http://onlinelibrary.wiley.com/rss/journal/10.1002/(ISSN)1521-4095

Zinc anodes face severe instability under extreme conditions of high current density, high areal capacity, and high depth of discharge (DOD) due to severe concentration polarization caused by the imbalance between Zn2⁺ consumption and transfer rates. To overcome this, a nanofluid layer is introduced to rapidly absorb Zn2⁺ and regulate interfacial ion transport, effectively mitigating polarization and enabling stable zinc deposition. This work provides key insights into interfacial engineering for next-generation high-performance zinc metal batteries.

The commercialization of zinc metal batteries aims at high-rate capability and lightweight, which requires zinc anodes working at high current density, high areal capacity, and high depth of discharge. However, frequent zinc anode fades drastically under extreme conditions. Herein, it is revealed that the primary reason for the anode instability is the severe concentration polarization caused by the imbalanced consumption rate and transfer rate of Zn2+ under extreme conditions. Based on this finding, a nanofluid layer is constructed to rapidly absorb Zn2+ and mitigate the polarization induced by the nonlinear transport of interfacial ions. The modified zinc anode sustains at extreme conditions for over 1573 h (40 mA cm−2, 40 mAh cm−2, DOD = 75.97%) and 490 h (100 mA cm−2, 100 mAh cm−2, DOD = 90.91%), and achieving an unprecedented cumulative capacity of 62.92 Ah cm−2. This work offers both fundamental and practical insights for the interface design in energy storage devices.

This review aims to highlight the effect of electrolyte regulation on alleviating issues on the cathode side in aqueous ZIBs. The recent advances of electrolyte regulation strategies are present, with a comprehensive discussion and summary of regulation mechanisms, which can provide guidance to develop novel and multifunctional electrolytes for next-generation aqueous ZIBs.

Enhancing cathodic performance is crucial for aqueous zinc-ion batteries, with the primary focus of research efforts being the regulation of the intrinsic material structure. Electrolyte regulation is also widely used to improve full-cell performance, whose main optimization mechanisms have been extensively discussed only in regard to the metallic anode. Considering that ionic transport begins in the electrolyte, the modulation of the electrolyte must influence the cathodic performance or even the reaction mechanism. Despite its importance, the discussion of the optimization effects of electrolyte regulation on the cathode has not garnered the attention it deserves. To fill this gap and raise awareness of the importance of electrolyte regulation on cathodic reaction mechanisms, this review comprehensively combs the underlying mechanisms of the electrolyte regulation strategies and classifies the regulation mechanisms into three main categories according to their commonalities for the first time, which are ion effect, solvating effect, and interfacial modulation effect, revealing the missing puzzle piece of the mechanisms of electrolyte regulation in optimizing the cathode.

This study investigates bias-induced structural transformations in 1T-TiSe2 devices, focusing on the transition from the 1T metallic phase to the distorted 1Td phase and ultimately to an orthorhombic Ti9Se2 conducting phase. Using ex-situ and in-situ TEM, dynamic structural changes and insights into the effect of thickness on phase transitions, providing valuable information for CDW-based device applications, are revealed.

Metallic transition metal dichalcogenides (MTMDCs) are of significant attention for various electronic applications due to their anisotropic conductivity, high electron mobility, superconductivity, and charge-density-waves (CDW). Understanding the correlations between electronic properties and structural transformations is crucial. In this study, a bias-induced structural transformation in vertical CDW-based 1T-TiSe2 devices, transitioning from a 1T metallic phase to a distorted transition 1Td phase and subsequently to an orthorhombic Ti9Se2 conducting phase, is reported. Using ex-situ and in-situ biasing transmission electron microscopy, dynamic structural changes, while electron energy loss spectroscopy analysis revealed valence state modifications in Ti and Se within the Ti-rich layer after biasing, are observed. In addition, the effect of varying 1T-TiSe2 thickness on the maximum current value is investigated. These observations reveal that increased thickness requires higher voltage to induce phase transitions. These insights contribute to understanding the structural and electronic dynamics of 1T-TiSe2, highlighting its potential as a promising material for future CDW-based device applications.

Ultra-small silver nanoparticles are formed in situ and activated in an amidoxime-modified polymer of intrinsic microporosity to fabricate a metallic nanocomposite membrane for C2H4/C2H6 separation. The activated silver nanoparticles promote C2H4 transport and effectively enhance C2H4/C2H6 separation selectivity, resulting in an outstanding membrane separation performance with C2H4 permeability of 322.1 barrer and C2H4/C2H6 selectivity as high as 8.8.

The separation of C2H4 and C2H6 is a critical yet energy-intensive operation in the petrochemical industry. Gas separation membranes offer energy-efficient alternatives, but their effectiveness is hindered by the similar physical properties of C2H4 and C2H6. Here, a metallic nanocomposite membrane (MNM) comprising ultra-small Ag nanoparticles embedded in an amidoxime-modified polymer of intrinsic microporosity (AOPIM-1) is reported for highly efficient C2H4/C2H6 separation. The microporous structure of AOPIM-1, combined with anchoring groups (amidoxime groups) inside the microcavities, enables size-controlled growth of Ag nanoparticles with ‒≈3 nm diameter, which maximizes the contact with ethylene molecules. The amidoxime groups as electron acceptors effectively enrich the positive charge on the surface of Ag nanoparticles. The activated Ag form reversible complexes with ethylene molecules endowing them with preferential affinity over ethane. The resulting Ag nanocomposite membrane demonstrates a ≈10-fold increase in C2H4 permeability, reaching 322.1 barrer, and a ≈3-fold increase in C2H4/C2H6 selectivity, reaching 8.8. The comprehensive separation performance is superior over all the polymer membranes and mixed matrix membranes reported so far. The MNMs also demonstrate stable mixed gas separation performance under elevated feed gas pressures. This study provides valuable insights into designing and fabricating polymer membranes with high C2H4/C2H6 separation performance.

A Co single-atom catalyst (Co-N₄) enhances Cl₂ adsorption and lowers LiCl reaction barriers in Li-Cl₂ batteries. The Li-Cl₂@Co-NC battery exhibits >600 cycles at 1500 mA g⁻¹ at room temperature and 650 cycles at 500 mA g⁻¹ at −40 °C, with a 0.6 V reduction in polarization voltage. This strategy delivers high-performance Li-Cl₂ batteries with wide temperature adaptability.

Lithium-chlorine (Li-Cl2) secondary batteries are emerging as promising candidates for high-energy-density power sources and an extensive operational temperature range. However, conventional electrode materials suffer from weak adsorption for chlorine gas (Cl2) and low conversion efficiency of lithium chloride (LiCl), leading to significant loss of chlorine-based active materials. This issue hampers the cyclability of Li-Cl2 batteries. In this work, it is demonstrated that synergistic Cl2 adsorption on the electrode surface and the energy barrier for LiCl reactions are crucial for enhancing Cl2/LiCl conversion efficiency. Consequently, a cobalt (Co) single-atom site catalyst with a Co-N4 coordination environment has been developed, which significantly diminishes the transformation barrier of solid LiCl particles into Cl2 and concurrently enhances the chemical adsorption of Cl2, facilitating uniform nucleation of LiCl. As a result, the Li-Cl2@Co-NC battery developed has achieved a 0.6 V reduction in polarization voltage under high current densities, effectively addressing the issue of low conversion efficiency between Cl2 and LiCl. At room temperature, the Li-Cl2@Co-NC battery achieves over 600 cycles at 1500 mA g−1; At −40 °C, it reaches 650 cycles at 500 mA g−1. The research overcomes the cycle stability barrier in high-current Li-Cl2 batteries and offers a strategy for batteries with a wide temperature range and long cycle life.