Title: Recent advances in developing organic electrode materials for multivalent rechargeable batteries
Due to the low cost and abundance of multivalent metallic resources (Mg/Al/Zn/Ca), multivalent rechargeable batteries (MRBs) are promising alternatives to Li-ion and Pb-acid batteries for grid-scale stationary energy storage applications. However, the high performance of inorganic electrode materials in Li-ion batteries does not extend to MRBs, because the high charge density of multivalent cations dramatically reduces their diffusivity in the crystal lattice of inorganic materials. To achieve high-performance MRBs, organic electrode materials (OEMs) with abundant structural diversity and high structural tunability offer opportunities. This review presents an overview of the state-of-the-art OEMs in MRBs, including non-aqueous rechargeable Mg/Al/Zn and aqueous rechargeable Mg/Al/Zn/Ca batteries. The advantages, challenges, development, mechanism, structure, and performance of OEMs in MRBs are discussed in detail. To provide a comprehensive and thorough understanding of OEMs in MRBs, the correlation between molecular structure and electrochemical behavior is also summarized and discussed. This review offers insights for the rational structure design and performance optimization of advanced OEMs in MRBs. more »« less
Holguin, Kathryn; Mohammadiroudbari, Motahareh; Qin, Kaiqiang; Luo, Chao
(, Journal of Materials Chemistry A)
null
(Ed.)
Na-ion batteries (NIBs) are promising alternatives to Li-ion batteries (LIBs) due to the low cost, abundance, and high sustainability of sodium resources. However, the high performance of inorganic electrode materials in LIBs does not extend to NIBs because of the larger ion size of Na + than Li + and more complicated electrochemistry. Therefore, it is vital to search for high-performance electrode materials for NIBs. Organic electrode materials (OEMs) with the advantages of high structural tunability and abundant structural diversity show great promise in developing high-performance NIBs. To achieve advanced OEMs for NIBs, a fundamental understanding of the structure–performance correlation is desired for rational structure design and performance optimization. In this review, recent advances in developing OEMs for non-aqueous, aqueous, and all-solid-state NIBs are presented. The challenges, advantages, mechanisms, development, and applications of advanced OEMs in NIBs are also discussed. Perspectives for the innovation of structure design principle and future research direction of OEMs in non-aqueous, aqueous, and all-solid-state NIBs are provided.
Wable, Minal; Marckx, Bret; Çapraz, Ömer Özgür
(, JOM)
The battery chemistry must be diversified to achieve a sustainable energy landscape by effectively utilizing renewable energy sources. Alkali metal-ion, all-solid-state, metal-air batteries, and multivalent batteries offer unique cost, safety, raw material abundance, energy, and power density solutions. However, realizing these “Beyond Li-ion batteries” must uncover their working principles and performance & property relationship. In this aspect, mitigating chemo-mechanical instabilities in the structure and surface of the electrodes plays a crucial role in their performance. Unfortunately, the coupling between electrochemical and mechanical interactions is often poorly understood due to a lack of operando characterization. This review article explains the working principles of curvature measurement and digital image correlation for measuring stress and strain generations in battery materials. We provided specific examples of how these operando mechanical measurements shed light on instabilities in alkali-metal ion electrodes, solid electrolytes, Li-O2 batteries, and aqueous Zn-ion batteries. Operando mechanical measurements offer an effective way to map changes in the physical fingerprint of the battery materials, therefore providing crucial information to elucidate instabilities in battery materials.
Datta, Joy; Koratkar, Nikhil; Datta, Dibakar
(, Energy Advances)
Lithium-ion batteries (LIBs) are ubiquitous in everyday applications. However, Lithium (Li) is a limited resource on the planet and, therefore, not sustainable. As an alternative to lithium, earth-abundant and cheaper multivalent metals such as aluminum (Al) and calcium (Ca) have been actively researched in battery systems. However, finding suitable intercalation hosts for multivalent-ion batteries is urgently needed. Open-tunneled oxides represent a specific category of microparticles distinguished by the presence of integrated one-dimensional channels or nanopores. This work focuses on two promising open-tunnel oxides: Niobium Tungsten Oxide (NTO) and Molybdenum Vanadium Oxide (MoVO). The MoVO structure can accommodate a larger number of multivalent ions than NTO due to its larger surface area and different shapes. Specifically, the MoVO structure can adsorb Ca, Li, and Al ions with adsorption potentials ranging from around 4 to 5 eV. However, the adsorption potential for hexagonal channels of Al ion drops to 1.73 eV due to the limited channel area. The NTO structure exhibits an insertion/adsorption potential of 4.4 eV, 3.4 eV, and 0.9 eV for one Li, Ca, and Al, respectively. Generally, Ca ions are more readily adsorbed than Al ions in both MoVO and NTO structures. Bader charge analysis and charge density plots reveal the role of charge transfer and ion size in the insertion of multivalent ions such as Ca and Al into MoVO and NTO systems. Exploring open-tunnel oxide materials for battery applications is hindered by vast compositional possibilities. The execution of experimental trials and quantum-based simulations is not viable for addressing the challenge of locating a specific item within a large and complex set of possibilities. Therefore, it is imperative to conduct structural stability testing to identify viable combinations with sufficient pore topologies. Data mining and machine learning techniques are employed to discover innovative transitional metal oxide materials. This study compares two machine learning algorithms, one utilizing descriptors and the other employing graphs to predict the synthesizability of new materials inside a laboratory setting. The outcomes of this study offer valuable insights into the exploration of alternative naturally occurring multiscale particles.
Ever-increasing demands for energy, particularly being environmentally friendly have promoted the transition from fossil fuels to renewable energy.1Lithium-ion batteries (LIBs), arguably the most well-studied energy storage system, have dominated the energy market since their advent in the 1990s.2However, challenging issues regarding safety, supply of lithium, and high price of lithium resources limit the further advancement of LIBs for large-scale energy storage applications.3Therefore, attention is being concentrated on an alternative electrochemical energy storage device that features high safety, low cost, and long cycle life. Rechargeable aqueous zinc-ion batteries (ZIBs) is considered one of the most promising alternative energy storage systems due to the high theoretical energy and power densities where the multiple electrons (Zn2+) . In addition, aqueous ZIBs are safer due to non-flammable electrolyte (e.g., typically aqueous solution) and can be manufactured since they can be assembled in ambient air conditions.4As an essential component in aqueous Zn-based batteries, the Zn metal anode generally suffers from the growth of dendrites, which would affect battery performance in several ways. Second, the led by the loose structure of Zn dendrite may reduce the coulombic efficiency and shorten the battery lifespan.5 Several approaches were suggested to improve the electrochemical stability of ZIBs, such as implementing an interfacial buffer layer that separates the active Zn from the bulk electrolyte.6However, the and thick thickness of the conventional Zn metal foils remain a critical challenge in this field, which may diminish the energy density of the battery drastically. According to a theretical calculation, the thickness of a Zn metal anode with an areal capacity of 1 mAh cm-2is about 1.7 μm. However, existing extrusion-based fabrication technologies are not capable of downscaling the thickness Zn metal foils below 20 μm. Herein, we demonstrate a thickness controllable coating approach to fabricate an ultrathin Zn metal anode as well as a thin dielectric oxide separator. First, a 1.7 μm Zn layer was uniformly thermally evaporated onto a Cu foil. Then, Al2O3, the separator was deposited through sputtering on the Zn layer to a thickness of 10 nm. The inert and high hardness Al2O3layer is expected to lower the polarization and restrain the growth of Zn dendrites. Atomic force microscopy was employed to evaluate the roughness of the surface of the deposited Zn and Al2O3/Zn anode structures. Long-term cycling stability was gauged under the symmetrical cells at 0.5 mA cm-2for 1 mAh cm-2. Then the fabricated Zn anode was paired with MnO2as a full cell for further electrochemical performance testing. To investigate the evolution of the interface between the Zn anode and the electrolyte, a home-developed in-situ optical observation battery cage was employed to record and compare the process of Zn deposition on the anodes of the Al2O3/Zn (demonstrated in this study) and the procured thick Zn anode. The surface morphology of the two Zn anodes after circulation was characterized and compared through scanning electron microscopy. The tunable ultrathin Zn metal anode with enhanced anode stability provides a pathway for future high-energy-density Zn-ion batteries.Obama, B., The irreversible momentum of clean energy.Science2017,355(6321), 126-129.Goodenough, J. B.; Park, K. S., The Li-ion rechargeable battery: a perspective.J Am Chem Soc2013,135(4), 1167-76.Li, C.; Xie, X.; Liang, S.; Zhou, J., Issues and Future Perspective on Zinc Metal Anode for Rechargeable Aqueous Zinc‐ion Batteries.Energy & Environmental Materials2020,3(2), 146-159.Jia, H.; Wang, Z.; Tawiah, B.; Wang, Y.; Chan, C.-Y.; Fei, B.; Pan, F., Recent advances in zinc anodes for high-performance aqueous Zn-ion batteries.Nano Energy2020,70.Yang, J.; Yin, B.; Sun, Y.; Pan, H.; Sun, W.; Jia, B.; Zhang, S.; Ma, T., Zinc Anode for Mild Aqueous Zinc-Ion Batteries: Challenges, Strategies, and Perspectives.Nanomicro Lett2022,14(1), 42.Yang, Q.; Li, Q.; Liu, Z.; Wang, D.; Guo, Y.; Li, X.; Tang, Y.; Li, H.; Dong, B.; Zhi, C., Dendrites in Zn-Based Batteries.Adv Mater2020,32(48), e2001854. Acknowledgment This work was partially supported by the U.S. National Science Foundation (NSF) Award No. ECCS-1931088. S.L. and H.W.S. acknowledge the support from the Improvement of Measurement Standards and Technology for Mechanical Metrology (Grant No. 22011044) by KRISS. Figure 1
Park, Min Je; Yaghoobnejad Asl, Hooman; Therese, Soosairaj; Manthiram, Arumugam
(, Journal of Materials Chemistry A)
The zinc-ion battery (ZIB) has been a system of particular interest in the research community as a possible alternative to lithium-ion batteries (LIB), and much work has been devoted to finding a suitable host material. In this article, monoclinic V 2 (PO 4 ) 3 is investigated as a host material for reversible insertion of Zn 2+ . Initial chemical assessment via a facile microwave-assisted chemical insertion method indicates the possibility of Zn 2+ insertion into the host. Electrochemical assessment, however, exhibits a significant capacity fade. In-depth analysis on the average and local structure of Li 3 V 2 (PO 4 ) 3 , the empty host V 2 (PO 4 ) 3 , and the Zn-inserted V 2 (PO 4 ) 3 reveals that heavy distortion is induced upon Zn 2+ insertion into the V 2 (PO 4 ) 3 framework, which is believed to be a result of a strong host–guest interaction jeopardizing the structural integrity. This is further supported by the dissolution of most of the material during the chemical oxidation of the Zn-inserted V 2 (PO 4 ) 3 . The underlying structural inadequacy poses difficulties for monoclinic V 2 (PO 4 ) 3 to be a viable reversible host for Zn-ion batteries. This work suggests that not only the electrostatic repulsions of multivalent ions in a structure during diffusion, but also the structural stability of the host upon insertion of multivalent ions, must be considered for a better design of suitable host materials for multivalent-ion batteries.
@article{osti_10212655,
place = {Country unknown/Code not available},
title = {Recent advances in developing organic electrode materials for multivalent rechargeable batteries},
url = {https://par.nsf.gov/biblio/10212655},
DOI = {10.1039/d0ee02111c},
abstractNote = {Due to the low cost and abundance of multivalent metallic resources (Mg/Al/Zn/Ca), multivalent rechargeable batteries (MRBs) are promising alternatives to Li-ion and Pb-acid batteries for grid-scale stationary energy storage applications. However, the high performance of inorganic electrode materials in Li-ion batteries does not extend to MRBs, because the high charge density of multivalent cations dramatically reduces their diffusivity in the crystal lattice of inorganic materials. To achieve high-performance MRBs, organic electrode materials (OEMs) with abundant structural diversity and high structural tunability offer opportunities. This review presents an overview of the state-of-the-art OEMs in MRBs, including non-aqueous rechargeable Mg/Al/Zn and aqueous rechargeable Mg/Al/Zn/Ca batteries. The advantages, challenges, development, mechanism, structure, and performance of OEMs in MRBs are discussed in detail. To provide a comprehensive and thorough understanding of OEMs in MRBs, the correlation between molecular structure and electrochemical behavior is also summarized and discussed. This review offers insights for the rational structure design and performance optimization of advanced OEMs in MRBs.},
journal = {Energy & Environmental Science},
volume = {13},
number = {11},
author = {Qin, Kaiqiang and Huang, Jinghao and Holguin, Kathryn and Luo, Chao},
editor = {null}
}
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