In response to the call for safer high‐energy‐density storage systems, high‐voltage solid‐state Li metal batteries have attracted extensive attention. Therefore, solid electrolytes are required to be ...stable against both Li anode and high‐voltage cathodes; nevertheless, the requirements still cannot be completely satisfied. Herein, a heterogeneous multilayered solid electrolyte (HMSE) is proposed to broaden electrochemical window of solid electrolytes to 0–5 V, through different electrode/electrolyte interfaces to overcome the interfacial instability problems. Oxidation‐resistance poly(acrylonitrile) (PAN) is in contact with the cathode, while reduction tolerant polyethylene glycol diacrylate contacts with Li metal anode. A Janus and flexible PAN@Li1.4Al0.4Ge1.6(PO4)3 (80 wt%) composite electrolyte is designed as intermediate layer to inhibit dendrite penetration and ensure compact interface. Paired with LiNi0.6Co0.2Mn0.2O2 and LiNi0.8Co0.1Mn0.1O2 cathodes, which are rarely used in solid‐state batteries, the solid‐state Li metal batteries with HMSE exhibit excellent electrochemical performance including high capacity and long cycle life. Besides, the Li||Li symmetric batteries maintain a stable polarization less than 40 mV for more than 1000 h under 2 mA cm−2 and effective inhibition of dendrite formation. This study offers a promising approach to extend the applications of solid electrolytes for high‐voltage solid‐state Li metal batteries.
A heterogeneous multilayered structure that expands the electrochemical window of solid electrolytes is designed. The oxidation‐resistant poly(acrylonitrile) (PAN) and reduction‐tolerant polyethylene glycol diacrylate integrated with the Janus and flexible PAN@Li1.4Al0.4Ge1.6(PO4)3 (80 wt%) composite electrolyte broaden the electrochemical window to 0–5 V, resulting in excellent performance for high‐voltage solid‐state Li‐metal batteries. Additionally, the thickness of electrolyte is below 25 μm.
Methodology development of robust linkages is fundamentally important for the synthesis and application of covalent organic frameworks (COFs). We report herein a new strategy based on multicomponent ...reactions (MCRs) to construct ultrastable COFs. With the one-pot formation of five covalent bonds in each cyclic joint, a series of imidazole-linked COFs were robustly constructed through the Debus–Radziszewski MCR from three easily available components. By reaching a higher level of complexity and precision in covalent assembly, this research explores a new direction in integrating sophisticated reversible/irreversible reactions to construct crystalline porous frameworks.
Assembly of single layers: Three‐dimensional assembly of single‐layered MoS2 is achieved on a large scale via a solution method. The as‐prepared tubular architectures have tunable size and mesopores ...in the shell, which are desirable for applications. As a example, they exhibit excellent lithium storage properties and are highly active for hydrodesulfurization of thiophene resulting from their structural advantages.
Chirality introduces a new dimension of functionality to materials, unlocking new possibilities across various fields. When integrated with plasmonic hybrid nanostructures, this attribute synergizes ...with plasmonic and other functionalities, resulting in unprecedented chiroptical materials that push the boundaries of the system's capabilities. Recent advancements have illuminated the remarkable chiral light–matter interactions within chiral plasmonic hybrid nanomaterials, allowing for the harnessing of their tunable optical activity and hybrid components. These advancements have led to applications in areas such as chiral sensing, catalysis, and spin optics. Despite these promising developments, there remains a need for a comprehensive synthesis of the current state‐of‐the‐art knowledge, as well as a thorough understanding of the construction techniques and practical applications in this field. This review begins with an exploration of the origins of plasmonic chirality and an overview of the latest advancements in the synthesis of chiral plasmonic hybrid nanostructures. Furthermore, representative emerging categories of hybrid nanomaterials are classified and summarized, elucidating their versatile applications. Finally, the review engages with the fundamental challenges associated with chiral plasmonic hybrid nanostructures and offer insights into the future prospects of this advanced field.
Emerging chiral plasmonic hybrid nanostructures that integrate chirality, plamonics, and rich functionalities into single entities are introduced in this review. A comprehensive overview of recent advancements is provided, including the origins of chirality, rationale design and construction techniques, and versatile applications. Additionally, current challenges and future prospects in this field are discussed in detail.
Herein, a novel dual single‐atom catalyst comprising adjacent Fe‐N4 and Mn‐N4 sites on 2D ultrathin N‐doped carbon nanosheets with porous structure (FeMn‐DSAC) was constructed as the cathode for a ...flexible low‐temperature Zn‐air battery (ZAB). FeMn‐DSAC exhibits remarkable bifunctional activities for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Control experiments and density functional theory calculations reveal that the catalytic activity arises from the cooperative effect of the Fe/Mn dual‐sites aiding *OOH dissociation as well as the porous 2D nanosheet structure promoting active sits exposure and mass transfer during the reaction process. The excellent bifunctional activity of FeMn‐DSAC enables the ZAB to operate efficiently at ultra‐low temperature of −40 °C, delivering 30 mW cm−2 peak power density and retaining up to 86 % specific capacity from the room temperature counterpart.
A Fe/Mn dual single‐atom catalyst with an excellent bifunctional activity is prepared as the cathode for a flexible low‐temperature Zn‐air battery (ZAB). Profiting from the combined Fe/Mn dual‐site effect as well as the porous 2D nanosheet structure, the ZAB could operate efficiently at the ultra‐low temperature of −40 °C.
Abstract
How does campaign-style law enforcement sustain authoritarian rule? Drawing on fieldwork data and published materials, this article enhances the understanding of law and politics in ...authoritarian regimes by investigating the role of the ‘sweep away black' campaign—designed to combat organized and gang crime—in strengthening China's authoritarian regime. It argues that the campaign helps the party-state enhance its authoritarian rule by resolving the legitimacy crisis caused by economic slowdown, gangs' infiltration in grassroots political structures and problems of police corruption and shirking. But the campaign distorts the criminal justice system by demanding that criminal justice organs deliver severe and swift justice. It also harms China's private sector because local governments may expand the targets of repression to include private enterprises.
Single‐crystalline cathode materials have attracted intensive interest in offering greater capacity retention than their polycrystalline counterparts by reducing material surfaces and phase ...boundaries. However, the single‐crystalline LiCoO2 suffers severe structural instability and capacity fading when charged to high voltages (4.6 V) due to Co element dissolution and O loss, crack formation, and subsequent electrolyte penetration. Herein, by forming a robust cathode electrolyte interphase (CEI) in an all‐fluorinated electrolyte, reversible planar gliding along the (003) plane in a single‐crystalline LiCoO2 cathode is protected due to the prevention of element dissolution and electrolyte penetration. The robust CEI effectively controls the performance fading issue of the single‐crystalline cathode at a high operating voltage of 4.6 V, providing new insights for improved electrolyte design of high‐energy‐density battery cathode materials.
Single‐crystalline cathode materials have attracted intensive interest. However, the single‐crystalline LiCoO2 suffers severe structural instability and capacity fading when charged to high voltages (4.6 V vs Li/Li+) due to Co and O element dissolution, crack formation, and electrolyte penetration. In this work, the above problems are inhibited by forming a robust cathode electrolyte interphase (CEI) on the surface of LiCoO2.
Development of new chemistry to simultaneously meet the demands for topology, connectivity, and functionality is highly desired in the research area of covalent organic frameworks (COFs). We explore ...herein the isocyanide chemistry so as to establish a facile paradigm to integrate functionality and ultrastability in COFs. Using the representative Groebke–Blackburn–Bienaymé (GBB) reaction based on isocyanide chemistry, we are able to construct a series of pyrimidazole-based COFs in one step from isocyanide, aminopyridine, and aldehyde monomers. Diversified functionalities have been bottom-up integrated by the simple replacement of readily available 2-aminopyridine monomers. Meanwhile, the ubiquitous formation of fused imidazole rings within the frameworks has guaranteed their ultrastability. In view of the rich synthetic possibilities provided by isocyanide chemistry, we expect that this contribution opens up a new avenue toward the divergent construction of robust COFs for practical applications.
The increasing demand for replacing conventional fossil fuels with clean energy or economical and sustainable energy storage drives better battery research today. Sodium‐ion batteries (SIBs) are ...considered as a promising alternative for grid‐scale storage applications due to their similar “rocking‐chair” sodium storage mechanism to lithium‐ion batteries, the natural abundance, and the low cost of Na resources. Searching for appropriate electrode materials with acceptable electrochemical performance is the key point for development of SIBs. Layered transition metal oxides represent one of the most fascinating electrode materials owing to their superior specific capacity, environmental benignity, and facile synthesis. However, three major challenges (irreversible phase transition, storage instability, and insufficient battery performance) are known for cathodes in SIBs. Herein, a comprehensive review on the latest advances and progresses in the exploration of layered oxides for SIBs is presented, and a detailed and deep understanding of the relationship of phase transition, air stability, and electrochemical performance in layered oxide cathodes is provided in terms of refining the structure–function–property relationship to design improved battery materials. Layered oxides will be a competitive and attractive choice as cathodes for SIBs in next‐generation energy storage devices.
The recent progress in layered oxide cathodes for sodium‐ion batteries is comprehensively reviewed. Some new perspectives concentrating on phase transition, air stability, and electrochemical performance in layered cathodes are provided, in terms of refining the structure–function–property relationship to rationally design better electrode materials.
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