B18-Core EXAFS
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Diamond Proposal Number(s):
[39528]
Open Access
Abstract: The accumulation of plastics such as polyethylene terephthalate (PET), Nylon 66, and polyurethane (PU) presents an environmental challenge that requires scalable circular solutions. Here, we report photoreforming (PR) of acid-hydrolyzed waste plastics into H2 and value-added products using an acid-stable photocatalyst composed of cyanamide-functionalized carbon nitride integrated with cobalt-promoted molybdenum disulfide (CoMoS2–CNx). Under AM 1.5G irradiation, CoMoS2–CNx yields 0.35 ± 0.02 mmol H2 gcat−1 from PET, increasing to 1.9 ± 0.1 mmol H2 gcat−1 under 405 nm LED (33 mW cm−2) irradiation. In 24 h, Nylon 66 and PU yield 1.0 ± 0.4 and 4.2 ± 0.1 mmol H2 gcat−1, respectively. From stability tests, the catalyst remains active over 11 days, affording up to 40% ethylene glycol conversion, 89% acetic acid selectivity, and a 9.0% quantum yield. Acid hydrolysis, enabled by recycled sulfuric acid from spent lead-acid batteries, underpins technoeconomic viability, indicating profitable solar-driven processing of ton-scale plastic waste.
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Apr 2026
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B18-Core EXAFS
I21-Resonant Inelastic X-ray Scattering (RIXS)
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Matthew J. W.
Ogley
,
Ashok S.
Menon
,
Gaurav C.
Pandey
,
Galo J.
Paez Fajardo
,
Beth J.
Johnston
,
Innes
Mcclelland
,
Veronika
Majherova
,
Steven
Huband
,
Debashis
Tripathy
,
Israel
Temprano
,
Stefano
Agrestini
,
Veronica
Celorrio
,
Gabriel E.
Perez
,
Samuel G.
Booth
,
Clare P.
Grey
,
Serena A.
Cussen
,
Louis F. J.
Piper
Diamond Proposal Number(s):
[33292, 33173]
Open Access
Abstract: This study refutes the commonly used ionic-bonding model that demarcates transition metal (TM) and oxygen redox using an archetypal Ni-rich layered oxide cathode, LiNi0.8Mn0.1Co0.1O2. Here, charge compensation during delithiation occurs without formal (ionic) Ni oxidation. Instead, oxygen-dominated states control the redox process, facilitated by strong TM-O hybridization, forming bulk-stable 3d8L and 3d8L2 electronic states, where L is a ligand hole. Bulk O–O dimers are observed with O K-edge resonant inelastic X-ray scattering but, critically, without the long-range TM migration or void formation observed in Li-rich layered oxides. Above 4.34 V vs. Li+/Li, the cathode loses O, forming a resistive surface rock-salt layer that causes capacity fade. This highlights the importance of cathode engineering when attempting to achieve higher energy densities with layered oxide cathodes, especially in those where O dominates the charge compensation mechanism.
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Oct 2024
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I12-JEEP: Joint Engineering, Environmental and Processing
I13-2-Diamond Manchester Imaging
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Bingkun
Hu
,
Shengming
Zhang
,
Ziyang
Ning
,
Dominic
Spencer-Jolly
,
Dominic L. R.
Melvin
,
Xiangwen
Gao
,
Johann
Perera
,
Shengda D.
Pu
,
Gregory J.
Rees
,
Longlong
Wang
,
Lechen
Yang
,
Hui
Gao
,
Shashidhara
Marathe
,
Genoveva
Burca
,
T. James
Marrow
,
Peter G.
Bruce
Diamond Proposal Number(s):
[26060, 30683, 28773]
Open Access
Abstract: Charging current densities of solid-state batteries with lithium metal anodes and ceramic electrolytes are severely limited due to lithium dendrites that penetrate the electrolyte leading to a short circuit. We show that dendrite growth can be inhibited by different crack deflection mechanisms when multi-layered solid electrolytes, such as Li6PS5Cl/Li3ScCl6/Li6PS5Cl and Li6PS5Cl/Li10GeP2S12/Li6PS5Cl, are employed but not when the inner layer is Li3PS4. X-ray tomographic imaging shows crack deflection along mechanically weak interfaces between solid electrolytes as a result of local mismatches in elastic moduli. Cracks are also deflected laterally within Li3ScCl6, which contains preferentially oriented particles. Deflection occurs without lithium being present. In cases where the inner layers react with lithium, the resulting decomposition products can fill and block crack propagation. All three mechanisms are effective at low stack pressures. Operating at 2.5 MPa, multi-layered solid electrolytes Li6PS5Cl/Li3ScCl6/Li6PS5Cl and Li6PS5Cl/Li10GeP2S12/Li6PS5Cl can achieve lithium plating at current densities exceeding 15 mA cm−2.
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Jul 2024
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I12-JEEP: Joint Engineering, Environmental and Processing
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Arthur
Fordham
,
Zoran
Milojevic
,
Emily
Giles
,
Wenjia
Du
,
Rhodri E.
Owen
,
Stefan
Michalik
,
Philip A.
Chater
,
Prodip K.
Das
,
Pierrot S.
Attidekou
,
Simon M.
Lambert
,
Phoebe K.
Allan
,
Peter R.
Slater
,
Paul A.
Anderson
,
Rhodri
Jervis
,
Paul R.
Shearing
,
Dan J. I.
Brett
Diamond Proposal Number(s):
[27719]
Open Access
Abstract: The growing demand for electric vehicles (EVs) continues to raise concern for the disposal of lithium-ion batteries reaching their end of life (EoL). The cells inside EVs age differently depending on multiple factors. Yet, following extraction, there are significant challenges with characterizing degradation in cells that have been aged from real-world EV usage. We employed four non-destructive techniques—infrared thermography, ultrasonic mapping, X-ray tomography, and synchrotron X-ray diffraction—to analyze the aging of Nissan Leaf large-format pouch cells that were arranged in different orientations and locations within the pack. The combination of these methods provided complementary insights into cell degradation, with rotated/vertically aligned cells exhibiting distinct aging patterns compared with flat/horizontally aligned cells. These findings offer valuable information for pack design and demonstrate how cost-effective non-destructive techniques can provide practical assessment capabilities comparable to synchrotron studies. This approach enables decision support during EoL, enhancing battery production efficiency and minimizing material waste.
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Nov 2023
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I12-JEEP: Joint Engineering, Environmental and Processing
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Dominic
Spencer-Jolly
,
Varnika
Agarwal
,
Christopher
Doerrer
,
Bingkun
Hu
,
Shengming
Zhang
,
Dominic L. R.
Melvin
,
Hui
Gao
,
Xiangwen
Gao
,
Paul
Adamson
,
Oxana
Magdysyuk
,
Patrick S.
Grant
,
Robert A.
House
,
Peter G.
Bruce
Diamond Proposal Number(s):
[26082]
Open Access
Abstract: Ag-carbon composite interlayers have been reported to enable Li-free (anodeless) cycling of solid-state batteries. Here, we report structural changes in the Ag-graphite interlayer, showing that on charge, Li intercalates electrochemically into graphite, subsequently reacting chemically with Ag to form Li-Ag alloys. Discharge is not the reverse of charge but rather passes through Li-deficient Li-Ag phases. At higher charging rates, Li intercalation into graphite outpaces the chemical reactions with Ag, delaying the formation of the Li-Ag phases and resulting in more Li metal deposition at the current collector. At and above 2.5 mA·cm−2, Li dendrites are not suppressed. Ag nanoparticles do not suppress dendrites more effectively than does an interlayer of graphite alone. Instead, Ag in the carbon interlayer results in more homogeneous Li and Li-Ag formation on the current collector during charge.
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Feb 2023
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E02-JEM ARM 300CF
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Diamond Proposal Number(s):
[22479]
Open Access
Abstract: Li-rich metal oxides, such as Li1.2Ni0.13Mn0.54Co0.13O2, can deliver high specific capacities because of the redox of lattice O2− in addition to the cations. Observing oxygen distortions is key to understand the redox process. Electron ptychography is a phase-reconstruction method in 4D scanning transmission electron microscopy, providing atomic-resolution phase images with high signal-to-noise ratio and dose efficiency. Herein, we use electron ptychography to image the oxygen shift in Li1.2Ni0.13Mn0.54Co0.13O2 during the first cycle. The picometer-scale precision measurement shows distinct oxygen shifts in the bulk and surface after charging and compares with various theoretical anionic redox models. The shift after discharging is not seen to recover in the bulk accounting for voltage hysteresis; however, it recovers close to the surface, although with a phase change. We suggest that Li1.2Ni0.13Mn0.54Co0.13O2 proceeds distinct oxygen redox in the bulk and surface. The altered oxygen sublattice after first cycle potentially explains the changed voltage profiles of following cycles.
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May 2022
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Abstract: Advanced batteries are critical to achieving net zero and are proposed within decarbonization strategies for transport and grid-scale applications, alongside their ubiquitous application in consumer devices. Immense progress has been made in lithium battery technology in recent years, but significant challenges remain and new development strategies are required to improve performance, fully exploit power density capacities, utilize sustainable resources, and lower production costs. Suitable characterization techniques are crucial for understanding, inter alia, three-dimensional (3D) diffusion processes and formation of passivation layers or dendrites, which can lead to drastic capacity reduction and potentially to hazardous short circuiting. Studies of such phenomena typically utilize 2D or 3D imaging techniques, providing locally resolved information. 3D X-ray imaging is a widely used standard method, while time-lapse (4D) tomography is increasingly required for understanding the processes and transformations in an operational battery. Neutron imaging overcomes some of the limitations of X-ray tomography for battery studies. Notably, the high visibility of neutrons for light-Z elements, in particular hydrogen and lithium, enables the direct observation of lithium diffusion, electrolyte consumption, and gas formation in lithium batteries. Neutron imaging as a non-destructive analytical tool has been steadily growing in many disciplines as a result of improvements to neutron detectors and imaging facilities, providing increasingly higher spatial and temporal resolutions. Further, ongoing developments in diffraction imaging for mapping the structural and microstructural properties of battery components make the use of neutrons increasingly attractive. Here, we provide an overview of neutron imaging techniques, generally outlining advances and limitations for studies on batteries and reviewing imaging studies of lithium batteries. We conclude with an outlook on development methods in the field and discuss their potential and significance for future battery research.
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Jan 2022
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B18-Core EXAFS
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Abstract: O-redox in compounds with Li on the transition-metal layers (TML) has recently been attributed to the formation of molecular O2 on charge, trapped in the lattice. Here, we show that a similar process occurs for P2-Na0.67[Mn0.72Mg0.28]O2, which contains Mg2+ on the TML. The molecular O2 is identified by high-resolution RIXS and quantified by magnetometry, showing that it equates to the charge passed. This O2 is trapped in voids that are formed by Mg2+ out-of-plane displacement and Mn4+ in-plane disordering and is then reduced on discharge associated with a large voltage hysteresis. In contrast to compounds containing Li+ in the TML, in which the honeycomb ordering and the high-voltage plateau are irreversibly lost after the first cycle, in P2-Na0.67[Mn0.72Mg0.28]O2, the plateau reappears partially on the second charge due to the partial reversibility of Mn in-plane and Mg out-of-plane migration and the local reformation of the honeycomb ordering.
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May 2021
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I13-2-Diamond Manchester Imaging
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Diamond Proposal Number(s):
[4999]
Abstract: Alternative battery technologies are required to meet growing energy demands and address the limitations of present technologies. As such, it is necessary to look beyond lithium-ion batteries. Zinc batteries enable high power density while being sourced from ubiquitous and cost-effective materials. This paper presents, for the first time known to the authors, multi-length scale tomography studies of failure mechanisms in zinc batteries with and without commercial microporous separators. In both cases, dendrites were grown, dissolved, and regrown, critically resulting in different morphology of dendritic layer formed on both the electrode and the separator. The growth of dendrites and their volume-specific areas were quantified using tomography and radiography data in unprecedented resolution. High-resolution ex situ analysis was employed to characterize single dendrites and dendritic deposits inside the separator. The findings provide unique insights into mechanisms of metal-battery failure effected by growing dendrites.
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Dec 2018
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I07-Surface & interface diffraction
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Wei
Li
,
Mengxue
Chen
,
Jinlong
Cai
,
Emma L. K.
Spooner
,
Huijun
Zhang
,
Robert S.
Gurney
,
Dan
Liu
,
Zuo
Xiao
,
David G.
Lidzey
,
Liming
Ding
,
Tao
Wang
Diamond Proposal Number(s):
[20419]
Abstract: Adjusting molecular ordering, orientation, and nanoscale morphology within the photoactive layer of polymer:non-fullerene organic solar cells is crucial in achieving high power-conversion efficiency (PCE). Herein, we demonstrate that the molecular ordering and orientation of the n-type small-molecule acceptor COi8DFIC can be tuned from flat-on and edge-on lamellar crystalline to H- and J-type π-π stacking during the solution-casting process, resulting in broadened photon absorption and fine phase separation with the electron donor PTB7-Th. This favorable morphology with face-on π-π stacked electron donors and acceptors promotes efficient exciton dissociation at the donor/acceptor interface, together with enhanced and balanced carrier mobility. The enhanced short-circuit current density and fill factor lead to the achievement of a maximum PCE of 13.8% in binary, single-junction PTB7-Th:COi8DFIC non-fullerene polymer solar cells while also exhibiting superior stability.
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Dec 2018
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