Browsing by Author "Wu, Y"

Now showing 1 - 10 of 10
  • Thumbnail Image
    Item
    Arginine catabolism is essential to polymyxin dependence in Acinetobacter baumannii
    (Elsevier, 2024-07) Han, ML; Alsaadi, Y; Zhao, JX; Zhu, Y; Lu, J; Jiang, X; Ma, W; Patil, NA; Dunstan, RA; Le Brun, AP; Wickremasinghe, H; Hu, X; Wu, Y; Yu, HH; Wang, J; Barlow, CK; Bergen, PJ; Shen, HH; Lithgow, T; Creek, DJ; Velkov, T; Li, J
    Polymyxins are often the only effective antibiotics against the "Critical" pathogen Acinetobacter baumannii. Worryingly, highly polymyxin-resistant A. baumannii displaying dependence on polymyxins has emerged in the clinic, leading to diagnosis and treatment failures. Here, we report that arginine metabolism is essential for polymyxin-dependent A. baumannii. Specifically, the arginine degradation pathway was significantly altered in polymyxin-dependent strains compared to wild-type strains, with critical metabolites (e.g., L-arginine and L-glutamate) severely depleted and expression of the astABCDE operon significantly increased. Supplementation of arginine increased bacterial metabolic activity and suppressed polymyxin dependence. Deletion of astA, the first gene in the arginine degradation pathway, decreased phosphatidylglycerol and increased phosphatidylethanolamine levels in the outer membrane, thereby reducing the interaction with polymyxins. This study elucidates the molecular mechanism by which arginine metabolism impacts polymyxin dependence in A. baumannii, underscoring its critical role in improving diagnosis and treatment of life-threatening infections caused by "undetectable" polymyxin-dependent A. baumannii. ª 2024 The Author(s). Published by Elsevier Inc. This is an open access article under the CC BY-NC licence
  • Thumbnail Image
    Item
    Austenite formation kinetics from multicomponent cementite-ferrite aggregates by in situ neutron powder diffraction
    (Australian Institute of Nuclear Science and Engineering (AINSE), 2020-11-11) Wu, Y; Wang, L; Sun, W; Styles, MJ; Studer, AJ; Brechet, Y; Hutchinson, C
    The development of third generation advanced high strength steels (AHSS) as the next generation sheet steel grade is driven by the automotive industry. The key processing step is called ‘intercritical annealing’ at temperatures in the region of the ferrite and austenite two-phase field. The transformed austenite during intercritical annealing will be retained at a metastable state in the final microstructure. Controlling the fraction and chemistry of austenite and resulting mechanical properties is critical for many AHSS. The kinetics of austenite formation depend sensitively on the initial microstructure and annealing conditions. In this talk, we will present detailed kinetic studies of austenite formation from cementite-ferrite aggregate in a range of AHSS grades via in situ neutron powder diffraction at WOMBAT. The quantitative phase analyses highlight that the saturation of transformation kinetics in relation to global equilibrium is affected by the competition between different interface migration. Depending on the relative contribution of cementite dissolution in respect to migrating interface of austenite/ferrite, the incomplete dissolution of enveloped cementite limited by slow diffusion in austenite could result in austenite plateauing below equilibrium, while fast dissolution of matrix cementite could result in austenite plateau above equilibrium. Both contributions need to be considered and modelled to describe the austenite formation kinetics. The experimental and computational work in this contribution would guide future processing and alloy design of AHSS.
  • No Thumbnail Available
    Item
    Elucidating negative thermal expansion in MOF-5
    (American Chemical Society, 2010-9-09) Lock, N; Wu, Y; Christensen, M; Cameron, L; Peterson, VK; Bridgeman, AJ; Kepert, CJ; Iversen, BB
    Multi-temperature X-ray diffraction studies show that twisting, rotation, and libration cause negative thermal expansion (NTE) of the nanoporous metal−organic framework MOF-5, Zn4O(1,4-benzenedicarboxylate)3. The near-linear lattice contraction is quantified in the temperature range 80−500 K using synchrotron powder X-ray diffraction. Vibrational motions causing the abnormal expansion behavior are evidenced by shortening of certain interatomic distances with increasing temperature according to single-crystal X-ray diffraction on a guest-free crystal over a broad temperature range. Detailed analysis of the atomic positional and displacement parameters suggests two contributions to cause the effect: (1) local twisting and vibrational motion of the carboxylate groups and (2) concerted transverse vibration of the linear linkers. The vibrational mechanism is confirmed by calculations of the dynamics in a molecular fragment of the framework. © 2010, American Chemical Society
  • Thumbnail Image
    Item
    In operando neutron diffraction study of the temperature and current rate-dependent phase evolution of LiFePO4 in a commercial battery
    (Elsevier, 2017-02-28) Sharma, N; Yu, DH; Zhu, Y; Wu, Y; Peterson, VK
    In operando NPD data of electrodes in lithium-ion batteries reveal unusual LiFePO4 phase evolution after the application of a thermal step and at high current. At low current under ambient conditions the LiFePO4 to FePO4 two-phase reaction occurs during the charge process, however, following a thermal step and at higher current this reaction appears at the end of charge and continues into the next electrochemical step. The same behavior is observed for the FePO4 to LiFePO4 transition, occurring at the end of discharge and continuing into the following electrochemical step. This suggests that the bulk (or the majority of the) electrode transformation is dependent on the battery's history, current, or temperature. Such information concerning the non-equilibrium evolution of an electrode allows a direct link between the electrode's functional mechanism that underpins lithium-ion battery behavior and the real-life operating conditions of the battery, such as variable temperature and current, to be made. Crown Copyright©2016 Published by Elsevier B.V
  • Thumbnail Image
    Item
    Interpenetration as a mechanism for negative thermal expansion in the metal–organic framework Cu3(btb)2 (MOF-14)
    (Wiley, 2014-04-01) Wu, Y; Peterson, VK; Luks, E; Darwish, TA; Kepert, CJ
    Metal–organic framework materials (MOFs) have recently been shown in some cases to exhibit strong negative thermal expansion (NTE) behavior, while framework interpenetration has been found to reduce NTE in many materials. Using powder and single-crystal diffraction methods we investigate the thermal expansion behavior of interpenetrated Cu3(btb)2 (MOF-14) and find that it exhibits an anomalously large NTE effect. Temperature-dependent structural analysis shows that, contrary to other interpenetrated materials, in MOF-14 the large positive thermal expansion of weak interactions that hold the interpenetrating networks together results in a low-energy contractive distortion of the overall framework structure, demonstrating a new mechanism for NTE. © 2014, WILEY‐VCH Verlag GmbH & Co. KGaA.
  • Thumbnail Image
    Item
    Lithium position and occupancy fluctuations in a cathode during charge/discharge cycling of lithium-ion battery
    (Australian Institute of Nuclear Science and Engineering (AINSE), 2012-11-07) Sharma, N; Yu, DH; Zhu, Y; Wu, Y; Peterson, VK
    Lithium-ion batteries are undergoing rapid development to meet the energy demands of the transportation and renewable energy-generation sectors. The capacity of a lithium-ion battery is dependent on the amount of lithium that can be reversibly incorporated into the cathode. Neutron diffraction provides greater sensitivity towards lithium relative to other diffraction techniques. In conjunction with the penetration depth afforded by neutron diffraction, the information concerning lithium gained in a neutron diffraction study allows commercial lithium-ion batteries to be explored with respect to the lithium content in the whole cathode. Furthermore, neutron diffraction instruments featuring area detectors that allow relatively fast acquisitions enable perturbations of lithium location and occupancy in the cathode during charge/discharge cycling to be determined in real time. Here, we present the time, current, and temperature dependent lithium transfer occurring within a cathode functioning under conventional charge-discharge cycling. The lithium location and content, oxygen positional parameter, and lattice parameter of the Li 1+yMn 2O4 cathode are measured and linked to the battery's charge/discharge characteristics (performance). We determine that the lithium-transfer mechanism involves two crystallographic sites, and that the mechanism differs between discharge and charge, explaining the relative ease of discharging (compared with charging) this material. Furthermore, we find that the rate of change of the lattice is faster on charging than discharging, and is dependent on the lithium insertion/ extraction processes (e.g. dependent on how the site occupancies evolve). Using in situ neutron diffraction data the atomic-scale understanding of cathode functionality is revealed, representing detailed information that can be used to direct improvements in battery performance at both the practical and fundamental level.
  • No Thumbnail Available
    Item
    Local vibrational mechanism for negative thermal expansion: a combined neutron scattering and first-principles study
    (Wiley-VCH Verlag Berlin, 2010-01-12) Peterson, VK; Kearley, GJ; Wu, Y; Ramirez-Cuesta, AJ; Kemner, E; Kepert, CJ
    Ask the locals: dynamic deformation of the dicopper tetracarboxylate paddlewheel unit within a metal-organic framework from square-prismatic to distorted occurs at very low energies. This deformation, which contributes strongly to the negative thermal expansion of this system, is a local vibration induced by a redistribution of electron density at the CuO junctions. © 2010, Wiley-VCH Verlag Berlin
  • No Thumbnail Available
    Item
    Negative thermal expansion in the metal-organic framework material Cu-3(1,3,5-benzenetricarboxylate)(2)
    (Wiley-VCH Verlag Berlin, 2008-08-08) Wu, Y; Kobayashi, A; Halder, GJ; Peterson, VK; Chapman, KW; Lock, N; Southon, PD; Kepert, CJ
    The metal–organic framework [Cu3(btc)2] displays negative thermal expansion (NTE) over a broad temperature range. This property arises from two coincident mechanisms, each of which are unique for NTE systems: the concerted transverse vibration of triangular organic linkers, and the local dynamic distortion of dinuclear metal centers within the framework lattice. © 2008, Wiley-VCH Verlag Berlin
  • No Thumbnail Available
    Item
    Non-equilibrium structural evolution of the lithium-rich Li1+yMn2O4 cathode within a battery
    (American Chemical Society., 2013-03-12) Sharma, N; Yu, DH; Zhu, Y; Wu, Y; Peterson, VK
    Lithium-ion batteries are undergoing rapid development to meet the energy demands of the transportation and renewable energy-generation sectors. The capacity of a lithium-ion battery is dependent on the amount of lithium that can be reversibly incorporated into the cathode. This work directly quantifies the time- and current-dependent lithium transfer within a cathode functioning under conventional charge?discharge cycling. We examine Li1+yMn2O4 under real working conditions using in situ neutron powder diffraction and link the atomic-scale structure to the battery performance. The lithium location and content, oxygen positional parameter, and lattice parameter of the cathode are measured and linked to the battery?s charge/discharge characteristics. Lithium insertion (discharge) differs from extraction (charge), a feature that may explain the relative ease of discharge (compared with charge) of this material. An atomic-scale understanding of cathode functionality, such as revealed here, will direct improvements in battery performance at both the practical and the fundamental level. © 2013, American Chemical Society.
  • No Thumbnail Available
    Item
    Scrutinizing negative thermal expansion in MOF-5 by scattering techniques and ab initio calculations
    (Royal Society of Chemistry, 2012-09-14) Lock, N; Christensen, M; Wu, Y; Peterson, VK; Thomsen, MK; Piltz, RO; Ramirez-Cuesta, AJ; McIntyre, GJ; Noren, K; Kutteh, R; Kepert, CJ; Kearley, GJ; Iversen, BB
    Complementary experimental techniques and ab initio calculations were used to determine the origin and nature of negative thermal expansion (NTE) in the archetype metal-organic framework MOF-5 (Zn4O(1,4-benzenedicarboxylate)3). The organic linker was probed by inelastic neutron scattering under vacuum and at a gas pressure of 175 bar to distinguish between the pressure and temperature responses of the framework motions, and the local structure of the metal centers was studied by X-ray absorption spectroscopy. Multi-temperature powder- and single-crystal X-ray and neutron diffraction was used to characterize the polymeric nature of the sample and to quantify NTE over the large temperature range 4-400 K. Ab initio calculations complement the experimental data with detailed information on vibrational motions in the framework and their correlations. A uniform and comprehensive picture of NTE in MOF-5 has been drawn, and we provide direct evidence that the main contributor to NTE is translational transverse motion of the aromatic ring, which can be dampened by applying a gas pressure to the sample. The linker motion is highly correlated rather than local in nature. The relative energies of different framework vibrations populated in MOF-5 are suggested by analysis of neutron diffraction data. We note that the lowest-energy motion is a librational motion of the aromatic ring which does not contribute to NTE. The libration is followed by transverse motion of the linker and the carboxylate group. These motions result in unit-cell contraction with increasing temperature. © 2012, Royal Society of Chemistry