Article
Energy & Fuels
Nitheesha Shaji, Feng Jiang, Jae Yoon Sung, Murugan Nanthagopal, Taehyung Kim, Byeong Jin Jeong, Soon Phil Jung, Chang Woo Lee
Summary: This study focuses on surface modification of LiFePO4 (LFP) cathode material for lithium-ion batteries (LIBs) using heteroatoms-doped carbon. The results demonstrate that the nitrogen and sulfur dual-doped carbon coating layer enhances the electrochemical activity, cycling stability, and rate capability of the NSC@LFP cathode.
JOURNAL OF ENERGY STORAGE
(2023)
Article
Multidisciplinary Sciences
Weixuan Xu, Shuangyan Lang, Kaiyang Wang, Rui Zeng, Huiqi Li, Xinran Feng, Mihail R. Krumov, Seong-Min Bak, Christopher J. Pollock, Jingjie Yeo, Yonghua Du, Hector D. Abruna
Summary: This study comprehensively investigates the catalytic mechanisms of a cobalt single-atom electrocatalyst on the redox processes of lithium-sulfur batteries using operando techniques. Real-time observations reveal that the electrocatalyst efficiently accelerates the lithium-sulfur reactions with zero-order kinetics. Under galvanostatic discharge conditions, the catalysis transforms the typical stepwise mechanism of the reactions to a concurrent pathway. Additionally, operando XAS studies elucidate the potential-dependent evolution of cobalt's oxidation state and the formation of cobalt-sulfur bonds.
Article
Mineralogy
Michael C. Jollands, Peter M. E. Tollan, Lukas P. Baumgartner, Othmar Muentener
Summary: The diffusivity and diffusion mechanisms of hydrogen, deuterium, and lithium in quartz were investigated, and a multi-site diffusion-reaction model was proposed to explain the complex diffusion profiles observed under different experimental conditions.
MINERALOGICAL MAGAZINE
(2022)
Article
Chemistry, Multidisciplinary
Martin T. Peschel, Piotr Kabacinski, Daniel P. Schwinger, Erling Thyrhaug, Giulio Cerullo, Thorsten Bach, Juergen Hauer, Regina de Vivie-Riedle
Summary: Lewis acids have been recognized as catalysts for enantioselective photochemical transformations, but mechanistic studies on these systems are rare. This work overcomes the challenges by using sub-30-fs transient absorption in the UV and accurate theoretical treatment. Investigations on the 2-cyclohexenone and boron trifluoride complex reveal that the Lewis acid remains attached to the substrate in the triplet state, leading to high enantioselectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Engineering, Environmental
Yufan Chen, Christopher J. Miller, T. David Waite
Summary: The study found that the adsorption and decomposition of formate and H2O2 in the presence of freshly formed ferrihydrite are controlled by surface-initiated reactions, affecting the surface Fenton reactions. Oxidation mainly occurs in the solid-liquid boundary layer, rather than in bulk or on the surface.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Multidisciplinary
Sohini Sarkar, Anwesha Maitra, William R. Lake, Robert E. Warburton, Sharon Hammes-Schiffer, Jahan M. Dawlaty
Summary: Proton-coupled electron transfer (PCET) is a fundamental step in electrochemical processes, and combining a proton donor with a vibrational Stark-shift probe can provide critical insight into the interplay between interfacial electrostatics and heterogeneous chemical reactions. The study identified three main stages of the PCET reaction and showed that the progress of the reaction is dependent on the applied potential.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Energy & Fuels
Yutong Liu, Jixi Zhang, Nataraju Bodappa, Rodney D. L. Smith
Summary: Combining Raman spectroscopy with traditional thermal analysis provides insights into the formation of α-Fe2O3, with protohematite formed between 200 and 400 degrees Celsius showing a significant impact on photoelectrocatalytic performance.
JOURNAL OF PHYSICS-ENERGY
(2021)
Article
Materials Science, Ceramics
Gui-Yang Luo, Yi-Jing Gu, Yuan Liu, Zi-Liang Chen, Yong-lin Huo, Fu-Zhong Wu, Yi Mai, Xin-Yi Dai, Yong Deng
Summary: LiFePO4 modified by N-doped graphene with a three-dimensional conductive network structure exhibits excellent electrochemical performance, making it a promising cathode material for Li-ion batteries.
CERAMICS INTERNATIONAL
(2021)
Review
Chemistry, Multidisciplinary
Ze-Cheng Yao, Tang Tang, Zhe Jiang, Lu Wang, Jin-Song Hu, Li-Jun Wan
Summary: This review discusses the challenges and solutions in catalyst design and performance optimization of the hydrogen oxidation reaction (HOR) in anion-exchange membrane fuel cells, focusing mainly on the research of anodic catalysts and emphasizing the unclear mechanism of alkaline HOR and the importance of antioxidation capability.
Article
Chemistry, Physical
Tingting Qin, Wenli Zhang, Yue Ma, Wei Zhang, Taowen Dong, Xianyu Chu, Tian Li, Zizhun Wang, Nailin Yue, Hongyan Liu, Lirong Zheng, Xiaofeng Fan, Xingyou Lang, Qing Jiang, Weitao Zheng
Summary: In this study, the interaction mechanism between bismuth (Bi) and alkali metal ions (Li+, Na+ and K+) in aqueous alkali-metal ion batteries (ARABs) was investigated using various experimental and theoretical methods. It was found that Bi exhibited high specific capacity for Na+ and K+ storage, but lower capacity for Li+ storage. The irreversibility of Li+ dealloying from Bi matrix due to large adsorption energy resulted in poor rate performance and cycling stability. The large volume expansion caused by the largest radius of K+ contributed to the poor cycling stability for K+ storage. Bi showed superior performance for Na+ storage due to the appropriate interaction strength between Bi and Na+.
ENERGY STORAGE MATERIALS
(2022)
Article
Chemistry, Physical
Baoquan Zhang, Shuzhong Wang, Lu Liu, Yanhui Li, Jianqiao Yang
Summary: LiFePO4/N-doped C composites with core-shell structures were synthesized using a solvothermal method, with CTAB and glucose as nitrogen and carbon sources. The presence of N atoms in pyridinic and graphitic forms in the carbon of LiFePO4/N-doped C enhanced the cathode's capacity performance. The electrochemical tests revealed a synergistic effect between N-doping and core-shell structure in improving the electrochemical performance of the cathode.
Article
Energy & Fuels
Sina Karimzadeh, Babak Safaei, Wei Huang, Tien-Chien Jen
Summary: In this study, first principle calculations were performed to investigate the properties of LiFePO4 (LFP) cathode material for Li-ion batteries and the effects of Nb doping on its crystalline structure. The results revealed that Nb doping at the Fe site significantly improved the conductivity of LFP, reduced the band gap, and enhanced the stability of the system. Geometrical analysis showed that Nb doping widened the Li passage channel, increased bond length, and reduced covalent strength, leading to a lower energy barrier for Li ion diffusion. Moreover, Nb doping had no adverse effect on the theoretical voltage of LFP. The findings also demonstrated that Nb doping decreased the energy barriers for Li migration and significantly improved the diffusion coefficient of Li-ion in LFP.
JOURNAL OF ENERGY STORAGE
(2023)
Article
Chemistry, Physical
E. Read, B. Lonetti, S. Gineste, A. T. Sutton, E. Di Cola, P. Castignolles, M. Gaborieau, A. -F. Mingotaud, M. Destarac, J. -D. Marty
Summary: The study focuses on investigating the structural changes of polyion complexes (PICs) composed of thermoresponsive polymers with temperature variations, and suggests that the polymer structure and PICs composition play a crucial role in the observed modifications.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2021)
Article
Engineering, Environmental
Sieon Jung, Raja Arumugam Senthil, Cheol Joo Moon, Natalie Tarasenka, Ahreum Min, Seung Jun Lee, Nikolai Tarasenko, Myong Yong Choi
Summary: A bifunctional electrocatalyst based on Ir-doped Co3O4-anchored N-doped carbon (IrCo3O4@NC) hybrid was successfully synthesized and showed excellent catalytic activity for overall water splitting. This research provides a viable bifunctional electrocatalyst for hydrogen production.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Physical
Y. Zhou, N. Emery, S. Franger, O. Nguyen, J. P. Pereira-Ramos, R. Baddour-Hadjean
Summary: The kinetics of electrochemical lithium intercalation in nitridonickelate is studied, and the results indicate reversible and stable capacity, as well as stable impedance during long cycling, highlighting the good chemical and structural stability of the material.
JOURNAL OF POWER SOURCES
(2022)
Article
Chemistry, Multidisciplinary
Josefine Sprachmann, Tommy Wachsmuth, Manik Bhosale, David Burmeister, Glen J. Smales, Maximilian Schmidt, Zdravko Kochovski, Niklas Grabicki, Robin Wessling, Emil J. W. List-Kratochvil, Birgit Esser, Oliver Dumele
Summary: Despite being unstable, 4n pi systems have gained attention for their unique optical and electronic properties. The first antiaromatic framework materials were synthesized and a series of highly crystalline and porous COFs based on DBP were obtained. These antiaromatic COFs show potential applications in positive electrode materials for Li-organic batteries and exhibit photoconductivity upon visible light irradiation.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Stephanos Karafiludis, Ana Guilherme Buzanich, Christian Heinekamp, Annett Zimathies, Glen J. Smales, Vasile-Dan Hodoroaba, Johan E. ten Elshof, Franziska Emmerling, Tomasz M. Stawski
Summary: We demonstrate a template-free method for engineering mesoporosity in transition metal phosphate materials. By thermally decomposing M-struvite precursors, we obtained amorphous and mesoporous phases with different structures depending on the transition metal involved. The resulting structures exhibit high surface areas and pore volumes, making them suitable for potential applications in (electro)catalysis. This environmentally friendly approach could utilize waste products from industrial and agricultural wastewaters as recycling sources.
Article
Nanoscience & Nanotechnology
Kinanti Aliyah, Christian Prehal, Justus S. Diercks, Natasa Diklic, Linfeng Xu, Secil Uensal, Christian Appel, Brian R. Pauw, Glen J. Smales, Manuel Guizar-Sicairos, Juan Herranz, Lorenz Gubler, Felix N. Buchi, Jens Eller
Summary: A method using small-angle X-ray scattering (SAXS) is proposed to quantify the presence of liquid water in polymer electrolyte fuel cell (PEFC) catalyst layers (CLs). The method is validated through wetting experiments and allows for interpretation of the measured SAXS data to derive the most probable wetting mechanism in a flow cell electrode.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Innes McClelland, Samuel G. Booth, Nirmalesh N. Anthonisamy, Laurence A. Middlemiss, Gabriel E. Perez, Edmund J. Cussen, Peter J. Baker, Serena A. Cussen
Summary: Ni-rich layered oxide cathodes, such as LiNi0.8Mn0.1Co0.1O2 (NMC811), have high capacities but suffer from irreversible first cycle capacity loss due to slow Li+ diffusion kinetics at a low state of charge. This study develops operando muon spectroscopy (mu SR) to investigate Li+ ion diffusion in NMC811 during the first cycle and compares it with electrochemical impedance spectroscopy (EIS) and galvanostatic intermittent titration technique (GITT). The results reveal that sluggish surface diffusion is likely the cause of first cycle irreversible capacity loss, and demonstrate the sensitivity of mu SR parameter to structural changes during cycling.
CHEMISTRY OF MATERIALS
(2023)
Article
Nanoscience & Nanotechnology
Fiona C. Coomer, Heather M. Mutch, Otto Mustonen, Charlotte Pughe, Serena A. Cussen, Silvia Ramos, Adrian D. Hillier, Edmund J. Cussen
Summary: New and exotic ground states of magnetic materials are highly sought after and extensively studied for their insights into the thermodynamics of disorder and fundamental magnetic interactions. By controlling the crystal structure of an appropriate magnetic lattice, it is possible to induce frustration in strong magnetic exchange interactions. These finely balanced systems offer a way of probing classical or quantum mechanical interactions that are of fundamental importance but are too weak to be observed in non-frustrated systems.
Article
Electrochemistry
Laura Wheatcroft, Arron Bird, Joe C. Stallard, Ria L. Mitchell, Samuel G. Booth, Alisyn J. Nedoma, Michael F. L. De Volder, Serena A. Cussen, Norman A. Fleck, Beverley J. Inkson
Summary: Fracture of cathode secondary particles is a critical degradation mechanism in lithium-ion batteries. In this study, the microindentation strength of LiNi0.8Mn0.1Co0.1O2 secondary particles was measured in situ in the scanning electron microscope (SEM) to visualize the fracture process. The results showed that crack propagation occurred between primary particles when compressed between flat platens, and directly beneath the cono-spherical tip and at the center of secondary particles when compressed between flat platens. Finite element modelling provided insights into the relationship between fracture load and cohesive strength and particle toughness.
BATTERIES & SUPERCAPS
(2023)
Article
Nanoscience & Nanotechnology
Hany El-Shinawi, Ed Darnbrough, Johann Perera, Innes McClelland, David E. J. Armstrong, Edmund J. Cussen, Serena A. Cussen
Summary: Deformable, fast-ion conducting sulfides make it possible to create bulk-type solid-state batteries that can rival current Li-ion batteries in terms of energy density and scalability. One way to optimize the energy density of these batteries is to minimize the size of the electrolyte layer by integrating the solid electrolyte into thin membranes. However, it is difficult to prepare or integrate additive-free thin membranes or membranes based on preprepared scaffolds on a large scale. In this study, a scalable solution-based approach is proposed to produce glass microfiber-reinforced composites that restore the deformability of sulfide electrolytes and can easily be shaped into thin membranes through cold pressing. This approach enables easy preparation and enhances the energy density of sulfide-based solid-state batteries.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Samuel W. Coles, Viktoria Falkowski, Harry S. Geddes, Gabriel E. Perez, Samuel G. Booth, Alexander G. Squires, Conn O'Rourke, Kit McColl, Andrew L. Goodwin, Serena A. Cussen, Simon J. Clarke, M. Saiful Islam, Benjamin J. Morgan
Summary: Short-range ordering in cation-disordered cathodes can have a significant effect on their electrochemical properties. We characterise the cation short-range order in Li2FeSO and find that the preference for polar cation configurations produces long-range disorder, in contrast to the predictions of a simple point-charge model, which instead suggests long-range crystallographic order. The absence of long-range order in Li2FeSO can be attributed to the relative stability of certain oxygen-coordination motifs.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Farzad Foroutan, Benjamin A. Kyffin, Athanasios Nikolaou, Jorge Merino-Gutierrez, Isaac Abrahams, Nasima Kanwal, Jonathan C. Knowles, Andrew J. Smith, Glen J. Smales, Daniela Carta
Summary: Mesoporous glasses with high surface area and extended porosity are ideal for controlled release of therapeutic ions and molecules. In this study, mesoporous phosphate-based glasses doped with copper ions were synthesized and their structures were characterized. The copper-doped glasses showed significant antibacterial properties and potential for controlled delivery of antibacterial ions.
Article
Chemistry, Physical
Wenke Mueller, Ralf Schweins, Bernd Noecker, Joachim Kohlbrecher, Glen J. Smales, Klaus Huber
Summary: The co-assembly of three one-fold negatively charged 3-chloro-4-hydroxy-phenylazo dyes with the cationic surfactant DTAB was investigated. Different phase separations and crystalline dye-DTAB complexes were observed for each dye, with varying stoichiometries in homogeneous solution. The observed stoichiometries are inversely correlated to the impact dye addition has on the morphology of DTAB micelles.
Review
Chemistry, Physical
Gabriel E. Perez, Jake M. Brittain, Innes McClelland, Stephen Hull, Martin O. Jones, Helen Y. Playford, Serena A. Cussen, Peter J. Baker, Emily M. Reynolds
Summary: Neutron and muon characterisation techniques have unique capabilities for studying the complex structure and dynamics of rechargeable battery systems. The neutron's interaction with atomic nuclei enables it to detect light elements and its weak interaction allows it to penetrate deep into the sample, while the non-invasive nature of the implanted positive muon makes it a probe for studying ionic diffusion phenomena at different depths. This review discusses the application of these techniques in ion battery research and provides an accessible overview of their working principles.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Materials Science, Multidisciplinary
Robert D. Hunter, Emily C. Hayward, Glen J. Smales, Brian R. Pauw, A. Kulak, Shaoliang Guan, Zoe Schnepp
Summary: This study investigates the impact of nitrogen on iron-catalyzed graphitization of biomass. Various nitrogen-rich saccharides and amino-acid/polypeptide biomass precursors were pyrolyzed using an iron catalyst, resulting in carbons with different chemical and structural characteristics. While nitrogen was found to inhibit graphitization, some nitrogen did survive the catalytic graphitization process and became incorporated into different chemical environments in the carbon product.
MATERIALS ADVANCES
(2023)
Article
Chemistry, Multidisciplinary
Josefine Sprachmann, Tommy Wachsmuth, Manik Bhosale, David Burmeister, Glen J. Smales, Maximilian Schmidt, Zdravko Kochovski, Niklas Grabicki, Robin Wessling, Emil J. W. List-Kratochvil, Birgit Esser, Oliver Dumele
Summary: In recent years, 4n pi systems have attracted significant attention due to their unique optical and electronic properties. We synthesized the first antiaromatic framework materials based on dibenzopentalene and obtained highly crystalline and porous covalent organic frameworks (COFs). These COFs exhibit excellent conductivity and photoconductivity, and show enhanced performance as positive electrode materials in Li-organic batteries.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Beth I. J. Johnston, Innes Mcclelland, Peter J. Baker, Serena A. Cussen
Summary: Understanding the Li-ion transport properties is crucial for optimizing the electrochemical performance of Ni-rich cathodes for high energy density Li-ion batteries.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Josefine Sprachmann, Niklas Grabicki, Anna Moeckel, Jeremy Maltitz, Jose Refugio Monroy, Glen J. Smales, Oliver Dumele
Summary: In this study, the synthesis of COFs using substituted benzophenones was investigated. It was found that all substituted benzophenone imines can be used in COF synthesis, leading to high crystallinity and porosity.
CHEMICAL COMMUNICATIONS
(2023)