Article
Chemistry, Physical
Yang Liu, Cai Qi, Dandan Cai, Xiao Tang, Ying Li, Wenxian Li, Qinsi Shao, Jiujun Zhang
Summary: The development of electrode materials with high capacity and rate capability is necessary for improving the energy density and cycle life of lithium-ion batteries (LIBs). In this study, a cathode material, LiFePO4/C, modified with high electrical conductivity compound tantalum carbide (TaC), was successfully synthesized via hydrothermal method. The co-coating of nano-sized TaC and amorphous carbon layer on the surface of LiFePO4 particles allows for efficient electron and Li ion transfer, resulting in improved electrochemical kinetics. As a cathode material for LIBs, this composite demonstrates excellent electrochemical performances with high reversible capacity (159.0 mAh g(-1), 0.1C) and improved rate capacity. This methodology provides a new prospect for the application of transition metal carbides (TMCs) in modifying battery electrode materials.
Article
Chemistry, Physical
Jia-Jun Han, Ao-Ran Guo, Yan-Fang Wang
Summary: PANI/LFP composites were successfully prepared through synthesis and structural control, exhibiting excellent electrochemical performance and higher energy storage capacity compared to pure LFP materials. This is of great significance for the development of battery technology.
Article
Engineering, Environmental
Xiaoxiao Zhang, Zengshe Liu, Deyang Qu
Summary: In this study, the commercially mature ion-exchange (IX) method was explored for the first time to recover lithium from spent lithium iron phosphate (LFP) cathodes. The Li-K IX reaction using oxalic acid as the feeding solution delivered a potential product of multi-elemental fertilizer. This simple and economical technology provides a practical recycling strategy for spent LFP batteries.
Article
Chemistry, Analytical
Jing Geng, Zhengguang Zou, Tianxing Wang, Shuchao Zhang, Shenglin Zhong, Wenqin Ling, Xiaoxiao Peng, Xixi Hu
Summary: Mn and K co-doped lithium iron phosphate (LFP) cathode materials were successfully synthesized by solvothermal method. The contributions of the two dopants to the LFP were investigated using density functional theory (DFT) calculations and various characterizations. The presence of Mn improved the energy band and diffusion kinetics, while K contributed to the stabilized structure and widened diffusion channel. The co-doped LFP cathode exhibited a high capacity of 145 mAhmiddotg-1 at 5 C and maintained a 96% retention rate after 400 cycles. The interaction between the two doping elements was discussed by comparing with a control group, and the KLMFP samples showed superior electrochemical performance in cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and charge-discharge cycling tests.
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
(2023)
Review
Materials Science, Multidisciplinary
Liming Lu, Guoqiang Jiang, Chunyan Gu, Jiangfeng Ni
Summary: Polyanionic phosphates like LiFePO4 exhibit excellent lattice stability and safety features due to the strong covalent bond of P-O, which constrains oxygen atoms and minimizes defects in the oxygen site, resulting in stable frameworks. Furthermore, the presence of the strong P-O covalent bond stabilizes the anti-bonding transitional metal redox couple through an M-O-P inductive effect, generating a relatively high potential.
FUNCTIONAL MATERIALS LETTERS
(2021)
Article
Electrochemistry
Rong He, Yongling He, Wenlong Xie, Bin Guo, Shichun Yang
Summary: This paper investigates the aging behavior and mechanism of cylindrical LFP batteries by designing a cross-comparison aging test, which uses three constant current and two different dynamic working conditions for accelerated aging at high temperature. The aging behavior and mechanism are quantitatively studied through in-situ electrochemical test and ex-situ Post-Mortem methods. External characteristic parameters such as capacity, internal resistance, and open circuit voltage are periodically checked during the long-term cycle of the battery. This multiscale analytical method enables a detailed understanding of the performance loss process, guiding performance prediction and safety diagnostics.
ELECTROCHIMICA ACTA
(2023)
Article
Engineering, Chemical
Yin Li, Li Wang, Keyu Zhang, Yaochun Yao, Lingxin Kong
Summary: LiFePO4 is a promising cathode material for lithium ion batteries due to its nontoxicity, high specific capacity, good safety characteristics, and low cost. The use of phytic acid as a new phosphorus source for synthesis has shown significant effects on morphology and electrochemical performance. After carbon coating, LiFePO4 exhibits outstanding initial discharge capacity and high temperature behavior, which is crucial for the controllable synthesis and improvement of its electrochemical characteristics.
ADVANCED POWDER TECHNOLOGY
(2021)
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
Kazuhiko Mukai, Takamasa Nonaka, Takeshi Uyama
Summary: Research revealed a two-phase reaction scheme in lithium titanium oxide during lithium-ion battery operation, with distinct structural transformations observed at different scales. Linear, reversible changes in bond distance between titanium and oxygen atoms were observed at the atomic scale, while hysteresis in lattice parameter between discharge and charge reactions was noted at the microscale. These differences in structural changes were attributed to variances in spatial resolutions between XAS and XRD techniques.
ENERGY STORAGE MATERIALS
(2022)
Article
Materials Science, Multidisciplinary
Dimitra Vernardou
Summary: In this review, the hydrothermal growth method of lithium iron phosphate and its effect on the electrochemical performance of cathodes are discussed. The advantages of the hydrothermal process, as well as the ability to tune growth parameters and modify material characteristics, are highlighted. Recent strategies involving carbon-based materials, N-doped graphene oxide, multi-wall carbon nanotubes, and metallic nanoparticles are explored for improving cathode performance and stability. Future directions include simultaneous growth of solid-state electrodes and powders, as well as improving morphology and orientation for standardized growth of energy storage materials.
Article
Chemistry, Physical
Ling Ding, Rita Leones, Toni Schmeida, Kornelius Nielsch, Daria Mikhailova
Summary: A quasi-solid-state polymer gel binder (PGB) has been investigated for its application in high-temperature lithium-ion batteries. The results showed that PGB exhibited better cycling performance and electrochemical kinetics compared to the conventional binder PVDF at 60 degrees C.
JOURNAL OF POWER SOURCES
(2022)
Article
Materials Science, Multidisciplinary
Eva Gerold, Reinhard Lerchbammer, Helmut Antrekowitsch
Summary: The need to recover critical elements from lithium-ion batteries is crucial, and adapting the hydrometallurgical recycling processes is necessary due to the development of cathode materials and the search for cheaper alternatives. By optimizing the leaching process, an effective way of recovering lithium from different cathode materials has been identified.
Article
Chemistry, Physical
Chen-Yi Huang, Tsung-Rong Kuo, Sibidou Yougbare, Lu-Yin Lin
Summary: Carbon coating can improve the electrical conductivity of lithium iron phosphate (LFP) as a promising cathode material for lithium ion batteries (LIB), with commercial organic binder Super P (R) (SP) being utilized for the first time to achieve uniform coating and enhance electrochemical performance.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Green & Sustainable Science & Technology
Dan Zhan, Xiaoqing Yuan, Cuili Xiang, Jun Lu, Gaopeng Dai, Ruofei Hu, Zuoan Xiao, Haiyan Mao, Marcus Fehse, Andre J. Simpson, Bing Wu
Summary: The study successfully prepared a carbon fiber/MnO/C composite material using cotton and pyrrole as raw materials, demonstrating excellent electrochemical performance attributed to its unique structure. The composite material maintained high discharge capacity, exhibited superior rate capability and long-term cycle stability compared to MnO/C and MnO.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2021)
Article
Electrochemistry
Hsun-Sheng Liu, Kun-You Chen, Chan-En Fang, Chi-cheng Chiu
Summary: Functional polymers as electrode binders enhance lithium ion conductivity and battery performance. Molecular dynamics simulations reveal that improving Li+ affinity and local mobility at the interface are crucial for a good binder, with free energy variations playing a dominant role.
ELECTROCHIMICA ACTA
(2021)
Article
Materials Science, Multidisciplinary
Yun-Feng Wu, Ji-Wei Ma, Yun-Hui Huang
Summary: Designing highly active and durable electrocatalysts for oxygen reduction reaction (ORR) is crucial for proton exchange membrane fuel cells. In this study, Pt-Co catalysts were synthesized using a facile soft-chemistry method, and they exhibited excellent activity and durability. Pt3Co/C showed significantly improved ORR activity and durability compared to commercial Pt/C.
Article
Electrochemistry
Chen Cai, Gary M. Koenig Jr
Summary: Lithium-ion batteries are widely used for energy storage, and research is focused on improving their properties. Increasing electrode thickness can enhance the loading of active material and reduce inactive components, but it may affect mechanical stability. This study investigates the processing of TiNb2O7 into all active material (AAM) electrodes, which can overcome the limitations in thick lithium-ion electrodes. The results provide insights into fabricating AAM electrodes with multicomponent oxide phases and their electrochemical consequences.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Un-Hyuck Kim, Tae-Yeon Yu, Jin Wook Lee, Han Uk Lee, Ilias Belharouak, Chong Seung Yoon, Yang-Kook Sun
Summary: Electric vehicles powered by Li-ion batteries can be dangerous due to the flammable liquid electrolytes, but all-solid-state batteries offer a safe alternative. This study demonstrates that B-doping and coating of a Ni-rich Li[Ni0.9Co0.05Mn0.05]-O2 cathode can enhance the microstructure and cathode-solid electrolyte interface, resulting in an all-solid-state battery that cycles stably for 300 cycles with minimal capacity fading. The B-doped, B-coated Li[Ni0.9Co0.05Mn0.05]O2 cathode achieves a discharge capacity of 214 mAh g-1, one of the highest among all-solid-state batteries, and retains 91% of its initial capacity after 300 cycles, surpassing previously reported all-solid-state batteries in terms of energy density without compromising cycling stability.
ACS ENERGY LETTERS
(2023)
Review
Chemistry, Physical
Albina Jetybayeva, Douglas S. Aaron, Ilias Belharouak, Matthew M. Mench
Summary: The potential of solid-state lithium-ion batteries (SSBs) is of interest due to their high energy density, superior mechanical and thermal stability, and inherent safety. However, the use of lithium metal as the anode presents challenges in terms of reactivity, oxidation, and abundance. Alternative anodes such as silicon are being investigated due to their high capacity and improved safety features. This study provides an analysis of current SSBs with lithium and non-lithium anodes and proposes future research directions.
JOURNAL OF POWER SOURCES
(2023)
Article
Chemistry, Physical
Zhenglu Zhu, Jie Ji, Xiaoqun Qi, Yongsheng Ji, Zhikang Liu, Weichen Du, Yujun Pan, Dan Yang, Jiwei Ma, Long Qie, Yunhui Huang
Summary: Recruiting anions from electrolyte additives into the lithium ion solvation structure is a promising strategy for the construction of long-lifespan Li-metal batteries (LMBs). However, inadequate understanding of the anion-involved Li+ solvation hinders the finding of new anion additives. The effects of the newly-introduced NO3- anion on the Li+ solvation structure are investigated, showing that it reduces the electrostatic potential of the Li+ solvation cluster, especially for solvated solvents, thus improving electrolyte stability against the Li anode. The anion selection coefficient, based on the anion size to the binding energy toward Li+, is proposed as a new selection principle, leading to the discovery of the beneficial hexafluorosilicate anion for LMBs.
ADVANCED ENERGY MATERIALS
(2023)
Article
Energy & Fuels
Jing Wang, Ziyang Nie, Gary M. Koenig
Summary: Thick sintered porous tellurium pellets without binders and additives show high areal capacity, which is beneficial for increasing cell energy density in lithium-tellurium batteries. By using a processing route, the tellurium powder is treated to reduce particle size and increase electroactive area, resulting in a significant improvement in gravimetric capacity and retention of capacity at increasing rates.
Article
Chemistry, Multidisciplinary
Rachid Essehli, Hamdi Ben Yahia, Ruhul Amin, Mengya Li, Daniel Morales, Steven G. Greenbaum, Ali Abouimrane, Anand Parejiya, Abdelfattah Mahmoud, Khalid Boulahya, Marm Dixit, Ilias Belharouak
Summary: Conventional sodium-based layered oxide cathodes have poor electrochemical performance due to air sensitivity and safety concerns at high voltage. However, a tailored derivative compound, Na3.2Ni0.2V1.8(PO4)(2)F2O, shows improved specific capacity and cycling stability, making it a promising cathode material for sodium-ion batteries.
Article
Chemistry, Multidisciplinary
Mengya Li, Marm Dixit, Rachid Essehli, Charl J. J. Jafta, Ruhul Amin, Mahalingam Balasubramanian, Ilias Belharouak
Summary: Seawater batteries (SWBs) have attracted significant interest in the field of electrochemical energy storage due to their low cost, abundance, and potential for long-duration energy storage. However, their practical application is hindered by poor electrochemical performance related to inadequate interfaces of the solid electrolyte (SE), as well as structural and chemical instabilities and slow ionic transport properties. This study focuses on improving the performance of a surrogate SWB by introducing tailored dopants into the Na3Zr2Si2PO12 (NZSP) solid electrolyte membrane and observing the resulting changes in surface chemistry, local structure, ionic conductivity, and critical current density. The doped NZSP exhibits a more densely packed pellet with a uniformly distributed porous structure, demonstrating enhanced cycling stability and reversible capacities based on different sodium storage mechanisms.
Article
Chemistry, Physical
Marm Dixit, Nitin Muralidharan, Anuj Bisht, Charl J. Jafta, Christopher T. Nelson, Ruhul Amin, Rachid Essehli, Mahalingam Balasubramanian, Ilias Belharouak
Summary: The development of thin, dense, defect-free solid electrolyte films is crucial for practical and commercial solid-state batteries. This study demonstrates a simple processing route for antiperovskite (Li2OHCl) solid electrolyte materials, which can produce films/pellets with very high densities (around 100%) and higher conductivities compared to conventional pressed pellets. The new protocol also improves the critical current density and lithiophilicity of the material through surface nitrogen enrichment. Distribution of relaxation time analysis confirms the faster transport mechanisms in the antiperovskite films/pellets produced using the new pathway. Overall, these findings highlight the feasibility of engineering antiperovskite solid electrolytes at the grain scale as a highly desirable approach for practical all-solid-state batteries.
ACS ENERGY LETTERS
(2023)
Article
Green & Sustainable Science & Technology
Yaocai Bai, Mengya Li, Charl J. Jafta, Qiang Dai, Rachid Essehli, Bryant J. Polzin, Ilias Belharouak
Summary: With the rapid growth of Li-ion battery production, a large amount of electrode scraps are generated and need to be recycled. This study presents a water-based recovery process that effectively delaminates anode films from Cu foils, allowing the critical materials to be reused in the battery supply chain. The recovered anode films and Cu foils are of battery grade quality and exhibit no physical or chemical damage, while the reprocessed anode shows similar electrochemical performance to the pristine anode. This environmentally friendly and cost-effective separation technique enables battery manufacturers to recycle and reuse their electrode scraps on-site safely and effectively.
SUSTAINABLE MATERIALS AND TECHNOLOGIES
(2023)
Article
Chemistry, Physical
Lu Yu, Yaocai Bai, Rachid Essehli, Anuj Bisht, Ilias Belharouak
Summary: Polyol-metallurgy is a promising method for recycling spent lithium-ion batteries. The method utilizes a dual-function green solution to leach valuable metal ions and selectively precipitate cobalt, without the need for additional precipitation agents. The unique characteristics of the solution enable efficient leaching, separation, and coprecipitation, making it more efficient and feasible than existing alternatives.
ENERGY STORAGE MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Zhenkai Ji, Min Sun, Tiantian Chen, Xinyi Shen, Xiuzhen Xu, Yan Zhong, Dadong Wang, Jiwei Ma, Bo Chen, Zhiguo Yi, Xiaobin Xu
Summary: Here, we present a simple method that combines top-down patterning transfer and bottom-up nanorod growth to fabricate large-area and ordered TiO2 nanorod arrays. Pre-crystallization seeding can be patterned with nanostructured morphologies through interfacial tension-driven precursor solution scattering on various types and period templates. This versatile strategy shows great operability in complex substrate morphologies and is applicable to capillary force-driven interfacial patterns. Customized patterned lithographic templates containing English words, Arabic numerals, and Chinese characters are utilized to verify the applicability and controllability of this hybrid method. In summary, this work provides a low-cost and facile approach for preparing hydrothermally growable metal oxide (e.g., ZnO and MnO2) nanostructures, which have potential applications in microelectronic devices, photoelectric devices, energy storage, and photocatalysis.
Article
Materials Science, Multidisciplinary
Yuwei Chen, Tengrui Wang, Huaican Chen, Wang Hay KAn, Wen Yin, Zhenyou Song, Chen Wang, Jiwei Ma, Wei Luo, Yunhui Huang
Summary: High-entropy ceramics (HECs) have shown great potential in designing materials with tailored properties due to their high configurational entropy and elemental synergies. However, the arrangement of multiple elements in the structure and their influence on bond length regulation remain unclear. In this study, a medium-entropy garnet-structured electrolyte Li6La3Zr0.5Hf0.5Ta0.5Nb0.5O12 (ME-LLZO) is synthesized and its short-range structure is elucidated through supercell calculations and neutron pair distribution function (PDF) refinement. Observations include extended bottleneck size, elongated Li-O bond length, and local clustering of certain sites. The differences between the multiple cations inevitably affect the short-range structure, providing insights for future exploration of HEC-based solid-state electrolytes.
Review
Nanoscience & Nanotechnology
Yiming Zhu, Jingyao Wang, Jiwei Ma
Summary: Single-atom catalysts (SACs) are cost-effective and have excellent performance for clean energy conversion. While carbon is commonly used as a support for SACs, non-C materials with flexible properties and unique metal-support interactions have gained attention for loading isolated metal atoms. This review provides a comprehensive summary of current research on non-C-supported SACs for green energy conversion, including synthesis methods, metal-support interactions, applications, in situ/operando approaches, and challenges in designing promising non-C-supported SACs.
Article
Chemistry, Physical
Chen Cai, Gary M. Koenig Jr
Summary: Lithium-ion batteries are widely used due to their high energy density. A common approach to increasing battery energy density is to use thick electrodes, but this poses limitations on electronic and ionic transport. This research explores the use of All Active Material (AAM) electrodes, specifically incorporating LiNi0.5Mn0.5O2 (LNMO) and LiCoO2 (LCO) as multicomponent AAM cathodes. The combination of LCO and LNMO improves the electrochemical properties, with LCO forming a conductive network while the two materials remain segregated. Pseudo-two-dimensional simulations further analyze the electrochemical outcomes. This study introduces a new concept for incorporating low electronic conductivity materials into AAM electrodes, enabling high energy electroactive materials at high loading.