Vanadium Hexacyanoferrate Nanoparticles Connected by Cross-Linked Carbon Nanotubes Conductive Networks for Aqueous Zinc-Ion Batteries

Abstract Developing high-performance aqueous Zn-ion batteries from sustainable biomass becomes increasingly vital for large-scale energy storage in the foreseeable future. Therefore, γ-MnO 2 uniformly loaded on N-doped carbon derived from grapefruit peel is successfully fabricated in this work, and particularly the composite cathode with carbon carrier quality percentage of 20 wt% delivers the specific capacity of 391.2 mAh g −1 at 0.1 A g −1 , outstanding cyclic stability of 92.17% after 3000 cycles at 5 A g −1 , and remarkable energy density of 553.12 Wh kg −1 together with superior coulombic efficiency of ~ 100%. Additionally, the cathodic biosafety is further explored specifically through in vitro cell toxicity experiments, which verifies its tremendous potential in the application of clinical medicine. Besides, Zinc ion energy storage mechanism of the cathode is mainly discussed from the aspects of Jahn–Teller effect and Mn domains distribution combined with theoretical analysis and experimental data. Thus, a novel perspective of the conversion from biomass waste to biocompatible Mn-based cathode is successfully developed. 

Discovering Cathodic Biocompatibility for Aqueous Zn–MnO2 Battery: An Integrating Biomass Carbon Strategy

Aqueous zinc-ion batteries (ZIBs) have attracted extensive attention in recent years because of its high volumetric energy density, the abundance of zinc resources, and safety. However, ZIBs still suffer from poor reversibility and sluggish kinetics derived from the unstable cathodic structure and the strong electrostatic interactions between bivalent Zn2+ and cathodes. Herein, magnesium doping into layered manganese dioxide (Mg-MnO2 ) via a simple hydrothermal method as cathode materials for ZIBs is proposed. The interconnected nanoflakes of Mg-MnO2 possess a larger specific surface area compared to pristine δ-MnO2 , providing more electroactive sites and boosting the capacity of batteries. The ion diffusion coefficients of Mg-MnO2 can be enhanced due to the improved electrical conductivity by doped cations and oxygen vacancies in MnO2 lattices. The assembled Zn//Mg-MnO2 battery delivers a high specific capacity of 370 mAh g-1 at a current density of 0.6 A g-1 . Furthermore, the reaction mechanism confirms that Zn2+ insertion occurred after a few cycles of activation reactions. Most important, the reversible redox reaction between Zn2+ and MnOOH is found after several charge-discharge processes, promoting capacity and stability. It believes that this systematic research enlightens the design of high-performance of ZIBs and facilitates the practical application of Zn//MnO2 batteries.

Triggering High Capacity and Superior Reversibility of Manganese Oxides Cathode via Magnesium Modulation for Zn//MnO2 Batteries.

Aqueous zinc‐ion micro‐batteries (ZIMBs) have attracted considerable attention owing to their reliable safety, low cost, and great potential for wearable devices. However, current ZIMBs still suffer from various critical issues, including short cycle life, poor mechanical stability, and inadequate energy density. Herein, the fabrication of flexible planar ZIMBs with ultrahigh energy density by interfacial engineering in the screen‐printing process based on high‐performance MnO2‐based cathode materials is reported. The Ce‐doped MnO2 (Ce‐MnO2) exhibits significantly enhanced capacity (389.3 mAh g−1), considerable rate capability and admirable cycling stability than that of the pure MnO2. Importantly, the fabrication of micro‐electrodes with ultrahigh mass loading of Ce‐MnO2 (24.12 mg cm−2) and good mechanical stability is achieved through optimizing the interfacial bonding between different printed layers. The fabricated planar ZIMBs achieve a record high capacity (7.21 mAh cm−2 or 497.31 mAh cm−3) and energy density (8.43 mWh cm−2 or 573.45 mWh cm−3), as well as excellent flexibility. Besides, a wearable self‐powered sensing system for environmental monitoring is further demonstrated by integrating the planar ZIMBs with flexible solar cells and a multifunctional sensor array. This work sheds light on the development of high‐performance planar ZIMBs for future self‐powered and eco‐friendly smart wearable electronics.

A Flexible and Safe Planar Zinc‐Ion Micro‐Battery with Ultrahigh Energy Density Enabled by Interfacial Engineering for Wearable Sensing Systems

MnO2 is a promising cathode for aqueous Zn batteries. However, the cycling stability is seriously hindered by active material dissolution, and the pre-addition of Mn2+ salts in electrolytes is widely required. Herein, we propose a structural engineering strategy for MnO2 to enhance the capacity contribution from the reversible two-electron transfer reaction of MnO2/Mn2+ and realize stable cycling in Mn2+-free electrolytes. By compositing with MoO3, MnO2 exhibits weakened Mn-O bonds, more oxygen vacancies, spontaneous generation of structural water, and thus a lowered energy barrier for Mn release during discharge. Meanwhile, the composite material presents stronger electrostatic attractions for dissolved Mn2+, which ensures highly reversible re-deposition during charge. As a result, the mass ratios between materials undergoing reversible two-electron and one-electron transfer reactions increase from 0.85 in MnO2 to 1.68 in the MnO2/MoO3 composite material. In the ZnSO4 electrolyte, the MnO2/MoO3 cathode achieves 92.6% capacity retention after 300 cycles at 0.1 A g-1 (>1900 h), superior to 62.7% for MnO2. MnO2/MoO3 also retains 80.1% capacity after 16 000 cycles at 1 A g-1 (>3200 h). This work presents an effective path to realize stable cycling of MnO2 in Zn batteries.

Enhancing Two-Electron Reaction Contribution in MnO2 Cathode Material by Structural Engineering for Stable Cycling in Aqueous Zn Batteries.

Encapsulation of Zn/Co nanocrystals into sponge‐like 3D porous carbon for Escherichia coli inactivation coupled with ultrasound: Characterization, kinetics and inactivation mechanism

In this study, Fe/N codoped porous graphitic carbon derived from macadamia shells was prepared at different temperatures as cathodic catalysts for microbial fuel cells (MFCs), with K2FeO4 as a bifunctional catalyst for porosity and graphitization. The catalyst prepared at 750 °C (referred to as MSAC-750) showed a large specific surface area (1670.3 m2 g−1), graphite structure, and high pyridine-N and Fe-NX contents. Through the electrochemical workstation test, MSAC-750 shows excellent oxygen reduction reaction (ORR) activity, with an onset potential of 0.172 V and a half-wave potential of −0.028 V (vs. Ag/AgCl) in a neutral medium, and the ORR electron transfer number is 3.89. When applied to the MFCs as cathodic catalysts, a higher maximum power density and voltage of 378.68 mW m−2 and 0.425 V were achieved with the MSAC-750 catalyst and is superior to that of the Pt/C catalyst (300.85 mW m−2 and 0.402 V). In this case, a promising method is hereby established for the preparation of an excellent electrochemical catalyst for microbial fuel cells using inexpensive and easily available macadamia shells.

https://pubs.rsc.org/en/content/articlepdf/2022/ra/d2ra04214b

Fe/N codoped porous graphitic carbon derived from macadamia shells as an efficient cathode oxygen reduction catalyst in microbial fuel cells

Encapsulation of Zn/Co Nanocrystals into Sponge‐Like 3d Porous Carbon for Escherichia Coli Inactivation Coupled with Ultrasound: Characterization, Kinetics and Inactivation Mechanism

Inexpensive and Eco-Friendly Nanostructured Birnessite-Type Δ-Mno2: A Design Strategy from Oxygen Defect Engineering and K+ Pre-Intercalation

Boosting Zinc Storage in Potassium-Birnessite Via Organic-Inorganic Electrolyte Strategy with Slight N-Methyl-2-Pyrrolidone Additive

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Encapsulation of Zn/Co nanocrystals into sponge‐like 3D porous carbon for Escherichia coli inactivation coupled with ultrasound: Characterization, kinetics and inactivation mechanism

Fe/N codoped porous graphitic carbon derived from macadamia shells as an efficient cathode oxygen reduction catalyst in microbial fuel cells

Encapsulation of Zn/Co Nanocrystals into Sponge‐Like 3d Porous Carbon for Escherichia Coli Inactivation Coupled with Ultrasound: Characterization, Kinetics and Inactivation Mechanism

Inexpensive and Eco-Friendly Nanostructured Birnessite-Type Δ-Mno2: A Design Strategy from Oxygen Defect Engineering and K+ Pre-Intercalation

Boosting Zinc Storage in Potassium-Birnessite Via Organic-Inorganic Electrolyte Strategy with Slight N-Methyl-2-Pyrrolidone Additive