Energy storage and conversion are key factors for enabling the transition from fossil fuels to intermittent renewables [...

Dsoke, Sonia

Marinaro, Mario

Nanomaterials

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Mario Marinaro

Sonia Dsoke

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Advances in Nanomaterials for Lithium-Ion/Post-Lithium-Ion Batteries and Supercapacitors

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Citation: Marinaro, M.; Dsoke, S.Advances in Nanomaterials forLithium-Ion/Post-Lithium-IonBatteries and Supercapacitors.Nanomaterials 2022, 12, 2512.https://doi.org/10.3390/nano12152512Received: 11 July 2022Accepted: 20 July 2022Published: 22 July 2022Publisher’s Note: MDPI stays neutralwith regard to jurisdictional claims inpublished maps and institutional affil-iations.Copyright: © 2022 by the authors.Licensee MDPI, Basel, Switzerland.This article is an open access articledistributed under the terms andconditions of the Creative CommonsAttribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/).nanomaterialsEditorialAdvances in Nanomaterials for Lithium-Ion/Post-Lithium-IonBatteries and SupercapacitorsMario Marinaro 1,* and Sonia Dsoke 2,*1 ZSW-Zentrum für Sonnenenergie und Wasserstoff-Forschung, Helmholtzstrasse 8, 89081 Ulm, Germany2 Institute for Applied Materials (IAM), Karlsruhe Institute of Technology (KIT),Hermann-von-Helmholtz-Platz 1, 76344 Eggenstein-Leopoldshafen, Germany* Correspondence: mario.marinaro@zsw-bw.de (M.M.); sonia.dsoke@kit.edu (S.D.)Energy storage and conversion are key factors for enabling the transition from fossilfuels to intermittent renewables. Moreover, the increasing number of electric vehicles onthe road (HEV, PHEV, BEV, FCEV) calls for high-performance, reliable, safe, and low-costenergy storage and conversion devices. Within this context, batteries and supercapacitorsas well as hydrogen and fuel cells play a central role. Our point of view is that dependingon the application, all storage and conversion devices should contribute to the final goal ofdecreasing greenhouse gas emissions by speeding up the electrification process.Lithium-ion batteries (LIBs) are paving the way as the technology of choice for theelectrification of road transport as well as for home storage. Since being commercialized bySony in 1991, the cost of this technology has decreased from USD ~1000 to ~100 per kW/h,representing approximately one order of magnitude. At the same time, achievable energieshave improved substantially. Increasing battery energy not only means developing newhigh-performance anode and cathode materials, but also means improving the performanceand minimizing the weight and volume fractions of all of the inactive components.Besides LIBs, there are new and emerging technologies, so-called “post Lithium-ion”batteries, such as Na-ion, solid-state, and Mg- and Ca-ion batteries, which, if successfully de-veloped, might introduce some advantages. It is worth noting that the abovementioned batterytechnologies are in different stages of development and therefore have different TechnologyReadiness Levels (TRLs), with Na-ion batteries being the closest to market introduction.This Special Issue focuses on the current developments and future perspectives ofvarious battery and supercapacitor technologies through eight original research papers andone review, all of which were written by well-respected scientists.As already mentioned, Na-ion batteries are the post-lithium battery technology that isthe closest to market introduction. In fact, Na-ion is often referred to as drop-in technology,as it may not require the full re-organization of the battery cell manufacturing process.Mosa and co-workers report on the electrochemical conversion reaction of NiO with Na-ions in an organic electrolyte [1]. NiO thin films (560 nm thick) are successfully preparedby magnetron sputtering (MS) deposition under an oblique angle configuration (OAD)and demonstrate a large capacity during the first cycle that then fades remarkably uponsuccessive cycles, demonstrating the limited reversibility of the electrochemically drivenconversion reaction.Bargnesi et al. still focus Na-ion batteries, this time with an aqueous electrolyte,and suggest the use of cross-linked chitosan as a binder for an environmentally friendlyelectrode preparation process [2]. A successful cross-linked reaction involving chitosanand succinic acid with the addition of a coupling agent, N-(3-Dimethylaminopropyl)-N′-ethylcarbodiimide hydrochloride, resulted in a water-insoluble binder that allows themanufacturing of free-standing electrodes for aqueous Na-ion batteries.Considering solid-state batteries, Yang and co-workers propose a solid electrolytebased on Li2(BH4)(NH2) that was nanoconfined in a mesoporous silica molecule sieveNanomaterials 2022, 12, 2512. https://doi.org/10.3390/nano12152512 https://www.mdpi.com/journal/nanomaterialsNanomaterials 2022, 12, 2512 2 of 3(SBA-15) and obtained via the melting–infiltration approach [3]. The SBA-15-modifiedelectrolyte shows improved Li-ion conductivity over the unmodified Li2(BH4)(NH2). Theauthors successfully demonstrate low-voltage proof-of-concept ASSBs using TiS2 as acathode material capable of achieving ~50 cycles at T = 55 ◦C.Silicon and silicon oxides are a very promising class of anode material for LIBs, asthey can reach a specific capacity that is up to 10× higher compared to state-of-the-artgraphite. Tenzg and co-workers proposed a silicon carbide (SiC)/graphitic carbon coatingmade of silicon flakes recycled from the waste produced from silicon wafers [4]. The coatedmaterial showed improved electrochemical performance in half cells. The authors ascribethe improved performance to the double effect of SiC, which provides physical strength andhelps to maintain the integrity of the silicon flakes and to isolate silicon from irreversiblereactions with the electrolytes. Moreover, the carbon coating provides enhanced electricalconductivity for the SiC-encapsulated silicon flakes.Magnesium-based batteries represent one of the more successful electrochemicalenergy storage chemistries that has been emerging. Magnesium is abundant in theEarth and, due to its high density, can provide a volumetric capacity higher than lithium(3850 vs. 2046 mAh·cm−3). The review proposed by Bella and co-workers [5] focuses onthe latest developments in anode materials for Mg-ion batteries. On the one hand, themanuscript offers insights into the challenges and, on the other, provides guidance on howthey may be addressed in order to further develop this battery technology.Materials that can be applied to supercapacitors can be classified into double-layer andfaradaic types. Faradaic materials can be further distinguished as batteries and pseudo-capacitive types depending on their electrochemical signature. So-called “pseudocapaci-tive” materials are compounds that, even though they undergo redox reactions, display anelectrochemical signature that is similar to that of a double-layer-type material (i.e., cyclicvoltammetry with a box-type shape). There are few materials with this particular property,with the most prominent examples being MnO2 and RuO2. In the framework of this SpecialIssue, a needle-like MnOx@graphite nanostructure has been proposed by Ray et al. [6]. Thisnanostructured electrode was used in a symmetric pouch cell configuration with a solid-statepolymer gel electrolyte, showing an encouraging performance (areal energy density (Ea) of7.87 mWh·cm−2 and areal power density (Pa) of 1099.64 mW·cm−2 with a 2.2.V cell voltage).Thierry Brousse’s group [7] proposed a novel material, Fe2WO6, which can be addedto the short list of compounds exhibiting pseudocapacitive behavior. When used in anaqueous electrolyte as a negative electrode, Fe2WO6 can be combined with MnO2-positiveelectrode material, thus resulting in a device with an enhanced energy density with respectto classical EDLCs based on carbon electrodes.In addition to the pseudocapacitive materials, high-power faradaic compounds withclear redox peaks can be used in an asymmetric configuration, where a battery-typeelectrode is coupled with a double-layer-type one. Sharma et al. [8] explored NiMoO4and NiWO4 as positive electrode materials and investigated the effects of their anioniccounterparts (MoO4− and NiWO4−) on the electrochemical properties. They found that theredox reaction of NiMoO4 only involves a reaction between Ni2+ and Ni3+ at the surface,while NiWO4 shows a two-step redox reaction that includes the participation of a tungstenoxide layer via a bulk-type reaction. Among these two materials, NiMoO4 is considered tobe the favorite candidate for supercapacitor applications.The crucial role of inactive components, such as binders, is highlighted by the work ofBargnesi et al., who implement a chitosan binder for both Na-ion batteries and supercapacitor-type electrodes based on activated carbon [2].A further step that would enhance the overall energy density is to find strategies forthe elimination of binders from electrodes also on a large-scale production. In this respect,Ahmed et al. [9] grew ZnO nanorods directly on an aluminum substrate and appliedthem as a high-power electrode. This electrode material is promising for use in hybridsupercapacitors due to its high rate capability and stability over 1000 cycles.Nanomaterials 2022, 12, 2512 3 of 3In summary, this Special Issue compiles a series of original research articles and onereview paper, providing new insights and advances in materials and components for post-lithium systems and high-power devices, and it will be of great interest to the readersof Nanomaterials.Acknowledgments: The Guest Editors thank all the authors for submitting their work to this SpecialIssue. We particularly acknowledge all of the reviewers and the Editorial Assistant, Steve Yan, whoensured that Special Issue preparation was a very efficient process. This work contributes to theresearch performed at CELEST (Center for Electrochemical Energy Storage Ulm-Karlsruhe) andwas funded by the German Research Foundation (DFG) under Project ID 390874152 (POLiS Clusterof Excellence).Conflicts of Interest: The authors declare no conflict of interest.References1. Mosa, J.; García-García, F.J.; González-Elipe, A.R.; Aparicio, M. New Insights on the Conversion Reaction Mechanism in MetalOxide Electrodes for Sodium-Ion Batteries. Nanomaterials 2021, 11, 966. [CrossRef] [PubMed]2. Bargnesi, L.; Gigli, F.; Albanelli, N.; Toigo, C.; Arbizzani, C. Crosslinked Chitosan Binder for Sustainable Aqueous Batteries.Nanomaterials 2022, 12, 254. [CrossRef] [PubMed]3. Yang, Q.; Lu, F.; Liu, Y.; Zhang, Y.; Wang, X.; Pang, Y.; Zheng, S. Li2(BH4)(NH2) Nanoconfined in SBA-15 as Solid-State Electrolytefor Lithium Batteries. Nanomaterials 2021, 11, 946. [CrossRef] [PubMed]4. Tzeng, Y.; He, J.-L.; Jhan, C.-Y.; Wu, Y.-H. Effects of SiC and Resorcinol-Formaldehyde (RF) Carbon Coatings on Silicon-Flake-BasedAnode of Lithium Ion Battery. Nanomaterials 2021, 11, 302. [CrossRef] [PubMed]5. Bella, F.; de Luca, S.; Fagiolari, L.; Versaci, D.; Amici, J.; Francia, C.; Bodoardo, S. An Overview on Anodes for MagnesiumBatteries: Challenges towards a Promising Storage Solution for Renewables. Nanomaterials 2021, 11, 810. [CrossRef] [PubMed]6. Ray, A.; Korkut, D.; Saruhan, B. Efficient Flexible All-Solid Supercapacitors with Direct Sputter-Grown Needle-LikeMn/MnOx@Graphite-Foil Electrodes and PPC-Embedded Ionic Electrolytes. Nanomaterials 2020, 10, 1768. [CrossRef] [PubMed]7. Espinosa-Angeles, J.C.; Goubard-Bretesché, N.; Quarez, E.; Payen, C.; Sougrati, M.-T.; Crosnier, O.; Brousse, T. Investigating theCycling Stability of Fe2WO6 Pseudocapacitive Electrode Materials. Nanomaterials 2021, 11, 1405. [CrossRef] [PubMed]8. Sharma, P.; Minakshi, M.; Whale, J.; Jean-Fulcrand, A.; Garnweitner, G. Effect of the Anionic Counterpart: Molybdate vs.Tungstate in Energy Storage for Pseudo-Capacitor Applications. Nanomaterials 2021, 11, 580. [CrossRef]9. Ahmed, F.; Almutairi, G.; AlOtaibi, B.; Kumar, S.; Arshi, N.; Hussain, S.G.; Umar, A.; Ahmad, N.; Aljaafari, A. Binder-FreeElectrode Based on ZnO Nanorods Directly Grown on Aluminum Substrate for High Performance Supercapacitors. Nanomaterials2020, 10, 1979. [CrossRef] [PubMed]

Advances in Nanomaterials for Lithium-Ion/Post-Lithium-Ion Batteries and Supercapacitors

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