Article
Chemistry, Multidisciplinary
Liguang Wang, Xincheng Lei, Tongchao Liu, Alvin Dai, Dong Su, Khalil Amine, Jun Lu, Tianpin Wu
Summary: The study proposes a strategy to enhance the electrochemical performance of Ni-rich layered oxides by leveraging low-strain analogues of Li- and Mn-rich layered oxides to reconstruct the surface. The new surface structure with gradient chemical composition and defect-rich structure facilitates lithium diffusion and stabilizes the crystal structure, leading to improved cycling stability and capacity retention of the batteries.
ADVANCED MATERIALS
(2022)
Article
Chemistry, Physical
Xueyan Hou, Takuya Katsumata, Yuta Kimura, Yusuke Tamenori, Kiyofumi Nitta, Hirona Yamagishi, Koji Amezawa, Takashi Nakamura
Summary: As a promising cathode material for high-energy-density Li-ion batteries, the Ni-rich layered oxide cathode active chemical performance degrades rapidly upon charge/discharge cycles probably due to electrochemical/thermochemical instabilities. Cationic doping has been regarded as an effective strategy to enhance the electrochemical performance. In this study, the impact of cationic doping on the electrochemical performance and lattice oxygen stability was quantitatively assessed.
ACS APPLIED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Yuefeng Su, Qiyu Zhang, Lai Chen, Liying Bao, Yun Lu, Shi Chen, Feng Wu
Summary: By coating ZrO2 on LiNi0.8Co0.1Mn0.1O2, its cycle performance can be improved, mainly attributed to the doped Zr4+ in the surface structure rather than the ZrO2 coating. The surface doping of Zr4+ resulted in the reduction of Ni3+ to Ni2+ on the surface of LiNi0.8Co0.1Mn0.1O2, leading to an increase in cation disordering and hindering side reactions at the interface, ultimately stabilizing the bulk structure.
ACTA PHYSICO-CHIMICA SINICA
(2021)
Article
Nanoscience & Nanotechnology
Luqman Azhari, Bryer Sousa, Ridwan Ahmed, Rui Wang, Zhenzhen Yang, Guanhui Gao, Yimo Han, Yan Wang
Summary: Doping lithium bromide or lithium chloride effectively improves the capacity retention and rate performance of Ni-rich NMC cathode materials, increases the specific surface area, and forms a stable CEI layer. In addition, the particle microstructure is better equipped to handle volume changes with longer critical crack lengths.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Multidisciplinary
Lianshan Ni, Hongyi Chen, Shuai Guo, Alvin Dai, Jinqiang Gao, Lei Yu, Yu Mei, Haoji Wang, Zhen Long, Jianguo Wen, Wentao Deng, Guoqiang Zou, Hongshuai Hou, Tongchao Liu, Khalil Amine, Xiaobo Ji
Summary: A multifunctional strategy of synchronously fabricating perovskite-type SrZrO3 coating and Sr/Zr co-doping is employed to strengthen the structure/interface stability and Li+ transport mobility of LiNi0.85Co0.10Mn0.05O2 (NCM) cathodes. The Sr/Zr-modified NCM exhibits remarkable capacity retention of 99.4% after 200 cycles at 1 C and a high rate capacity of 168.9 mAh g(-1) at 10 C, demonstrating its potential for high-performance electric vehicle cathodes. This work opens new avenues for developing NCM cathodes with high energy and high power for EVs with long calendar life.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Hoon-Hee Ryu, Hyung-Woo Lim, Sin Gyu Lee, Yang -Kook Sun
Summary: The doping of Ni-rich layered cathodes is an important strategy to enhance their long-term cycling performance. This study explores the effect of Mo dopant content and lithiation temperature on the properties and electrochemical performance of a Ni-rich layered cathode material. It is found that sufficient Mo content leads to cathode materials with fine primary particles and higher crystallinity, resulting in higher capacity and better long-term cycling performance. The optimized Mo-doped Ni-rich cathode developed in this study demonstrates excellent stability and enables Li-ion batteries with a long cycle life.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Lin Wang, Baofu Zhu, Dongdong Xiao, Xu Zhang, Boya Wang, Haifeng Li, Tianhao Wu, Shiqi Liu, Haijun Yu
Summary: A strategy of high-valence W doping is proposed to improve the stability and electrochemical performance of Ni-rich layered oxide cathode materials for lithium-ion batteries.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
J. C. Luo, J. F. Luo, C. -L. Chen, W. -H. Huang, C. -K. Chang, Y. -C. Chuang, J. L. Zhang, R. R. Zhao
Summary: This study comprehensively characterizes and analyzes the structural modulations associated with trace amounts of Zr dopants in LiNi0.9Co0.1O2 layered cathodes. The results show that Zr4+ preferentially replaces Co3+ at the Ni/Co site, leading to relaxation of Ni-O bonds and reducing the Jahn-Teller effect and charge excitation in the battery.
MATERIALS TODAY CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Xinyan Li, Ang Gao, Zhexin Tang, Fanqi Meng, Tongtong Shang, Shengnan Guo, Jiarun Ding, Yanhong Luo, Dongdong Xiao, Xuefeng Wang, Dong Su, Qinghua Zhang, Lin Gu
Summary: The study reports that surface reconstruction induced by specific antisites can suppress the outward migration of transition metals and oxygen ions, achieving a stable surface structure for layered oxide cathodes of lithium-ion batteries.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Weiyuan Huang, Cong Lin, Mingjian Zhang, Shunning Li, Zhefeng Chen, Wenguang Zhao, Chen Zhu, Qi Zhao, Haibiao Chen, Feng Pan
Summary: This study investigates the effects of Co and Ni substitution on Mn-rich layered cathodes for lithium-ion batteries. Results show that Co4+ is detrimental to structural stability, while Ni substitution of Co enhances lattice oxygen stability and improves cycling stability. These findings contribute to the development of Co-free Mn-rich layered cathode materials for future rechargeable lithium-ion batteries.
ADVANCED ENERGY MATERIALS
(2021)
Article
Engineering, Environmental
Daoyan Feng, Yu Liu, Chen Zhao, Han Su, Xia Kong, Yu Zhong, Junzhang Wang, Zhou Xu, Xiuli Wang, Xingzhong Guo, Jonghee Lee, Jiangping Tu
Summary: The study proposes a simple surface modification approach to achieve a highly stable interface by dual doping of Zr and F in LiNi0.83Co0.12Mn0.05O2 (NCM83) cathodes via acid washing and annealing. The modified cathode exhibits exceptional long-cycle stability, offering a new perspective for the design of high-performance sulfide-based all-solid-state batteries.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Yongkang Han, Yingchuan Zhang, Yike Lei, Dongdong Xiao, Jie Ni, Weiguang Lin, Pingwen Ming, Cunman Zhang, Qiangfeng Xiao
Summary: To address the issues of Ni-rich NCM, Al (CF3SO3)(3) was proposed as a solid electrolyte additive to regulate the CEI in single-crystalline NCM811. The facile oxidation of CF3SO3- and subsequent reactions with reactive species from NCM811 and electrolyte lead to the formation of a robust sandwich CEI film containing sulfur and aluminum species. This CEI film not only prevents electrolyte decomposition but also alleviates the formation of inactive rock-salt phase on NCM811 surface, resulting in a high-capacity retention of 91.5% after 200 cycles under 0.5 C.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Chemistry, Physical
Linzhe Wang, Jian Qin, Zhimin Bai, Huaming Qian, Yanyan Cao, Hirbod Maleki Kheimeh Sari, Yukun Xi, Hui Shan, Shuai Wang, Jiaxuan Zuo, Xiaohua Pu, Wenbin Li, Jingjing Wang, Xifei Li
Summary: In this study, in situ Zn-doped NCM material was successfully designed by atomic layer deposition combined with annealing. Compared with ex situ Zn-doped NCM, in situ Zn-NCM exhibited better stability and reduced surface defects due to its lower migration energy barrier and more uniform distribution of heteroatoms. As a result, it showed higher reversible capacity and initial Coulombic efficiency. Therefore, in situ doping is an effective strategy to enhance the performance of lithium-ion battery cathodes.
Article
Chemistry, Physical
Fangkun Li, Zhengbo Liu, Caijian Liao, Xijun Xu, Min Zhu, Jun Liu
Summary: A reliable high-voltage Ni-rich cathode material has been successfully developed through a multifunctional modification strategy involving gradient engineering and surface lattice modulation. The cathode operates stably under high voltage and shows potential for pushing the development of lithium-ion batteries towards higher energy density.
ACS ENERGY LETTERS
(2023)
Article
Nanoscience & Nanotechnology
Qun Liu, Te Xie, Qingshui Xie, Wei He, Yinggan Zhang, Hongfei Zheng, Xiangjun Lu, Wensheng Wei, Baisheng Sa, Laisen Wang, Dong-Liang Peng
Summary: A multiscale deficiency integration is realized in a Li-rich manganese-based cathode material through Na-rich engineering, significantly improving the electrochemical properties of the electrode materials. It enhances capacity retention, voltage retention, and energy density maintenance of the cathode material.
ACS APPLIED MATERIALS & INTERFACES
(2021)
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
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
Sundeep Vema, Farheen N. Sayed, Supreeth Nagendran, Burcu Karagoz, Christian Sternemann, Michael Paulus, Georg Held, Clare P. Grey
Summary: Garnet solid-electrolyte-based Li-metal batteries have the potential to be used in high-energy density and thermally stable energy storage devices. However, the formation of lithium hydroxide and carbonate on the garnet surface in an ambient atmosphere poses processing challenges. This study investigates the decomposition of surface layers under different gas environments and identifies that heating under an oxygen atmosphere leads to a clean garnet surface, while low oxygen partial pressures result in additional carbon deposits. The clean garnet surface reacts with moisture and carbon dioxide, indicating a need for control over CO2 concentration during garnet handling. Symmetric cells with low interface resistance and dendrite-free plating currents are achieved by heating under O₂ and avoiding H₂O and CO₂.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Adam J. Lovett, Venkateswarlu Daramalla, Farheen N. Sayed, Debasis Nayak, Muireann de h-Ora, Clare P. Grey, Sian E. Dutton, Judith L. MacManus-Driscoll
Summary: Epitaxial cathodes in lithium-ion microbatteries are ideal model systems for studying mass and charge transfer across interfaces and degradation processes. In this study, we report the growth of epitaxial LiMn2O4 (LMO) thin films on a new current collector material, NiCo2O4 (NCO), at a low temperature of 360°C. Our films show a discharge capacity of >100 mAh g(-1) for >6000 cycles, indicating long-term electrochemical stability of our NCO current collector. This research offers a route towards high-performance microbatteries for miniaturized electronic devices.
ACS ENERGY LETTERS
(2023)
Article
Chemistry, Physical
Arvind Pujari, Byung-Man Kim, Farheen N. Sayed, Kate Sanders, Wesley M. Dose, Angus Mathieson, Clare P. Grey, Neil C. Greenham, Michael De Volder
Summary: Light-rechargeable photobatteries are a solution to the intermittency of solar irradiation. This study analyzes the thermal contributions to the increase in capacity of two promising photoactive cathode materials under different charging conditions. The results show that the increase in capacity is mainly due to thermal effects.
ACS ENERGY LETTERS
(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
Materials Science, Multidisciplinary
Hrishit Banerjee, Clare P. Grey, Andrew J. Morris
Summary: Using ab initio dynamical mean-field theory, this study explores the electronic and magnetic states of layered LixMnO2 as a function of x, the state-of-charge. The results show different states of the system during delithiation at various charge states, and the presence of high-spin state is observed to be most likely.
Article
Chemistry, Physical
Svetlana Menkin, Jana B. Fritzke, Rebecca Larner, Cas de Leeuw, Yoonseong Choi, Anna B. Gunnarsdottir, Clare P. Grey
Summary: This study reveals the presence of soft shorts, which are often overlooked due to their indistinguishable electrochemical signatures, in realistic conditions using impedance spectroscopy and operando NMR. It also demonstrates the predictability of soft shorts and the potential use of electrochemical impedance spectroscopy for early detection of catastrophic shorts and battery failure.
FARADAY DISCUSSIONS
(2023)
Article
Chemistry, Physical
Erlendur Jonsson, Astrid H. Berge, Clare P. Grey, Israel Temprano
Summary: In this study, the role of electrolyte composition in the solvation of I- in iodide-based redox mediation in Li-O-2 batteries was investigated using a molecular dynamics approach. The results showed that shorter glymes allow for a closer packing of I- redox mediator, and increasing the concentration of I- reduces the solvation of Li+ in glymes. The presence of water further facilitates the interaction between I- and Li+, with a more pronounced effect in monoglyme. The competition between Li+ and I- for water coordination is modulated by different solvents, with longer chain lengths being less affected by increases in water concentrations.
FARADAY DISCUSSIONS
(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)
