Zn metal has been regarded as the most promising anode for aqueous batteries due to its high capacity, low cost, and environmental benignity. Zn anode still suffers, however, from low Coulombic efficiency due to the side reactions and dendrite growth in slightly acidic electrolytes. Here, the Zn plating/stripping mechanism is thoroughly investigated in 1 m ZnSO4 electrolyte, demonstrating that the poor performance of Zn metal in mild electrolyte should be ascribed to the formation of a porous by-product (Zn4SO4(OH)6·xH2O) layer and serious dendrite growth. To suppress the side reactions and dendrite growth, a highly viscoelastic polyvinyl butyral film, functioning as an artificial solid/electrolyte interphase (SEI), is homogeneously deposited on the Zn surface via a simple spin-coating strategy. This dense artificial SEI film not only effectively blocks water from the Zn surface but also guides the uniform stripping/plating of Zn ions underneath the film due to its good adhesion, hydrophilicity, ionic conductivity, and mechanical strength. Consequently, this side-reaction-free and dendrite-free Zn electrode exhibits high cycling stability and enhanced Coulombic efficiency, which also contributes to enhancement of the full-cell performance when it is coupled with MnO2 and LiFePO4 cathodes.

Designing Dendrite-Free Zinc Anodes for Advanced Aqueous Zinc Batteries

Aqueous Zn-ion batteries (ZIBs) have inspired an overwhelming number of literature studies due to their safety, cost effectiveness, and environmental benignity. Directly employing metallic Zn foil as an anode significantly simplifies battery manufacturing and simultaneously broadens the operating voltage window of aqueous batteries, benefiting from its high overpotential against electrolyte decomposition. Nevertheless, serious issues, such as dendrite growth and side reactions, occurring at the Zn/electrolyte interphase, make the Coulombic efficiency and lifespan of Zn metal electrodes far from satisfactory, which has also been motivating new research interest in interfacial engineering to solve these problems. Owing to the rapid evolution of this new area, it is highly desirable to provide current and timely updates of interfacial strategies and their effectiveness evaluation. From the two sides – the electrode and the electrolyte at the interphase – this review thoroughly summarizes our fundamental understanding of interfacial strategies, including designing mechanisms, creating new methods, and technical challenges. Importantly, this review also analyses the effectiveness evaluation techniques for interfacial strategies, including electrochemical methods, characterization measurements, and computational simulations, providing guidelines for the accurate evaluation and analysis of ZIBs in the future.

Regulation methods for the Zn/electrolyte interphase and the effectiveness evaluation in aqueous Zn-ion batteries

Solid-state lithium–sulfur batteries (SSLSBs) with high energy densities and high safety have been considered among the most promising energy storage devices to meet the demanding market requirements for electric vehicles. However, critical challenges such as lithium polysulfide shuttling effects, mismatched interfaces, Li dendrite growth, and the gap between fundamental research and practical applications still hinder the commercialization of SSLSBs. This review aims to combine the fundamental and engineering perspectives to seek rational design parameters for practical SSLSBs. The working principles, constituent components, and practical challenges of SSLSBs are reviewed. Recent progress and approaches to understand the interfacial challenges via advanced characterization techniques and density functional theory (DFT) calculations are summarized and discussed. A series of design parameters including sulfur loading, electrolyte thickness, discharge capacity, discharge voltage, and cathode sulfur content are systematically analyzed to study their influence on the gravimetric and volumetric energy densities of SSLSB pouch cells. The advantages and disadvantages of recently reported SSLSBs are discussed, and potential strategies are provided to address the shortcomings. Finally, potential future directions and prospects in SSLSB engineering are examined.

Towards high-performance solid-state Li-S batteries: from fundamental understanding to engineering design.

Application of MOFs and COFs for photocatalysis in CO2 reduction, H2 generation, and environmental treatment

The shuttling of soluble lithium polysulfides between the electrodes leads to serious capacity fading and excess use of electrolyte, which severely bottlenecks practical use of Li-S batteries. Here, selective catalysis is proposed as a fundamental remedy for the consecutive solid-liquid-solid sulfur redox reactions. The proof-of-concept Indium (In)-based catalyst targetedly decelerates the solid-liquid conversion, dissolution of elemental sulfur to polysulfides, while accelerates the liquid-solid conversion, deposition of polysulfides into insoluble Li2 S, which basically reduces accumulation of polysulfides in electrolyte, finally inhibiting the shuttle effect. The selective catalysis is revealed, experimentally and theoretically, by changes of activation energies and kinetic currents, modified reaction pathway together with the probed dynamically changing catalyst (LiInS2 catalyst), and gradual deactivation of the In-based catalyst. The In-based battery works steadily over 1000 cycles at 4.0 C and yields an initial areal capacity up to 9.4 mAh cm-2 with a sulfur loading of ≈9.0 mg cm-2 .

/pdf/selective-catalysis-remedies-polysulfide-shuttling-in-51pdwc75ce.pdf

Selective Catalysis Remedies Polysulfide Shuttling in Lithium-Sulfur Batteries.

Metal halide perovskite quantum dots, with high light-absorption coefficients and tunable electronic properties, have been widely studied as optoelectronic materials, but their applications in photocatalysis are hindered by their insufficient stability because of the oxidation and agglomeration under light, heat, and atmospheric conditions. To address this challenge, herein, we encapsulated CsPbBr3 nanocrystals into a stable iron-based metal-organic framework (MOF) with mesoporous cages (∼5.5 and 4.2 nm) via a sequential deposition route to obtain a perovskite-MOF composite material, CsPbBr3@PCN-333(Fe), in which CsPbBr3 nanocrystals were stabilized from aggregation or leaching by the confinement effect of MOF cages. The monodispersed CsPbBr3 nanocrystals (4-5 nm) within the MOF lattice were directly observed by transmission electron microscopy and corresponding mapping analysis and further confirmed by powder X-ray diffraction, infrared spectroscopy, and N2 adsorption characterizations. Density functional theory calculations further suggested a significant interfacial charge transfer from CsPbBr3 quantum dots to PCN-333(Fe), which is ideal for photocatalysis. The CsPbBr3@PCN-333(Fe) composite exhibited excellent and stable oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalytic activities in aprotic systems. Furthermore, CsPbBr3@PCN-333(Fe) composite worked as the synergistic photocathode in the photoassisted Li-O2 battery, where CsPbBr3 and PCN-333(Fe) acted as optical antennas and ORR/OER catalytic sites, respectively. The CsPbBr3@PCN-333(Fe) photocathode showed lower overpotential and better cycling stability compared to CsPbBr3 nanocrystals or PCN-333(Fe), highlighting the synergy between CsPbBr3 and PCN-333(Fe) in the composite.

Perovskite Quantum Dots Encapsulated in a Mesoporous Metal-Organic Framework as Synergistic Photocathode Materials.

Lean-electrolyte conditions are highly pursued for practical lithium (Li) metal batteries. The previous studies on the Li metal anodes, in general, exhibited good stability with a large excess of e...

Revealing Principles for Design of Lean-Electrolyte Lithium Metal Anode via In Situ Spectroscopy.

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Perovskite Quantum Dots Encapsulated in a Mesoporous Metal-Organic Framework as Synergistic Photocathode Materials.

Revealing Principles for Design of Lean-Electrolyte Lithium Metal Anode via In Situ Spectroscopy.