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Keywords = MnO2−Zn battery

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15 pages, 3882 KiB  
Article
Performance of Low-Cost Energy Dense Mixed Material MnO2-Cu2O Cathodes for Commercially Scalable Aqueous Zinc Batteries
by Gautam G. Yadav, Malesa Sammy, Jungsang Cho, Megan N. Booth, Michael Nyce, Jinchao Huang, Timothy N. Lambert, Damon E. Turney, Xia Wei and Sanjoy Banerjee
Batteries 2025, 11(8), 291; https://doi.org/10.3390/batteries11080291 - 1 Aug 2025
Viewed by 160
Abstract
Zinc (Zn)-based batteries have attracted significant interest for applications ranging from electric bikes to grid storage because of its advantageous properties like high abundance, non-toxicity and low-cost. Zn offers a high theoretical capacity of two electrons per atom, resulting in 820 mAh/g, making [...] Read more.
Zinc (Zn)-based batteries have attracted significant interest for applications ranging from electric bikes to grid storage because of its advantageous properties like high abundance, non-toxicity and low-cost. Zn offers a high theoretical capacity of two electrons per atom, resulting in 820 mAh/g, making it a promising anode material for the development of highly energy dense batteries. However, the advancement of Zn-based battery systems is hindered by the limited availability of cathode materials that simultaneously offer high theoretical capacity, long-term cycling stability, and affordability. In this work, we present a new mixed material cathode system, comprising of a mixture of manganese dioxide (MnO2) and copper oxide (Cu2O) as active materials, that delivers a high theoretical capacity of ~280 mAh/g (MnO2 + Cu2O active material) (based on the combined mass of MnO2 and Cu2O) and supports stable cycling for >200 cycles at 1C. We further demonstrate the scalability of this novel cathode system by increasing the electrode size and capacity, highlighting its potential for practical and commercial applications. Full article
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11 pages, 2330 KiB  
Article
Separations of Strategic Metals from Spent Electronic Waste Using “Green Methods”
by Urszula Domańska, Anna Wiśniewska and Zbigniew Dąbrowski
Separations 2025, 12(6), 167; https://doi.org/10.3390/separations12060167 - 18 Jun 2025
Viewed by 457
Abstract
Next-generation recycling technologies must be urgently innovated to tackle huge volumes of spent batteries, photovoltaic panels or printed circuit boards (WPCBs). Current e-waste recycling industrial technology is dominated by traditional recycling technologies. Herein, ionic liquids (ILs), deep eutectic solvents (DESs) and promising oxidizing [...] Read more.
Next-generation recycling technologies must be urgently innovated to tackle huge volumes of spent batteries, photovoltaic panels or printed circuit boards (WPCBs). Current e-waste recycling industrial technology is dominated by traditional recycling technologies. Herein, ionic liquids (ILs), deep eutectic solvents (DESs) and promising oxidizing additives that can overcome some traditional recycling methods of metal ions from e-waste, used in our works from last year, are presented. The unique chemical environments of ILs and DESs, with the application of low-temperature extraction procedures, are important environmental aspects known as “Green Methods”. A closed-loop system for recycling zinc and manganese from the “black mass” (BM) of waste, Zn-MnO2 batteries, is presented. The leaching process achieves a high efficiency and distribution ratio using the composition of two solvents (Cyanex 272 + diethyl phosphite (DPh)) for Zn(II) extraction. High extraction efficiency with 100% zinc and manganese recovery is also achieved using DESs (cholinum chloride/lactic acid, 1:2, DES 1, and cholinum chloride/malonic acid, 1:1, DES 2). New, greener recycling approaches to metal extraction from the BM of spent Li-ion batteries are presented with ILs ([N8,8,8,1][Cl], (Aliquat 336), [P6,6,6,14][Cl], [P6,6,6,14][SCN] and [Benzet][TCM]) eight DESs, Cyanex 272 and D2EHPA. A high extraction efficiency of Li(I) (41–92 wt%) and Ni(II) (37–52 wt%) using (Cyanex 272 + DPh) is obtained. The recovery of Ni(II) and Cd(II) from the BM of spent Ni-Cd batteries is also demonstrated. The extraction efficiency of DES 1 and DES 2, contrary to ILs ([P6,6,6,14][Cl] and [P6,6,6,14][SCN]), is at the level of 30 wt% for Ni(II) and 100 wt% for Cd(II). In this mini-review, the option to use ILs, DESs and Cyanex 272 for the recovery of valuable metals from end-of-life WPCBs is presented. Next-generation recycling technologies, in contrast to the extraction of metals from acidic leachate preceded by thermal pre-treatment or from solid material only after thermal pre-treatment, have been developed with ILs and DESs using the ABS method, as well as Cyanex 272 (only after the thermal pre-treatment of WPCBs), with a process efficiency of 60–100 wt%. In this process, four new ILs are used: didecyldimethylammonium propionate, [N10,10,1,1][C2H5COO], didecylmethylammonium hydrogen sulphate, [N10,10,1,H][HSO4], didecyldimethylammonium dihydrogen phosphate, [N10,10,1,1][H2PO4], and tetrabutylphosphonium dihydrogen phosphate, [P4,4,4,4][H2PO4]. The extraction of Cu(II), Ag(I) and other metals such as Al(III), Fe(II) and Zn(II) from solid WPCBs is demonstrated. Various additives are used during the extraction processes. The Analyst 800 atomic absorption spectrometer (FAAS) is used for the determination of metal content in the solid BM. The ICP-OES method is used for metal analysis. The obtained results describe the possible application of ILs and DESs as environmental media for upcycling spent electronic wastes. Full article
(This article belongs to the Section Materials in Separation Science)
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12 pages, 2114 KiB  
Article
Interface-Sensitive Charge Storage and Activation Behavior of Mn(1,3,5-Benzenetricarboxylic Acid (BTC))-Derived Mn3O4/Carbon Cathodes for Aqueous Zinc-Ion Batteries
by Jieun Lee and Byoungnam Park
Molecules 2025, 30(12), 2566; https://doi.org/10.3390/molecules30122566 - 12 Jun 2025
Viewed by 360
Abstract
In this study, we couple precise interface engineering via alternating current electrophoretic deposition (AC–EPD) with performance-enhancing structural transformation via annealing, enabling the development of high-performance, stable, and tunable Mn-based cathodes for aqueous zinc-ion batteries (ZIBs). Using AC–EPD to fabricate Mn(BTC) (BTC = 1,3,5-benzenetricarboxylic [...] Read more.
In this study, we couple precise interface engineering via alternating current electrophoretic deposition (AC–EPD) with performance-enhancing structural transformation via annealing, enabling the development of high-performance, stable, and tunable Mn-based cathodes for aqueous zinc-ion batteries (ZIBs). Using AC–EPD to fabricate Mn(BTC) (BTC = 1,3,5-benzenetricarboxylic acid) cathodes followed by thermal annealing to synthesize MOF-derived Mn3O4 offers a synergistic approach that addresses several key challenges in aqueous ZIB systems. The Mn3O4 cathode prepared via AC–EPD from Mn(BTC) exhibited a remarkable specific capacity of up to 430 mAh/g at a current density of 200 mA/g. Interestingly, the capacity continued to increase progressively with cycling, suggesting dynamic structural or interfacial changes that improved Zn2+ transport and utilization over time. Such capacity enhancement behavior during prolonged cycling at elevated rates has not been observed in previously reported Mn3O4-based ZIB systems. Kinetic analysis further revealed that the charge storage process is predominantly governed by diffusion-controlled mechanisms. This behavior can be attributed to the intrinsic characteristics of the Mn3O4 phase formed from the MOF precursor, where the bulk redox reactions involving Zn2+ insertion require ion migration into the electrode interior. Even though the electrode was processed as an ultrathin film with enhanced electrolyte contact, the charge storage remains limited by solid-state ion diffusion rather than fast surface-driven reactions, reinforcing the diffusion-dominant nature of the system. Full article
(This article belongs to the Special Issue Functional Porous Frameworks: Synthesis, Properties, and Applications)
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13 pages, 4057 KiB  
Article
Enhanced Anionic Redox Reaction of Na-Layered Li-Containing Mn-Based Cathodes by Cu-Mediated Reductive Coupling Mechanism
by Danyang Li, Can Liu, Shu Zhao, Fujie Li, Hao Li, Chao Wang and Xiu Song Zhao
Nanomaterials 2025, 15(12), 893; https://doi.org/10.3390/nano15120893 - 10 Jun 2025
Viewed by 399
Abstract
Na-layered Li-containing Mn-based cathodes (NaxLiyMn1-yO2, NLMOs) with additional Na+ storage ability resulting from the anionic redox reaction (ARR) hold great promise for sodium-ion batteries (NIBs). However, practical applications of NLMOs encounter challenges, such as [...] Read more.
Na-layered Li-containing Mn-based cathodes (NaxLiyMn1-yO2, NLMOs) with additional Na+ storage ability resulting from the anionic redox reaction (ARR) hold great promise for sodium-ion batteries (NIBs). However, practical applications of NLMOs encounter challenges, such as migration of transition metal Mn, loss of lattice oxygen, and voltage decay during cycling. Here, we show that Cu plays an important role in enhancing the ARR via the reductive coupling mechanism (RCM). Results shows that a Cu2+/Fe3+ modified NLMO sample delivers a Na+ storage capacity as high as 174 mA h g−1 at 0.2C, higher than that of a Zn2+/Fe3+ modified NLMO sample (130 mA h g−1) and NLMO (154 mA h g−1). Both in situ and ex situ characterization results indicate that the obvious improvement in the electrochemical performance of the Cu2+/Fe3+ modified NLMO is due to the additional overlaps between the Cu 3d and O 2p orbitals, which is beneficial for the RCM. As a result, the ARR is enhanced so as to increase the Na+ storage capacity. Full article
(This article belongs to the Section Energy and Catalysis)
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11 pages, 1352 KiB  
Article
Free-Standing Composite Film Based on Zinc Powder and Nanocellulose Achieving Dendrite-Free Anode of Aqueous Zinc–Ion Batteries
by Guanwen Wang, Minfeng Chen and Jizhang Chen
Materials 2025, 18(12), 2696; https://doi.org/10.3390/ma18122696 - 8 Jun 2025
Viewed by 526
Abstract
Aqueous zinc–ion batteries (AZIBs) have garnered considerable attention owing to their inherent safety, cost-effectiveness, and promising electrochemical performance. However, challenges associated with Zn metal anodes, such as dendrite formation, corrosion, and hydrogen evolution, continue to impede their widespread adoption. To overcome these limitations, [...] Read more.
Aqueous zinc–ion batteries (AZIBs) have garnered considerable attention owing to their inherent safety, cost-effectiveness, and promising electrochemical performance. However, challenges associated with Zn metal anodes, such as dendrite formation, corrosion, and hydrogen evolution, continue to impede their widespread adoption. To overcome these limitations, a flexible and self-standing composite film anode (denoted ZCN) is engineered from a synergistic combination of Zn powder, nanocellulose, and carbon fiber to serve as a high-performance alternative to conventional Zn foil. These three constituents play the roles of enhancing the active area, improving mechanical properties and electrolyte affinity, and establishing a conductive network, respectively. This innovative design effectively mitigates dendrite growth and suppresses parasitic side reactions, thereby significantly improving the cycling stability of ZCN. As a result, this electrode enables the Zn//Zn cell to offer an ultralong lifespan of 2000 h. And the Zn-MnO2 battery with ZCN anode demonstrates remarkable performance, realizing over 80% capacity retention after 1000 cycles. This study presents a straightforward, scalable, and cost-effective strategy for the development of dendrite-free metal electrodes, paving the way for durable and high-performance AZIBs. Full article
(This article belongs to the Topic Advanced Energy Storage in Aqueous Zinc Batteries)
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15 pages, 1059 KiB  
Article
Adsorption Kinetics and Isotherms of Cd (II), As (III), and Pb (II) on Green Zn-Mn Ferrite Soft Magnetic Material
by Jia Wang, Mengyi Guan, Zijian Qin, Shihao Zhang, Jian Cheng and Baoping Xin
Water 2025, 17(11), 1630; https://doi.org/10.3390/w17111630 - 27 May 2025
Viewed by 373
Abstract
In this study, a Zn-Mn ferrite soft magnetic material (Mn0.6Zn0.4Fe2O4) was successfully prepared from a spent Zn-Mn battery using a novel multi-step process involving bioleaching, co-precipitation, and boiling reflux. The green Zn–Mn ferrite exhibited optimal [...] Read more.
In this study, a Zn-Mn ferrite soft magnetic material (Mn0.6Zn0.4Fe2O4) was successfully prepared from a spent Zn-Mn battery using a novel multi-step process involving bioleaching, co-precipitation, and boiling reflux. The green Zn–Mn ferrite exhibited optimal magnetic properties, with Ms, Mr, and Hc values of 68.9 emu/g, 4.7 emu/g, and 53.6 Oe, respectively. The adsorption kinetics and isotherms of Cd (II), As (III), and Pb (II) in wastewater on Mn0.6Zn0.4Fe2O4 were subsequently investigated. The sorption dosages of Cd (II), As (III), and Pb (II) were 22.9 mg/g, 8.7 mg/g, and 33.9 mg/g, respectively. The pseudo-second-order kinetic model provided a fitting correlation with the experimental data. The adsorption process exhibited a good correlation with the Langmuir model, with R2 = 0.997, and the qm and b values were 33.44 mg/g and 2.43 L/mg, respectively. The sorption rates followed the sequence Pb (II) > Cd (II) > As (III). On increasing the temperature, the saturated adsorption capacity of the Cd (II), As (III), and Pb (II) increased, thus indicating that the adsorption reaction was endothermic, with the corresponding activation energy (Ea) values determined to be 9.5 KJ/mol, 32.2 KJ/mol, and 1.4 KJ/mol, respectively. Full article
(This article belongs to the Section Wastewater Treatment and Reuse)
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21 pages, 10702 KiB  
Review
Recent Progress in Cathode-Free Zinc Electrolytic MnO2 Batteries: Electrolytes and Electrodes
by Shiwei Liu, Zhongqi Liang, Hang Zhou, Weizheng Cai, Jiazhen Wu, Qianhui Zhang, Guoshen Yang, Walid A. Daoud, Zanxiang Nie, Pritesh Hiralal, Shiqiang Luo and Gehan A. J. Amaratunga
Batteries 2025, 11(5), 171; https://doi.org/10.3390/batteries11050171 - 23 Apr 2025
Viewed by 965
Abstract
Zinc–manganese dioxide (Zn–MnO2) batteries, pivotal in primary energy storage, face challenges in rechargeability due to cathode dissolution and anode corrosion. This review summarizes cathode-free designs using pH-optimized electrolytes and modified electrodes/current collectors. For electrolytes, while acidic systems with additives (PVP, HAc) [...] Read more.
Zinc–manganese dioxide (Zn–MnO2) batteries, pivotal in primary energy storage, face challenges in rechargeability due to cathode dissolution and anode corrosion. This review summarizes cathode-free designs using pH-optimized electrolytes and modified electrodes/current collectors. For electrolytes, while acidic systems with additives (PVP, HAc) enhance ion transport, dual-electrolyte configurations (ion-selective membranes/hydrogels) reduce Zn corrosion. Near-neutral strategies utilize nanomicelles/complexing agents to regulate MnO2 deposition. Moreover, mediators (I, Br, Cr3+) reactivate MnO2 but require shuttle-effect control. For the electrodes/current collectors, electrode innovations including SEI/CEI layers and surfactant-driven phase tuning are introduced. Electrode-free designs and integrated “supercapattery” systems combining supercapacitors with Zn–MnO2/I2 chemistries are also discussed. This review highlights electrolyte–electrode synergy and hybrid device potential, paving the way for sustainable, high-performance Zn–MnO2 systems. Full article
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12 pages, 8366 KiB  
Article
Active Poly(o-phenylenediamine)-Intercalated Layered δ-MnO2 Cathode for High-Performance Aqueous Zinc-Ion Batteries
by Ziqian Yuan, Bosi Yin, Wenhui Mi, Minghui Liu and Siwen Zhang
Polymers 2025, 17(8), 1003; https://doi.org/10.3390/polym17081003 - 8 Apr 2025
Cited by 2 | Viewed by 608
Abstract
Aqueous zinc-ion batteries (ZIBs) represent an emerging energy storage solution that offers significant advantages in terms of safety, cost-effectiveness, and longevity in cycling. Among the various materials available, manganese-based oxides stand out as the most promising options for cathodes due to their impressive [...] Read more.
Aqueous zinc-ion batteries (ZIBs) represent an emerging energy storage solution that offers significant advantages in terms of safety, cost-effectiveness, and longevity in cycling. Among the various materials available, manganese-based oxides stand out as the most promising options for cathodes due to their impressive theoretical specific capacity, suitable operating voltage, and abundant natural availability. In published reports, pre-embedding is frequently used to modify the layered cathode; however, non-electrochemically active molecular embedding often results in a decrease in battery capacity. In this paper, a hydrothermal method is employed to intercalate poly(o-phenylenediamine) (PoPD) into δ-MnO2 (MO) to produce PoPD-MO cathode materials. Here, PoPD serves a dual role in the cathode: (1) PoPD is inserted into the interlayer of MO, providing support within the intercalation layer, enhancing material stability, increasing ionic storage sites, and creating space for more Zn2+ to be embedded, and (2) inserting PoPD into the interlayer structure of MO effectively expands the space between layers, thus allowing for greater ion storage, which in turn enhances the rate and efficiency of electrochemical reactions. Consequently, PoPD-MO shows remarkable cycling durability and adaptability in ZIBs, achieving a specific capacity of 359 mAh g−1 at a current density of 0.1 A g−1, and even under the strain of a high current density of 3 A g−1, it maintains a respectable capacity of 107 mAh g−1. Based on this, PoPD-MO may emerge as a new cathode material with promising applications in the future. Full article
(This article belongs to the Special Issue Polymeric Conductive Materials for Energy Storage)
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16 pages, 3757 KiB  
Article
Improved Performances of Zn//MnO2 Batteries with an Electrolyte Containing Co-Additives of Polyethylene Glycol and Lignin Derivatives
by Muzammil Hussain Memon, Md. Asraful Alam, Qiyuan Xie, Abdul Rahman Abbasi, Lele Wang, Jingliang Xu and Wenlong Xiong
Polymers 2025, 17(7), 888; https://doi.org/10.3390/polym17070888 - 26 Mar 2025
Viewed by 766
Abstract
Multi-component electrolyte additives may significantly contribute to improving the performance of rechargeable aqueous zinc-ion batteries. Herein, we propose a mixed electrolyte system employing polyethylene glycol 200 (PEG200) and quaternized kraft lignin (QKL) as co-additives in Zn//MnO2 batteries. Reduced corrosion and the suppression [...] Read more.
Multi-component electrolyte additives may significantly contribute to improving the performance of rechargeable aqueous zinc-ion batteries. Herein, we propose a mixed electrolyte system employing polyethylene glycol 200 (PEG200) and quaternized kraft lignin (QKL) as co-additives in Zn//MnO2 batteries. Reduced corrosion and the suppression of the hydrogen evolution reaction on the zinc electrode were achieved when 0.5 wt.% of PEG200 and 0.2 wt.% of QKL were added to the reference aqueous electrolyte. This optimized electrolyte, 0.5% PEG200 + 0.2% QKL, was conducive to improving Zn reversibility in Zn//Zn symmetric batteries and resulted in higher cycling stability, with a coulombic efficiency of 98.01% under 1 mA cm−2 and 1 mAh cm−2 for Zn//Cu cells. Furthermore, Zn//MnO2 full batteries with 0.5% PEG200 + 0.2% QKL presented good overall electrochemical performance and exhibited a decent discharge capacity of around 85 mAh g−1 after 2000 cycles at 1.5 A g−1. As confirmed by X-ray diffraction and scanning electron microscopy, a dominant (002) oriental dendrite-free Zn deposition was achieved on the zinc anode of the battery using 0.5% PEG200 + 0.2% QKL, and the byproducts were also reduced significantly. This study has contributed to the development of electrolyte co-additives for zinc-ion batteries. Full article
(This article belongs to the Section Smart and Functional Polymers)
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13 pages, 3038 KiB  
Article
Enhanced Electrochemical Performance of Aqueous Zinc-Ion Batteries Using MnSO4 Electrolyte Additive and α-MnO2 Cathode
by Xinfeng Zhou, Chenchen Ji, Lingyun Wan, Xiaohui Zhang, Haopeng Wang, Longfei Xie and Jie Gao
Energies 2025, 18(6), 1420; https://doi.org/10.3390/en18061420 - 13 Mar 2025
Cited by 1 | Viewed by 1257
Abstract
Zinc-ion batteries (ZIBs) are an ideal choice for large-scale energy storage due to their high safety, environmental friendliness, and low cost. However, their performance is constrained by challenges related to cathode materials, such as poor conductivity, dissolution of active materials, and structural instability [...] Read more.
Zinc-ion batteries (ZIBs) are an ideal choice for large-scale energy storage due to their high safety, environmental friendliness, and low cost. However, their performance is constrained by challenges related to cathode materials, such as poor conductivity, dissolution of active materials, and structural instability during cycling. In this study, α-MnO2 cathode material with a tunnel structure was synthesized via a hydrothermal method, and MnSO4 was introduced into the ZnSO4 electrolyte to optimize the electrochemical performance of ZIBs. Characterizations through XRD, SEM, and BET revealed excellent crystal morphology and nanorod structures, which provided superior ion transport pathways. With the addition of MnSO4, the discharge specific capacity of ZIBs at 0.1 A g⁻1 was significantly improved from 172.9 mAh g⁻1 to 263.2 mAh g⁻1, the cycling stability was also notably enhanced, namely, after 1000 cycles with the current density of 1 mA cm−2, the capacity settled at 50 mAh g−1, which is a 47.4% increase in relation to the case of absent additive. The experimental results indicate that MnSO4 additives effectively suppress manganese dissolution, improving the rate capability and reducing self-discharge. This study provides a novel approach to the development of high-performance aqueous zinc-ion batteries. Full article
(This article belongs to the Section D2: Electrochem: Batteries, Fuel Cells, Capacitors)
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13 pages, 5818 KiB  
Article
Total Component Recovery of Waste Zn-Mn Batteries via Reduction Roasting Followed by Leaching Process: In Situ Preparation of Nano-ZnO Whiskers
by Wei Lv, Qiuyu Li and Zijian Su
Metals 2025, 15(3), 256; https://doi.org/10.3390/met15030256 - 27 Feb 2025
Viewed by 849
Abstract
Waste Zn-Mn batteries represent a significant contributor to e-waste, which is typically a hazardous material. Furthermore, Zn-Mn batteries possess more valuable metals than primary ore minerals, making them a crucial secondary resource for Zn and Mn extractive metallurgy. Current hydrometallurgy techniques primarily use [...] Read more.
Waste Zn-Mn batteries represent a significant contributor to e-waste, which is typically a hazardous material. Furthermore, Zn-Mn batteries possess more valuable metals than primary ore minerals, making them a crucial secondary resource for Zn and Mn extractive metallurgy. Current hydrometallurgy techniques primarily use acids as leaching agents, and the products are then purified by precipitating, extraction, etc. However, the Mn-Zn spinel formed in spent batteries exhibits exceptional structural stability, which can only be dissolved under strong acidic conditions. Therefore, eliminating the spinel’s effects helps improve recovery efficiency. This study introduces an innovative approach for selectively recovering Zn and Mn from spent batteries by integrating reduction roasting with acid leaching, utilizing spent graphite electrodes as environmentally friendly reductants. Meanwhile, the effect of roasting and leaching on recovery efficiency is explored, as well as the phase transformation of Zn-Mn oxides during the total component recovery process. In addition, high-value-added products, nano-ZnO whiskers, are in situ synthesized via a two-stage atmosphere-controlled process. Finally, Mn and Zn recoveries of 99.8% and 99.5% are obtained under optimal conditions, and hexagonal nano-ZnO with a crystallinity of 99.9% with a grain size of 46.3 nm is synthesized successfully. Full article
(This article belongs to the Special Issue Advances in Recycling of Valuable Metals—2nd Edition)
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11 pages, 2929 KiB  
Article
Dendrite-Free Zn Anode Modified by Organic Coating for Stable Aqueous Zinc Ion Batteries
by Fujie Li, Hongfei Zhang, Xuehua Liu, Binghui Xu and Chao Wang
Batteries 2024, 10(12), 420; https://doi.org/10.3390/batteries10120420 - 29 Nov 2024
Cited by 2 | Viewed by 1912
Abstract
Aqueous zinc-ion batteries (AZIBs) have emerged as highly promising options for large-scale energy storage systems due to their cost-effectiveness, substantial energy capacity, and improved safety features. However, the Zn anode faces challenges such as self-corrosion and dendrite formation, which limit its practical use [...] Read more.
Aqueous zinc-ion batteries (AZIBs) have emerged as highly promising options for large-scale energy storage systems due to their cost-effectiveness, substantial energy capacity, and improved safety features. However, the Zn anode faces challenges such as self-corrosion and dendrite formation, which limit its practical use in AZIB applications. In this work, a simple blade-coating method was used to successfully coat poly (vinylidene fluoride–hexafluoro propylene) (PVDF-HFP) on the Zn anode. The coated Zn anode (P-Zn) displayed a stable cycling performance (700 h) at 1 mA cm−2 current density in the symmetric cell. In addition, the full cell using MnO2 as the cathode and P-Zn as the anode retained almost full capacity even after 1400 cycles at 2C, far outperforming the full cell using the unmodified Zn anode with only 50% capacity retention after 600 cycles. In situ optical observations of Zn deposition demonstrate that the special organic coating significantly enhances the uniform deposition of Zn2+, thus effectively mitigating corrosion and hydrogen evolution. Density Functional Theory (DFT) calculations show that the PVDF-HFP coating effectively narrows the adsorption energy gap between the P-Zn (002) and (101) planes, leading to the homogeneous deposition of Zn2+ with fewer Zn dendrites. A simple and feasible strategy for designing ultra-stable AZIBs by coating an organic protective layer on the Zn surface is provided by this work. Full article
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10 pages, 1305 KiB  
Article
Manganese-Coordinated Cellulose Based-Separator for Efficient and Reliable Zn-Ion Transport
by Jiazhe Cheng, Kai Wang, Xiaoyu Ning, Jichao Zhang, Hao Jia, Benjamin Tawiah and Shouxiang Jiang
Batteries 2024, 10(12), 416; https://doi.org/10.3390/batteries10120416 - 27 Nov 2024
Viewed by 1059
Abstract
Aqueous zinc-ion batteries (AZIBs) are increasingly being acknowledged as a promising candidate to safely power large-scale energy storage systems and portable devices. However, the development of effective separator materials remains a significant challenge due to issues such as harmful dendrite growth on zinc [...] Read more.
Aqueous zinc-ion batteries (AZIBs) are increasingly being acknowledged as a promising candidate to safely power large-scale energy storage systems and portable devices. However, the development of effective separator materials remains a significant challenge due to issues such as harmful dendrite growth on zinc (Zn) anodes and parasitic side reactions in aqueous electrolytes. To address this challenge, we synthesize a manganese-coordinated cellulose nanofibril (Mn-CNF)-based separator for high-performance AZIBs. This separator affords enhanced ion transport channel, a large number of hydroxyl groups, and exceptional mechanical properties, with a tensile strength of 2.8 MPa and superior ionic conductivity of 5.14 mS·cm−1. These attributes collectively enhance Zn-ion transport, minimize nucleation overpotential for Zn, and accelerate the Zn deposition kinetics, thus significantly outperforming the untreated CNF separators. Consequently, the Zn||MnO2 battery with the Mn-CNF separator shows a marked improvement in the galvanostatic rate performance and cycling stability by effectively accelerating and optimizing Zn-ion transport. This study offers valuable insights into the development of efficient and reliable separators for advanced electrochemical energy storage technologies. Full article
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23 pages, 6021 KiB  
Article
Structural, Optical, Magnetic, and Dielectric Investigations of Pure and Co-Doped La0.67Sr0.33Mn1-x-yZnxCoyO3 Manganites with (0.00 < x + y < 0.20)
by Mansour Mohamed, A. Sedky, Abdullah S. Alshammari, Z. R. Khan, M. Bouzidi and Marzook S. Alshammari
Crystals 2024, 14(11), 981; https://doi.org/10.3390/cryst14110981 - 14 Nov 2024
Cited by 1 | Viewed by 1044
Abstract
Here, we report the structural, optical, magnetic, and dielectric properties of La0.67Sr0.33Mn1-x-yZnxCoyO3 manganite with various x and y values (0.025 < x + y < 0.20). The pure and co-doped samples are [...] Read more.
Here, we report the structural, optical, magnetic, and dielectric properties of La0.67Sr0.33Mn1-x-yZnxCoyO3 manganite with various x and y values (0.025 < x + y < 0.20). The pure and co-doped samples are called S1, S2, S3, S4, and S5, with (x + y) = 0.00, 0.025, 0.05, 0.10, and 0.20, respectively. The XRD confirmed a monoclinic structure for all the samples, such that the unit cell volume and the size of the crystallite and grain were generally decreased by increasing the co-doping content (x + y). The opposite was true for the behaviors of the porosity, the Debye temperature, and the elastic modulus. The energy gap Eg was 3.85 eV for S1, but it decreased to 3.82, 3.75, and 3.65 eV for S2, S5, and S3. Meanwhile, it increased and went to its maximum value of 3.95 eV for S4. The values of the single and dispersion energies (Eo, Ed) were 9.55 and 41.88 eV for S1, but they were decreased by co-doping. The samples exhibited paramagnetic behaviors at 300 K, but they showed ferromagnetic behaviors at 10 K. For both temperatures, the saturated magnetizations (Ms) were increased by increasing the co-doping content and they reached their maximum values of 1.27 and 15.08 (emu/g) for S4. At 300 K, the co-doping changed the magnetic material from hard to soft, but it changed from soft to hard at 10 K. In field cooling (FC), the samples showed diamagnetic regime behavior (M < 0) below 80 K, but this behavior was completely absent for zero field cooling (ZFC). In parallel, co-doping of up to 0.10 (S4) decreased the dielectric constant, AC conductivity, and effective capacitance, whereas the electric modulus, impedance, and bulk resistance were increased. The analysis of the electric modulus showed the presence of relaxation peaks for all the samples. These outcomes show a good correlation between the different properties and indicate that co-doping of up to 0.10 of Zn and Co in place of Mn in La:113 compounds is beneficial for elastic deformation, optoelectronics, Li-batteries, and spintronic devices. Full article
(This article belongs to the Special Issue Crystal Structures and Magnetic Interactions of Magnetic Materials)
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14 pages, 9773 KiB  
Article
High-Entropy and Component Stoichiometry Tuning Strategies Boost the Sodium-Ion Storage Performance of Cobalt-Free Prussian Blue Analogues Cathode Materials
by Yuan-Ting Lin, Bai-Tong Niu, Zi-Han Wang, Yu-Xi Li, Yun-Peng Xu, Shi-Wei Liu, Yan-Xin Chen and Xiu-Mei Lin
Molecules 2024, 29(19), 4559; https://doi.org/10.3390/molecules29194559 - 25 Sep 2024
Cited by 2 | Viewed by 2047
Abstract
Prussian blue analogs (PBAs) are appealing cathode materials for sodium-ion batteries because of their low material cost, facile synthesis methods, rigid open framework, and high theoretical capacity. However, the poor electrical conductivity, unavoidable presence of [Fe(CN)6] vacancies and crystalline water within [...] Read more.
Prussian blue analogs (PBAs) are appealing cathode materials for sodium-ion batteries because of their low material cost, facile synthesis methods, rigid open framework, and high theoretical capacity. However, the poor electrical conductivity, unavoidable presence of [Fe(CN)6] vacancies and crystalline water within the framework, and phase transition during charge–discharge result in inferior electrochemical performance, particularly in terms of rate capability and cycling stability. Here, cobalt-free PBAs are synthesized using a facile and economic co-precipitation method at room temperature, and their sodium-ion storage performance is boosted due to the reduced crystalline water content and improved electrical conductivity via the high-entropy and component stoichiometry tuning strategies, leading to enhanced initial Coulombic efficiency (ICE), specific capacity, cycling stability, and rate capability. The optimized HE-HCF of Fe0.60Mn0.10-hexacyanoferrate (referred to as Fe0.60Mn0.10-HCF), with the chemical formula Na1.156Fe0.599Mn0.095Ni0.092Cu0.109Zn0.105 [Fe(CN)6]0.724·3.11H2O, displays the most appealing electrochemical performance of an ICE of 100%, a specific capacity of around 115 and 90 mAh·g−1 at 0.1 and 1.0 A·g−1, with 66.7% capacity retention observed after 1000 cycles and around 61.4% capacity retention with a 40-fold increase in specific current. We expect that our findings could provide reference strategies for the design of SIB cathode materials with superior electrochemical performance. Full article
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