Article
Chemistry, Multidisciplinary
Xiangsi Liu, Ziteng Liang, Yuxuan Xiang, Min Lin, Qi Li, Zigeng Liu, Guiming Zhong, Riqiang Fu, Yong Yang
Summary: The recent applications of solid-state nuclear magnetic resonance (ssNMR) and magnetic resonance imaging (MRI) techniques in Li/Na batteries are reviewed, emphasizing the importance of investigating battery materials structure, solid electrolyte interfaces, and in situ research.
ADVANCED MATERIALS
(2021)
Review
Electrochemistry
Yao Liu, Wei Li, Yongyao Xia
Summary: While carbon, oxide, and silicon-based materials have limitations in current LIB applications, polyanionic compounds have gained attention for their ability to stabilize structures, adjust redox couples, and provide migration channels for guest ions, leading to electrode materials with long-term cycling, high energy density, and outstanding rate capability.
ELECTROCHEMICAL ENERGY REVIEWS
(2021)
Article
Nanoscience & Nanotechnology
Mewin Vincent, Damian Kowalski
Summary: Anodizing is a powerful method to form electrochemically active materials, such as self-organized TiO2 nanotubes (TiNTs), which are highly interesting in battery field due to their unique 1D geometry and high volume expansion tolerance. A Raman spectroscopy study under current control was conducted to investigate Li+/Na+ storage in TiNTs. Real-time measurements revealed sequential phase transformations during lithium intercalation and slight crystallinity rupture during sodium-ion insertion, providing insights for further scale-up and application of TiNTs as negative electrodes in lithium-ion batteries.
ACS APPLIED NANO MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Jie Liu, Yanan Gao, Chenjie Lou, Yongjin Chen, Xiang Gao, Ligang Xu, Qi Wei, Guangcan Bai, Guoquan Liu, Mingxue Tang
Summary: Hybrid architectures integrating Fe7S8@NC@MoS2 with a three-dimensional heterostructure are designed in this study. The adjustable voids of the material can buffer the volume change during intercalation of metal ions. Additionally, the presence of MoS2 enhances electronic conductivity and metal ion transfer, resulting in improved battery performance.
ACS MATERIALS LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Yinger Xiang, Xinyu Hu, Xue Zhong, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Xiaobo Ji
Summary: This study proposes a strategy of hierarchical double carbon/Sb composite to enhance the performance of Sb anode. The composite employs carbon spheres to encapsulate Sb nanoparticles with strong interfacial chemical bonds, and utilizes graphene as a conductive network to connect the composite materials. The hierarchical double carbon/Sb composite shows excellent rate and long cycling performance, and provides theoretical guidance for the development of metal anodes.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
U. Younis, I. Muhammad, F. Qayyum, W. Wu, Q. Sun
Summary: A novel two-dimensional pentadiamond monolayer C-558 composed of pentagons and octagons is proposed, showing metallic properties and high ion adsorption sites, suitable for high-performance lithium, sodium, and potassium ion batteries.
MATERIALS TODAY ENERGY
(2021)
Article
Chemistry, Physical
Shao-Fei Wang, Bao-Tian Wang, Tao Bo, Jun-Rong Zhang, Fang-Wei Wang
Summary: The Ti2B monolayer, based on first-principles calculations, shows high capacity and low diffusion barriers compared with other materials, indicating high structural stability and steady metallic character. The magnetic effects in the ground state of ferromagnetism impact thermal stability, charge transfer, ion diffusion, operating voltage and storage capacity.
APPLIED SURFACE SCIENCE
(2021)
Article
Chemistry, Physical
Yunjung Kim, Kyungbae Kim, Hyungeun Seo, Sung-Min Lee, Cheol-Min Park, Jae-Hun Kim
Summary: The study introduces a porous Sn2Nb2O7-graphene oxide composite material as an anode material for both lithium-ion and sodium-ion batteries, showing high reversible capacity and cycling stability. The enhanced electrode performance is attributed to the combination of porous structure and graphene oxide.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Chemistry, Multidisciplinary
Qiong Peng, Javed Rehman, Kamel Eid, Ayman S. Alofi, Amel Laref, Munirah D. Albaqami, Reham Ghazi Alotabi, Mohamed F. Shibl
Summary: This study utilizes density-functional theory to investigate the performance of V4C3 MXene as an anode for Li-ion batteries and Na-ion batteries. The results show that V4C3 exhibits excellent electrical conductivity, low voltages, and good storage capacity and cycling performance, suggesting its potential application in future ion batteries.
Article
Chemistry, Multidisciplinary
Darren M. C. Ould, Svetlana Menkin, Christopher A. O'Keefe, Fazlil Coowar, Jerry Barker, Clare P. Grey, Dominic S. Wright
Summary: This study presents a new method for synthesizing high-purity sodium hexafluorophosphate for electrolytes in sodium-ion batteries, which is purer than commercial materials. Experimental results indicate that higher concentrations of electrolyte are beneficial for the degradation dynamics of the sodium metal-electrolyte interface, potentially improving battery performance.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Hae-Ri Yang, Youngmo Yang, Hyungeun Seo, Kyungbae Kim, Hyun Seung Lee, Jaegab Lee, Jae-Hun Kim
Summary: In this study, carbon-coated SnS nanosheets were proposed as anodes for Li- and Na-ion batteries on flexible carbon foam composite materials, demonstrating good electrochemical performance. The flexibility of the electrode was ensured by the flexible carbon foam substrate without any conducting agent and binder.
APPLIED SURFACE SCIENCE
(2021)
Article
Electrochemistry
Bo Han, Shuangqiang Chen, Chaofei Guo, Minghong Wu, Yong Wang
Summary: This study designed alumina-coated electrodes with iron sulfide/molybdenum disulfide yolk-shell structure, successfully addressing the challenges faced by transition metal sulfides in alkaline ion batteries and achieving higher reversible capacities and better electrochemical performance.
ELECTROCHIMICA ACTA
(2022)
Article
Chemistry, Physical
Darshil Chodvadiya, Ujjawal Jha, Piotr Spiewak, Krzysztof J. Kurzydlowski, Prafulla K. Jha
Summary: In this study, the applicability of the h-AlC monolayer as an anode material was investigated using first principles based density functional theory. It was found that the h-AlC monolayer exhibited excellent metallic behavior and high storage capacity for Li and Na ions. The diffusion barrier for Li and Na ions on the h-AlC monolayer was also found to be favorable. This research provides valuable experimental work for the future storage mechanisms of lithium-ion batteries and sodium-ion batteries.
APPLIED SURFACE SCIENCE
(2022)
Article
Chemistry, Multidisciplinary
Shuang Li, Yipeng Sun, Ning Li, Wei Tong, Xueliang Sun, Charles T. Black, Sooyeon Hwang
Summary: In this study, two different types of porous structures in high-voltage lithium, manganese-rich layered cathodes are revealed, along with the significance of the interface between the cathode and electrolyte in solid-state batteries. Nanopores are found near the interface, while nanovoids are formed during in situ Li+ extraction. Despite the development of nanovoids, the layered structure is preserved.
Article
Engineering, Multidisciplinary
Vinoth Ganesan, Do-Hyeon Kim, Ki-Hun Nam, Cheol-Min Park
Summary: A robust hierarchical nanocube framework CoS2-C-CNT composite with nanocrystalline CoS2 encapsulated in a carbon matrix entangled in carbon nanotubes was synthesized and showed superior Li/Na-ion storage performances, delivering large reversible capacity, excellent cycling, and fast rate behavior during insertion and extraction processes.
COMPOSITES PART B-ENGINEERING
(2022)
Review
Chemistry, Multidisciplinary
Zongyan Gao, Israel Temprano, Jiang Lei, Linbin Tang, Junjian Li, Clare P. Grey, Tao Liu
Summary: This article reviews the development of LiOH-based nonaqueous lithium-air batteries (LABs). Various catalytic systems that can activate LiOH-based electrochemistry are compared, with a focus on the oxygen reduction and evolution reactions in nonaqueous media. Key factors that can switch the cell chemistry between Li2O2 and LiOH are identified, and the debate and potential causes for opposing opinions are discussed.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Angela F. F. Harper, Steffen P. P. Emge, Pieter C. M. M. Magusin, Clare P. P. Grey, Andrew J. J. Morris
Summary: Understanding the electronic structure of materials is vital for the development of functional devices such as semiconductors, solar cells, and Li-ion batteries. However, the disorder in atomic arrangement poses challenges in determining the structure and properties of amorphous materials. In this study, we propose a method to develop amorphous models by combining experimental techniques like solid-state NMR and XAS with ab initio molecular dynamics simulations. We apply this method to amorphous alumina and successfully predict its atomic arrangement and electronic density of states. This work represents a significant advancement in the field of solid-state amorphous modeling.
Article
Chemistry, Physical
Zachary Ruff, Chloe S. Coates, Katharina Marker, Amoghavarsha Mahadevegowda, Chao Xu, Megan E. Penrod, Caterina Ducati, Clare P. Grey
Summary: Nickel-rich layered oxide cathodes like NMC811 have high practical capacities, approaching 200 mAh/g. Delithiation of NMC811 results in a solid-solution behavior, maintaining the same layered structure. However, further delithiation is kinetically challenging and there are side reactions between the electrolyte and cathode surface.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Nadia L. Farag, Rajesh B. Jethwa, Alice E. Beardmore, Teresa Insinna, Christopher A. O'Keefe, Peter A. A. Klusener, Clare P. Grey, Dominic S. Wright
Summary: A series of triarylamines were synthesized and tested as catholytes in all-aqueous redox flow batteries. Tris(4-aminophenyl)amine showed the highest potential as a candidate. However, polymerization occurred during electrochemical cycling, leading to a decrease in active material and limitation in ion transport. The use of a mixed electrolyte system of H3PO4 and HCl inhibited polymerization, resulting in improved electrochemical performance.
Article
Chemistry, Physical
Evelyna Wang, Erlendur Jonsson, Clare P. Grey
Summary: Similar to fuel cells, the poor mass transport of redox active species is a challenge for lithium-air batteries (LABs). In this study, nuclear magnetic resonance (NMR) spectroscopy was used to measure the concentration and transport of oxygen in LAB electrolytes, and the results were compared with values obtained from electrochemical or pressure methods. The NMR methodology was successfully used to quantify O-2 in LAB electrolytes, experimentally demonstrate solvation environments of O-2, and detect O-2 evolution in situ in a LAB flow cell.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Jennifer P. Allen, Christopher A. O'Keefe, Clare P. Grey
Summary: Transition metal dissolution is a major cause of capacity fade in lithium-ion cells, and nuclear magnetic relaxation rates can be used to quantify dissolved transition metals in battery electrolytes. This study measured relaxation rates of Li-7, P-31, F-19, and H-1 to investigate the presence of transition metals in LiPF6 electrolyte solutions. Sensitivities varied depending on the nuclide and transition metal, with F-19 and H-1 measurements showing higher sensitivity. The quantification method was found to be accurate except for heat-degraded LiPF6 electrolytes. Rating: 7/10
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Jennifer P. Allen, Clare P. Grey
Summary: NMR spectroscopy is used to evaluate the degradation of lithium-ion battery electrolyte solutions, but the presence of paramagnetic ions from cathode materials can affect the NMR spectra by inducing spectral broadening. This study investigates the effects of Ni2+ and Mn2+ on the NMR spectra of electrolyte solutions and finds that Mn2+ causes greater peak broadening than Ni2+. The 19F peaks from PF6- degradation species are most affected, followed by 31P and 1H peaks. The degree of broadening also depends on the solvent used. Mn2+ can be mitigated by diluting the electrolyte samples with a coordinating NMR solvent or by adding Li3PO4 to precipitate Mn2+ out of the solution.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Electrochemistry
Shrinidhi S. S. Pandurangi, David S. S. Hall, Clare P. P. Grey, Vikram S. S. Deshpande, Norman A. A. Fleck
Summary: Single crystal, Ni-rich layered lithium metal oxides are potential cathodes for next-generation lithium-ion batteries. However, their anisotropic swelling and contraction during cycling may lead to internal stresses, fracture, and capacity loss. This study predicts the evolution of lithium concentration and stress state within a LiNi0.8Mn0.1Co0.1O2 single crystal using a chemo-mechanical model. The results show that intraparticle fracture is not a significant degradation mode for well-designed NMC811 single crystals.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Teresa Insinna, Euan N. Bassey, Katharina Marker, Alberto Collauto, Anne-Laure Barra, Clare P. Grey
Summary: Graphite is a highly suitable anode material for lithium-ion batteries due to its low cost, low toxicity, and abundance. This study utilized electron paramagnetic resonance (EPR) spectroscopy to investigate the electronic structures of lithiated graphite anodes at different states of lithiation. The results demonstrated the heterogeneity within graphite particles and the presence of hyperfine coupling to lithium nuclei, highlighting the power of EPR spectroscopy in characterizing the local electronic structure of graphite and paving the way for its use in screening and investigating novel materials for lithium-ion batteries.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Ioan-Bogdan Magdau, Daniel J. Arismendi-Arrieta, Holly E. Smith, Clare P. Grey, Kersti Hermansson, Gabor Csanyi
Summary: In this study, a powerful machine learning approach is presented for simulating the molecular behavior of the EC:EMC binary solvent in liquid electrolytes. This method accurately captures the key properties of the organic molecule mixture and addresses the challenge of scale separation between intra- and inter-molecular interactions in condensed phase molecular systems.
NPJ COMPUTATIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Annalena R. Genreith-Schriever, Hrishit Banerjee, Ashok S. Menon, Euan N. Bassey, Louis F. J. Piper, Clare P. Grey, Andrew J. Morris
Summary: Ni-rich lithium-ion cathode materials exhibit high voltages and capacities, but face issues of structural instability and oxygen loss. The instability arises from the oxidation of oxygen during delithiation, with nickel displaying a charge state of approximately +2 and oxygen varying between -2 (NiO), -1.5 (LiNiO2), and -1 (NiO2). Computational calculations and X-ray spectroscopy demonstrate agreement with experimental spectra. Molecular dynamics simulations reveal oxygen loss from the (012) surface of delithiated LiNiO2, resulting in the formation of peroxide ions and subsequent oxidation to oxygen gas.
Article
Chemistry, Physical
Rory C. McNulty, Elizabeth Hampson, Lewis N. Cutler, Clare P. Grey, Wesley M. Dose, Lee R. Johnson
Summary: As state-of-the-art lithium-ion intercalation materials like nickel-rich chemistries are being pushed to their limits, understanding specific degradation and performance limitations becomes crucial. Half-cells, commonly used in industry and academia, are limited by the reactivity of lithium metal, which leads to early electrolyte degradation and cell failure. In this study, the limitations of half-cell studies of NMC811 electrodes with commercial loading are investigated, and it is found that the presence of Li has a detrimental impact on the NMC811 chemistry. The use of Li4Ti5O12 (LTO) as an alternative counter electrode is proposed for studying NMC positive electrode materials due to its high coulombic efficiency and low reactivity.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Cassius Clark, Christopher A. O'Keefe, Dominic S. Wright, Clare P. Grey
Summary: By optimizing the annealing time, nitrogen-doped graphitic spheres (NDGSs) with high nitrogen content were fabricated. These NDGSs exhibited stable bulk nitrogen doping level of 9% and performed well as anodes in lithium-ion batteries. However, they did not perform well in sodium-ion batteries.
Article
Chemistry, Physical
Jennifer P. Allen, Clare P. Grey
Summary: NMR spectroscopy is used to evaluate degradation of lithium-ion battery electrolyte solutions, but the presence of paramagnetic ions may affect the NMR spectra, inducing spectral broadening. This study investigates how dissolved Ni2+ and Mn2+ ions in LiPF6 electrolyte solutions affect the NMR spectra of pristine and degraded electrolyte solutions, and finds that Mn2+ causes greater broadening than Ni2+. The paramagnetic metals mainly affect the peak intensities of PF6- degradation species, followed by 31P and 1H peaks. The degree of broadening is solvent-dependent and can be mitigated by using a solvent with higher donor number. Dilution with a coordinating NMR solvent is effective in minimizing broadening caused by dissolved Mn2+. Li3PO4 addition also helps restore spectral resolution by precipitating Mn2+ out of the electrolyte samples.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Inorganic & Nuclear
Rosa Muller, Olivia Georghiades, Joshua D. Bocarsly, Farheen N. Sayed, Victor Riesgo-Gonzalez, Andrew D. Bond, Clare P. Grey, Dominic S. Wright
Summary: This study investigates the potential of lanthanide-containing polyoxotitanates as single-source precursors for hybrid oxides. The properties of the compounds were characterized using magnetic measurements, and their stability at high temperatures was observed.
DALTON TRANSACTIONS
(2023)