant resources, high power and energy density have attracted great attention for applications in Li-ion batteries. We have previously investigated the Li2Mn1–xTixO2F (0 ≤ x≤ 2/3, LMTOF) cathode system showing an attractive cycling behavior, which is however limited by poor long-cycle stability and the unclear cation and anion redox activities in the presence of supposedly inactive Ti. In this work, synchrotron operandoX-ray absorption spectroscopy (XAS) is performed to study the chemical and structural evolution of Mn and Ti in the cathode compounds during cycling. Selected electrodes with low (x = 1/3) and high (x = 2/3) Ti content are synthesized, and their structural and electrochemical properties are first characterized accordingly. X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) are combined to track the change in oxidation states and local coordination environment for the active transition metals. In order to follow the dynamics of the active species, chemometric methods such as principal component analysis (PCA) and multivariate curve resolution (MCR) are applied. Subsequently, the Mn and Ti redox activities are monitored from initial to extended cycles, in combination with ex-situstudies and operandodifferential electrochemical mass spectrometry (DEMS) to understand the capacity fading and the redox-based degradation processes. The results provide insights into the development of Mn double-redox reactions in the DRS cathodes from initial cycles to prolonged cycling and elucidate the impacts of the reduced Mn redox activity and the increased local ordering on the cycling stability.

Published
2023
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34. Evaluation of strategies to modify Anti-SARS-CoV-2 monoclonal antibodies for optimal functionality as therapeutics

Author

House, Robert V., primary, Broge, Thomas A., additional, Suscovich, Todd J., additional, Snow, Doris M., additional, Tomic, Milan T., additional, Nonet, Genevieve, additional, Bajwa, Kamaljit, additional, Zhu, Guangyu, additional, Martinez, Zachary, additional, Hackett, Kyal, additional, Earnhart, Christopher G., additional, Dorsey, Nicole M., additional, Hopkins, Svetlana A., additional, Natour, Dalia S., additional, Davis, Heather D., additional, Anderson, Michael S., additional, Gainey, Melicia R., additional, and Cobb, Ronald R., additional

Published
2022
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36. Transition metal migration and O2 formation underpin voltage hysteresis in oxygen-redox disordered rocksalt cathodes.

Author

McColl, Kit, House, Robert A., Rees, Gregory J., Squires, Alexander G., Coles, Samuel W., Bruce, Peter G., Morgan, Benjamin J., and Islam, M. Saiful

Subjects
TRANSITION metals, CATHODES, VOLTAGE, INELASTIC scattering, DENSITY functional theory, X-ray scattering, HYSTERESIS
Abstract

Lithium-rich disordered rocksalt cathodes display high capacities arising from redox chemistry on both transition-metal ions (TM-redox) and oxygen ions (O-redox), making them promising candidates for next-generation lithium-ion batteries. However, the atomic-scale mechanisms governing O-redox behaviour in disordered structures are not fully understood. Here we show that, at high states of charge in the disordered rocksalt Li2MnO2F, transition metal migration is necessary for the formation of molecular O2 trapped in the bulk. Density functional theory calculations reveal that O2 is thermodynamically favoured over other oxidised O species, which is confirmed by resonant inelastic X-ray scattering data showing only O2 forms. When O-redox involves irreversible Mn migration, this mechanism results in a path-dependent voltage hysteresis between charge and discharge, commensurate with the hysteresis observed electrochemically. The implications are that irreversible transition metal migration should be suppressed to reduce the voltage hysteresis that afflicts O-redox disordered rocksalt cathodes. The oxygen-redox mechanism in lithium-rich disordered rocksalt cathode materials is still not well understood. Here, the authors show that in Li2MnO2F, molecular oxygen forms in the bulk during charge and is re-incorporated into the structure as oxygen anions on discharge, but this process is associated with irreversible Mn migration, causing voltage hysteresis. [ABSTRACT FROM AUTHOR]

Published
2022
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37. Controlling Iron Versus Oxygen Redox in the Layered Cathode Na0.67Fe0.5Mn0.5O2: Mitigating Voltage and Capacity Fade by Mg Substitution.

Author

Boivin, Edouard, House, Robert A., Marie, John‐Joseph, and Bruce, Peter G.

Subjects
*OXIDATION-reduction reaction, *CATHODES, *VOLTAGE, *TRANSITION metals, *IRON, *OXYGEN, *IRON-nickel alloys
Abstract

Layered oxides for Na‐ion batteries containing Fe have attracted strong interest mainly due to their low cost. However, full oxidation of Fe3+ to Fe4+ is rarely seen before O‐redox sets in and is typically accompanied by voltage and capacity fade on cycling. On charging P2‐Na0.67[Fe0.5Mn0.5]O2, Fe3+ is oxidized to only ≈Fe3.3+ before the onset of O‐redox. O‐redox occurs when the Na content is sufficiently low (Na ≈0.3) to permit the transition from P‐type to O‐type stacking, thus enabling Fe3+ migration to the Na layer. Fe3+ migration generates cation vacancies in the transition metal layer, forming □‐O‐□ configurations, which trigger the onset of O‐redox. In contrast, doping this material with Mg2+ to form P2‐Na0.67[Fe0.25Mn0.6Mg0.15]O2 allows full oxidation of Fe3+ to Fe4+ before the Na content is low enough to favor O‐type stacking. During O‐redox, Mg2+ is displaced into the Na layers instead of Fe. Mg substitution enables greater reversibility of the Fe3+/Fe4+ redox couple and significantly suppresses Fe migration, which is responsible for the voltage and capacity fade observed for P2‐Na0.67Fe0.5Mn0.5O2. [ABSTRACT FROM AUTHOR]

Published
2022
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38. Atomistic Interpretation of the Oxygen K-Edge X-ray Absorption Spectra of Layered Li-Ion Battery Cathode Materials

Author

Ramesh, Namrata, Banerjee, Hrishit, Swallow, Jack E. N., Björklund, Erik, Dean, Ava, Didwal, Pravin, Fraser, Michael, Phelan, Conor M. E., An, Lijin, Singh, Jasper, Lewis, Jarrod, Song, Weixin, House, Robert A., Morris, Andrew J., Weatherup, Robert S., and Nicholls, Rebecca J.

Abstract

Core loss spectroscopies can provide powerful element-specific insight into the redox processes occurring in Li-ion battery cathodes, but this requires an accurate interpretation of the spectral features. Here, we systematically interpret oxygen K-edge core loss spectra of layered lithium transition-metal (TM) oxides (LiMO2, where M = Co, Ni, Mn) from first principles using density-functional theory (DFT). Spectra are simulated using three exchange–correlation functionals, comprising the generalized gradient approximation (GGA) functional PBE, the DFT–PBE + Hubbard Umethod, and the meta-GGA functional rSCAN. In general, rSCAN provides a better match to experimentally observed excitation energies of spectral features compared to both PBE and PBE + U, especially at energies close to the main edge. Projected density of states of core-hole calculations show that the O orbitals are better described by rSCAN. Hybridization, structural distortions, chemical composition, and magnetism significantly influence the spectra. The O K-edge spectrum of LiNiO2obtained using rSCAN shows a closer match to the experimental X-ray absorption spectroscopy (XAS) when derived from a simulation cell which includes a Jahn–Teller distortion, showing that the DFT-calculated pre-edge feature contains information about not only chemical species but also geometric distortion. Core loss spectra derived from DFT can also differentiate between materials with the same structure and magnetic configuration but comprising different TMs; these differences are comparable to those observed in experimental XAS from the same materials. This foundational work helps establish the extent to which DFT can be used to bridge the interpretation gap between experimental spectroscopic signatures and ab initio methods describing complex battery materials, such as lithium nickel manganese cobalt oxides.

Published
2024
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39. Reversible Electron–Holes on O in P2‐type Na0.67Li0.1Ni0.3Mn0.6O2.

Author

Marie, John‐Joseph, Jenkins, Max, Chen, Jun, Rees, Gregory, Cellorio, Veronica, Choi, Jaewon, Agrestini, Stefano, Garcia‐Fernandez, Mirian, Zhou, Ke‐Jin, House, Robert A., and Bruce, Peter G.

Subjects
*ENERGY density, *HIGH voltages, *TRANSITION metals, *CATHODES, *HONEYCOMB structures
Abstract

Achieving reversible O‐redox through the formation of electron–holes on O could hold the key to a new generation of high energy density Na‐ion cathodes. However, to date, it has only been demonstrated in a small handful of cathode materials and none of these materials exploit the dual benefit of high voltage transition metal redox and O‐redox, instead relying on Mn3+/4+ capacity close to 2 V vs Na+/Na. Here, a new Na‐ion cathode exhibiting electron–holes on O is demonstrated, P2‐type Na0.67Li0.1Ni0.3Mn0.6O2, which also utilizes the high voltage Ni3+/4+ redox couple to deliver the highest reported energy density among this class of compound. By employing a low Li content and avoiding honeycomb ordering within the transition metal layer, it is possible to stabilize the hole states, and the high voltage plateau is preserved in Na0.67Li0.1Ni0.3Mn0.6O2 over cycling. [ABSTRACT FROM AUTHOR]

Published
2024
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40. Vibrationally-resolved RIXS reveals OH-group formation in oxygen redox active Li-ion battery cathodes.

Author

Hirsbrunner M, Mikheenkova A, Törnblom P, House RA, Zhang W, Asmara TC, Wei Y, Schmitt T, Rensmo H, Mukherjee S, Hahlin M, and Duda LC

Abstract

Vibrationally-resolved resonant inelastic X-ray scattering (VR-RIXS) at the O K-edge is emerging as a powerful tool for identifying embedded molecules in lithium-ion battery cathodes. Here, we investigate two known oxygen redox-active cathode materials: the commercial Li x Ni 0.90 Co 0.05 Al 0.05 O 2 (NCA) used in electric vehicles and the high-capacity cathode material Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 (LRNMC) for next-generation Li-ion batteries. We report the detection of a novel vibrational RIXS signature for Li-ion battery cathodes appearing in the O K pre-peak above 533 eV that we attribute to OH-groups. We discuss likely locations and pathways for OH-group formation and accumulation throughout the active cathode material. Initial-cycle behaviour for LRNMC shows that OH-signal strength correlates with the cathodes state of charge, though reversibility is incomplete. The OH-group RIXS signal strength in long-term cycled NCA is retained. Thus, VR-RIXS offers a path for gaining new insights to oxygen reactions in battery materials.

Published
2024
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