Research

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12 pages, 5059 KiB

Open AccessArticle

Rational Design of Ni-Doped V₂O₅@3D Ni Core/Shell Composites for High-Voltage and High-Rate Aqueous Zinc-Ion Batteries

by Songhe Zheng, Jianping Chen, Ting Wu, Ruimin Li, Xiaoli Zhao, Yajun Pang and Zhenghui Pan

Materials 2024, 17(1), 215; https://0-doi-org.brum.beds.ac.uk/10.3390/ma17010215 - 30 Dec 2023

Viewed by 914

Abstract

Aqueous zinc-ion batteries (ZIBs) have significant potential for large energy storage systems because of their high energy density, cost-effectiveness and environmental friendliness. However, the limited voltage window, poor reaction kinetics and structural instability of cathode materials are current bottlenecks which contain the further [...] Read more.

Aqueous zinc-ion batteries (ZIBs) have significant potential for large energy storage systems because of their high energy density, cost-effectiveness and environmental friendliness. However, the limited voltage window, poor reaction kinetics and structural instability of cathode materials are current bottlenecks which contain the further development of ZIBs. In this work, we rationally design a Ni-doped V₂O₅@3D Ni core/shell composite on a carbon cloth electrode (Ni-V₂O₅@3D Ni@CC) by growing Ni-V₂O₅ on free-standing 3D Ni metal nanonets for high-voltage and high-capacity ZIBs. Impressively, embedded Ni doping increases the interlayer spacing of V₂O₅, extending the working voltage and improving the zinc-ion (Zn₃₀²⁺) reaction kinetics of the cathode materials; at the same time, the 3D structure, with its high specific surface area and superior electronic conductivity, aids in fast Zn₃₀²⁺ transport. Consequently, the as-designed Ni-V₂O₅@3D Ni@CC cathodes can operate within a wide voltage window from 0.3 to 1.8 V vs. Zn₃₀/Zn₃₀²⁺ and deliver a high capacity of 270 mAh g⁻¹ (~1050 mAh cm⁻³) at a high current density of 0.8 A g⁻¹. In addition, reversible Zn²⁺ (de)incorporation reaction mechanisms in the Ni-V₂O₅@3D Ni@CC cathodes are investigated through multiple characterization methods (SEM, TEM, XRD, XPS, etc.). As a result, we achieved significant progress toward practical applications of ZIBs. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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18 pages, 4182 KiB

Open AccessArticle

Unraveling the Phase Transition Behavior of MgMn₂O₄ Electrodes for Their Use in Rechargeable Magnesium Batteries

by Carmen Miralles, Teresa Lana-Villarreal and Roberto Gómez

Materials 2023, 16(15), 5402; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16155402 - 01 Aug 2023

Cited by 1 | Viewed by 883

Abstract

Rechargeable magnesium batteries are an attractive alternative to lithium batteries because of their higher safety and lower cost, being spinel-type materials promising candidates for their positive electrode. Herein, MgMn₂O₄ with a tetragonal structure is synthesized via a simple, low-cost Pechini [...] Read more.

Rechargeable magnesium batteries are an attractive alternative to lithium batteries because of their higher safety and lower cost, being spinel-type materials promising candidates for their positive electrode. Herein, MgMn₂O₄ with a tetragonal structure is synthesized via a simple, low-cost Pechini methodology and tested in aqueous media. Electrochemical measurements combined with in-situ Raman spectroscopy and other ex-situ physicochemical characterization techniques show that, in aqueous media, the charge/discharge process occurs through the co-intercalation of Mg²⁺ and water molecules. A progressive structure evolution from a well-defined spinel to a birnessite-type arrangement occurs during the first cycles, provoking capacity activation. The concomitant towering morphological change induces poor cycling performance, probably due to partial delamination and loss of electrical contact between the active film and the substrate. Interestingly, both MgMn₂O₄ capacity retention and cyclability can be increased by doping with nickel. This work provides insights into the positive electrode processes in aqueous media, which is vital for understanding the charge storage mechanism and the correlated performance of spinel-type host materials. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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24 pages, 18801 KiB

Open AccessArticle

An Efficient Methodology Combining K-Means Machine Learning and Electrochemical Modelling for the Determination of Ionic Diffusivity and Kinetic Properties in Battery Electrodes

by Odile Capron and Luis D. Couto

Materials 2023, 16(14), 5146; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16145146 - 21 Jul 2023

Viewed by 807

Abstract

This paper presents an innovative and efficient methodology for the determination of the solid-state diffusion coefficient in electrode materials with phase transitions for which the assumption of applying the well-known formula from the work of Weppner et al. is not satisfied. This methodology [...] Read more.

This paper presents an innovative and efficient methodology for the determination of the solid-state diffusion coefficient in electrode materials with phase transitions for which the assumption of applying the well-known formula from the work of Weppner et al. is not satisfied. This methodology includes a k-means machine learning screening of Galvanostatic Intermittent Titration Technique (GITT) steps, whose outcomes feed a physics-informed algorithm, the latter involving a pseudo-two-dimensional (P2D) electrochemical model for carrying out the numerical simulations. This methodology enables determining, for all of the 47 steps of the GITT characterization, the dependency of the Na⁺ diffusion coefficient as well as the reaction rate constant during the sodiation of an NVPF electrode to vary between

9

×

10^{- 18}

and

6.8

×

10^{- 16}

m²·s⁻¹ and between

2.7

×

10^{- 14}

and

1.5

×

10^{- 12}

m^2.5·mol^−0.5·s⁻¹, respectively. This methodology, also validated in this paper, is (a) innovative since it presents for the first time the successful application of unsupervised machine learning via k-means clustering for the categorization of GITT steps according to their characteristics in terms of voltage; (b) efficient given the considerable reduction in the number of iterations required with an average number of iterations equal to 8, and given the fact the entire experimental duration of each step should not be simulated anymore and hence can be simply restricted to the part with current and a small part of the rest period; (c) generically applicable since the methodology and its physics-informed algorithm only rely on “if” and “else” statements, i.e., no particular module/toolbox is required, which enables its replication and implementation for electrochemical models written in any programming language. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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17 pages, 2706 KiB

Open AccessArticle

Recycled and Nickel- or Cobalt-Doped Lead Materials from Lead Acid Battery: Voltammetric and Spectroscopic Studies

by Simona Rada, Andrei Pintea, Razvan Opre, Mihaela Unguresan and Adriana Popa

Materials 2023, 16(13), 4507; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16134507 - 21 Jun 2023

Cited by 2 | Viewed by 808

Abstract

The active mass of the plates of aspent car battery with higher wear after an efficient desulfatization can be used as sources of a new electrode. This paper proposes the recycling of spent electrodes from a lead acid battery and the incorporation of [...] Read more.

The active mass of the plates of aspent car battery with higher wear after an efficient desulfatization can be used as sources of a new electrode. This paper proposes the recycling of spent electrodes from a lead acid battery and the incorporation of NiO or Co₃O₄ contents by the melt-quenching method in order to enrich the electrochemical properties. The analysis of X-ray diffractograms indicates the gradual decrease in the sulfated crystalline phases, respectively, 4PbO·PbSO₄ and PbO·PbSO₄ phases, until their disappearance for higher dopant concentrations. Infrared (IR) spectra show a decreasing trend in the intensity of the bands corresponding to the sulfate ions and a conversion of [PbO₃] pyramidal units into [PbO₄] tetrahedral units by doping with high dopant levels, yielding to the apparition of the PbO₂ crystalline phase. The observed electron paramagnetic resonance (EPR) spectra confirm three signals located on the gyromagnetic factor, g~2, 2.2 and 8 assigned to the nickel ions in higher oxidation states as well as the metallic nickel nanoparticles. This compositional evolution can be explained by considering a process of the drastic reduction in nickel ions from the superior oxidation states to metallic nickel. The linewidth and the intensity of the resonance lines situated at about g~2, 2.17, 4.22 and 7.8 are attributed to the Co⁺² ions from the EPR data. The best reversibility of the cyclic voltammograms was highlighted for the samples with x = 10 mol% of NiO and 15 mol% of Co₃O₄, which are recommended as suitable in applications as new electrodes for the lead acid battery. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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17 pages, 4185 KiB

Open AccessArticle

Nanostructured Thick Electrode Strategies toward Enhanced Electrode–Electrolyte Interfaces

by Anukriti Pokhriyal, Rosa M. González-Gil, Leandro N. Bengoa and Pedro Gómez-Romero

Materials 2023, 16(9), 3439; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16093439 - 28 Apr 2023

Viewed by 1837

Abstract

This article addresses the issue of bulk electrode design and the factors limiting the performance of thick electrodes. Indeed, one of the challenges for achieving improved performance in electrochemical energy storage devices (batteries or supercapacitors) is the maximization of the ratio between active [...] Read more.

This article addresses the issue of bulk electrode design and the factors limiting the performance of thick electrodes. Indeed, one of the challenges for achieving improved performance in electrochemical energy storage devices (batteries or supercapacitors) is the maximization of the ratio between active and non-active components while maintaining ionic and electronic conductivity of the assembly. In this study, we developed and compared supercapacitor thick electrodes using commercially available carbons and utilising conventional, easily scalable methods such as spray coating and freeze-casting. We also compared different binders and conductive carbons to develop thick electrodes and analysed factors that determine the performance of such thick electrodes, such as porosity and tortuosity. The spray-coated electrodes showed high areal capacitances of 1428 mF cm⁻² at 0.3 mm thickness and 2459 F cm⁻² at 0.6 mm thickness. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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14 pages, 3476 KiB

Open AccessEditor’s ChoiceArticle

Bismuth−Antimony Alloy Embedded in Carbon Matrix for Ultra-Stable Sodium Storage

by Wensheng Ma, Bin Yu, Fuquan Tan, Hui Gao and Zhonghua Zhang

Materials 2023, 16(6), 2189; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16062189 - 09 Mar 2023

Cited by 2 | Viewed by 1529

Abstract

Alloy-type anodes are the most promising candidates for sodium-ion batteries (SIBs) due to their impressive Na storage capacity and suitable voltage platform. However, the implementation of alloy-type anodes is significantly hindered by their huge volume expansion during the alloying/dealloying processes, which leads to [...] Read more.

Alloy-type anodes are the most promising candidates for sodium-ion batteries (SIBs) due to their impressive Na storage capacity and suitable voltage platform. However, the implementation of alloy-type anodes is significantly hindered by their huge volume expansion during the alloying/dealloying processes, which leads to their pulverization and detachment from current collectors for active materials and the unsatisfactory cycling performance. In this work, bimetallic Bi−Sb solid solutions in a porous carbon matrix are synthesized by a pyrolysis method as anode material for SIBs. Adjustable alloy composition, the introduction of porous carbon matrix, and nanosized bimetallic particles effectively suppress the volume change during cycling and accelerate the electrons/ions transport kinetics. The optimized Bi₁Sb₁@C electrode exhibits an excellent electrochemical performance with an ultralong cycle life (167.2 mAh g⁻¹ at 1 A g⁻¹ over 8000 cycles). In situ X-ray diffraction investigation is conducted to reveal the reversible and synchronous sodium storage pathway of the Bi₁Sb₁@C electrode: (Bi,Sb) Na(Bi,Sb) Na₃(Bi,Sb). Furthermore, online electrochemical mass spectrometry unveils the evolution of gas products of the Bi₁Sb₁@C electrode during the cell operation. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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13 pages, 3414 KiB

Open AccessArticle

Natrium Diacid Phosphate-Manganese-Lead Vitroceramics Obtained from Spent Electrodes

by Denisa Cuibus, Simona Rada, Sergiu Macavei and Horatiu Vermesan

Materials 2023, 16(5), 2018; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16052018 - 28 Feb 2023

Cited by 1 | Viewed by 1086

Abstract

NaH₂PO₄-MnO₂-PbO₂-Pb vitroceramics were studied usinginfrared (IR), ultraviolet-visible (UV-Vis) and electron paramagnetic resonance (EPR) spectroscopies to understand the structural modifications as potential candidates for electrode materials. The electrochemical performances of the NaH₂PO₄-MnO [...] Read more.

NaH₂PO₄-MnO₂-PbO₂-Pb vitroceramics were studied usinginfrared (IR), ultraviolet-visible (UV-Vis) and electron paramagnetic resonance (EPR) spectroscopies to understand the structural modifications as potential candidates for electrode materials. The electrochemical performances of the NaH₂PO₄-MnO₂-PbO₂-Pb materials were investigated through measurements of cyclic voltammetry. Analysis of the results indicates that doping with a suitable content of MnO₂ and NaH₂PO₄ removes hydrogen evolution reactions and produces a partial desulphatization of the anodic and cathodic plates of the spent lead acid battery. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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17 pages, 4871 KiB

Open AccessArticle

Water Kefir Grains—Microbial Biomass Source for Carbonaceous Materials Used as Sulfur-Host Cathode in Li-S Batteries

by Ana L. Páez Jerez, M. Fernanda Mori, Victoria Flexer and Alvaro Y. Tesio

Materials 2022, 15(24), 8856; https://0-doi-org.brum.beds.ac.uk/10.3390/ma15248856 - 12 Dec 2022

Cited by 3 | Viewed by 1782

Abstract

Nowadays, the use of biomass to produce cathode materials for lithium–sulfur (Li-S) batteries is an excellent alternative due to its numerous advantages. Generally, biomass-derived materials are abundant, and their production processes are environmentally friendly, inexpensive, safe, and easily scalable. Herein, a novel biomass-derived [...] Read more.

Nowadays, the use of biomass to produce cathode materials for lithium–sulfur (Li-S) batteries is an excellent alternative due to its numerous advantages. Generally, biomass-derived materials are abundant, and their production processes are environmentally friendly, inexpensive, safe, and easily scalable. Herein, a novel biomass-derived material was used as the cathode material in Li-S batteries. The synthesis of the new carbonaceous materials by simple carbonization and washing of water kefir grains, i.e., a mixed culture of micro-organisms, is reported. The carbonaceous materials were characterized morphologically, texturally and chemically by using scanning electron microscopy, N₂ adsorption–desorption, thermogravimetric analysis, X-ray diffraction, and both Raman and X-ray photoelectron spectroscopy. After sulfur infiltration using the melt diffusion method, a high sulfur content of ~70% was achieved. Results demonstrated that the cell fitted with a cathode prepared following a washing step with distilled water after carbonization of the water kefir grains only, i.e., not subjected to any chemical activation, achieved good electrochemical performance at 0.1 C. The cell reached capacity values of 1019 and 500 mAh g⁻¹ sulfur for the first cycle and after 200 cycles, respectively, at a high mass loading of 2.5 mg_S cm⁻². Finally, a mass loading study was carried out. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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Review

Jump to: Research

33 pages, 7084 KiB

Open AccessReview

Review and New Perspectives on Non-Layered Manganese Compounds as Electrode Material for Sodium-Ion Batteries

by Ricardo Alcántara, Carlos Pérez-Vicente, Pedro Lavela, José L. Tirado, Alejandro Medina and Radostina Stoyanova

Materials 2023, 16(21), 6970; https://0-doi-org.brum.beds.ac.uk/10.3390/ma16216970 - 30 Oct 2023

Viewed by 1142

Abstract

After more than 30 years of delay compared to lithium-ion batteries, sodium analogs are now emerging in the market. This is a result of the concerns regarding sustainability and production costs of the former, as well as issues related to safety and toxicity. [...] Read more.

After more than 30 years of delay compared to lithium-ion batteries, sodium analogs are now emerging in the market. This is a result of the concerns regarding sustainability and production costs of the former, as well as issues related to safety and toxicity. Electrode materials for the new sodium-ion batteries may contain available and sustainable elements such as sodium itself, as well as iron or manganese, while eliminating the common cobalt cathode compounds and copper anode current collectors for lithium-ion batteries. The multiple oxidation states, abundance, and availability of manganese favor its use, as it was shown early on for primary batteries. Regarding structural considerations, an extraordinarily successful group of cathode materials are layered oxides of sodium, and transition metals, with manganese being the major component. However, other technologies point towards Prussian blue analogs, NASICON-related phosphates, and fluorophosphates. The role of manganese in these structural families and other oxide or halide compounds has until now not been fully explored. In this direction, the present review paper deals with the different Mn-containing solids with a non-layered structure already evaluated. The study aims to systematize the current knowledge on this topic and highlight new possibilities for further study, such as the concept of entatic state applied to electrodes. Full article

(This article belongs to the Special Issue Advanced Electrode Materials for Batteries)

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