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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 redox chemistry of oxygen in cathode materials for rechargeable alkali-ion batteries

Author

House, Robert and Bruce, Peter

Subjects
Synthesis, X-ray spectroscopy, Chemistry, Inorganic, Materials, Diffraction, Solid state chemistry, Chemistry, Energy storage
Abstract

There is a clear and urgent need for rechargeable batteries of higher energy density. Alkali-ion batteries based on Li-ions are the state-of-the-art, although Na-ion may offer a cheaper alternative. In both cases the cathode imposes the biggest limitation on overall energy density. Alkali-rich cathode materials can store alkali-ions and electrons densely by invoking redox chemistry of both the transition metal (TM) and oxide ions in the lattice. However, O-redox is accompanied by voltage hysteresis, irreversible O-loss and complex structural changes. In this thesis, model Na-ion materials have been investigated to isolate and examine these phenomena. Firstly, Na0.67[Mg0.28Mn0.72]O2, with Mg2+ ions occupying the TM layer rather than alkali-ions, is studied and shown to exhibit O-redox. This reveals that ionic interactions between the TM layer substituent and O are the necessary precondition for O-redox. Secondly, by comparing the O-loss behaviours of Na0.67[Mg0.28Mn0.72]O2 and Na0.75[Li0.25Mn0.75]O2, the critical role of the TM layer substituent is revealed; when removed from the structure, the co-ordination number around O can drop below three and O-loss is triggered. Unlike Li+, Mg2+ is retained within the structure preventing O-loss. Thirdly, O-redox materials Na0.75[Li0.25Mn0.75]O2 and Na0.6[Li0.2Mn0.8]O2 are studied in parallel to understand why the former exhibits voltage hysteresis and the latter not. The preservation of the TM layer ordering scheme is shown to prevent hysteresis maintaining stable electron holes on O2- in Na0.6[Li0.2Mn0.8]O2. For Na0.75[Li0.25Mn0.75]O2, severe in-plane TM migration destroys the ordering scheme, triggered by formation of molecular O2 gas which is directly evidenced for the first time in the bulk. Reduction of O2 occurs on discharge at low voltage giving rise to hysteresis. Finally, a new Li-rich oxyfluoride, Li2MnO2F, with a stable disordered rocksalt structure is presented. Li2MnO2F stores charge utilising both Mn and O-redox with negligible O-loss demonstrating the potential of disordered rocksalts to deliver high energy densities.

Published
2019

10. 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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11. 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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14. 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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19. 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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20. 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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21. 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

22. 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

23. 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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27. 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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28. 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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30. Superstructure control of first-cycle voltage hysteresis in oxygen-redox cathodes

Author

House, Robert A., Maitra, Urmimala, Pérez-Osorio, Miguel A., Lozano, Juan G., Jin, Liyu, Somerville, James W., and Duda, Laurent C.

Subjects
Control, Chemical properties, Electric properties, Oxygen -- Electric properties -- Chemical properties, Hysteresis (Physics) -- Control, Cathodes -- Electric properties, Hysteresis -- Control
Abstract

Author(s): Robert A. House [sup.1] , Urmimala Maitra [sup.1] , Miguel A. Pérez-Osorio [sup.1] , Juan G. Lozano [sup.1] [sup.2] , Liyu Jin [sup.1] , James W. Somerville [sup.1] , [...], In conventional intercalation cathodes, alkali metal ions can move in and out of a layered material with the charge being compensated for by reversible reduction and oxidation of the transition metal ions. If the cathode material used in a lithium-ion or sodium-ion battery is alkali-rich, this can increase the battery's energy density by storing charge on the oxide and the transition metal ions, rather than on the transition metal alone.sup.1-10. There is a high voltage associated with oxidation of O.sup.2- during the first charge, but this is not recovered on discharge, resulting in reduced energy density.sup.11. Displacement of transition metal ions into the alkali metal layers has been proposed to explain the first-cycle voltage loss (hysteresis).sup.9,12-16. By comparing two closely related intercalation cathodes, Na.sub.0.75[Li.sub.0.25Mn.sub.0.75]O.sub.2 and Na.sub.0.6[Li.sub.0.2Mn.sub.0.8]O.sub.2, here we show that the first-cycle voltage hysteresis is determined by the superstructure in the cathode, specifically the local ordering of lithium and transition metal ions in the transition metal layers. The honeycomb superstructure of Na.sub.0.75[Li.sub.0.25Mn.sub.0.75]O.sub.2, present in almost all oxygen-redox compounds, is lost on charging, driven in part by formation of molecular O.sub.2 inside the solid. The O.sub.2 molecules are cleaved on discharge, reforming O.sup.2-, but the manganese ions have migrated within the plane, changing the coordination around O.sup.2- and lowering the voltage on discharge. The ribbon superstructure in Na.sub.0.6[Li.sub.0.2Mn.sub.0.8]O.sub.2 inhibits manganese disorder and hence O.sub.2 formation, suppressing hysteresis and promoting stable electron holes on O.sup.2- that are revealed by X-ray absorption spectroscopy. The results show that voltage hysteresis can be avoided in oxygen-redox cathodes by forming materials with a ribbon superstructure in the transition metal layers that suppresses migration of the transition metal. In oxygen-redox intercalation cathodes, voltage hysteresis can be avoided by forming cathode materials with a 'ribbon' superstructure in the transition metal layers that suppresses transition metal migration.

Published
2020
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37. 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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42. Contributors

Author

Ali, Mohsin H., primary, Bleicher, Isaac, additional, Chen, Xi, additional, Dandridge, Alexandria, additional, El-Dairi, Mays, additional, Ely, Amanda, additional, Finn, Avni P., additional, Freedman, Sharon F., additional, Gabr, Hesham, additional, Grewal, Dilraj S., additional, House, Robert J., additional, Hsu, S. Tammy, additional, Kelly, Michael P., additional, Mangalesh, Shwetha, additional, Mruthyunjaya, Prithvi, additional, Ong, Sally S., additional, Rothman, Adam L., additional, Sarin, Neeru, additional, Scott, Adrienne W., additional, Tai, Vincent, additional, Thomas, Akshay, additional, Tian, James, additional, Toth, Cynthia A., additional, Tran-Viet, Du, additional, Vajzovic, Lejla, additional, Viehland, Christian, additional, Winter, Katrina Postell, additional, Yiu, Glenn, additional, Yoon, Steven, additional, and Zhang, Wenlan, additional

Published
2020
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