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The practical applications of aqueous Zn/I2 batteries (AZIBs) operating within a wide temperature range are severely hindered by the uncontrolled shutting of polyiodide ions (I3−/ I5−) and rampant side reactions. In this study, a wide temperature tolerant polyanionic hydrogel (borax‐bacteria cellulose / p(AMPS‐AM)) with ion selective permeability is designed for inhibiting shutting effect and side reactions under extreme temperatures range from −50 to 50 °C. The zincophilic R−SO3− significantly enhances the transport of Zn2+ cations and promotes uniform growth of Zn metal along the (002) plane. Moreover, the abundant hydrophilic groups in hydrogels effectively suppress both the hydrogen evolution reaction and the formation of by‐products by reducing the water reactivity. Furthermore, theoretical calculations, visualization experiment and in situ Raman spectroscopy confirm that R−SO3− group effectively hinders the shuttle process of I3−/I5− anions through electrostatic repulsion. Consequently, this gel electrolyte facilitates the ultra‐stable Zn/I2 full cell at a low current density of 2 C over a wide temperature range of 100 °C. A Zn/I2 pouch cell with a low negative/positive capacity ratio of 3.3 exhibits a stable performance over 350 cycles with an impressive high‐areal capacity of 2.03 mA h cm−2, thereby establishing a solid foundation for its practical applications. [ABSTRACT FROM AUTHOR]

Sodium‐ion batteries (SIBs) with wide operating temperature are regarded as promising candidates for large‐scale energy storage systems. However, SIBs operating under elevated temperature aggravate the electrolyte decomposition with unstable cathode‐electrolyte interphase (CEI), causing a rapid capacity degradation. Herein, anion receptor tris(pentafluorophenyl)borane (TPFPB) is selected as electrolyte additive to construct robust NaF‐rich CEI. The strong interactions between anion and TPFPB via the electron‐deficient boron atoms weaken ClO4− solvation and promote the coordination capability between solvents and Na+ cations, demonstrating greatly improved oxidative stability. Na3V2(PO4)3 cathode in TPFPB‐containing electrolyte delivers long‐term stability with a capacity retention of 86.9% after 100 cycles at a high cut‐off voltage of 4.2 V (vs. Na+/Na) and a high temperature of 60 °C. Besides, TPFPB also works well with enhanced performance over a temperature range from −30 to 60 °C. This study proposes a prospective method by manipulating the solvation chemistry for constructing high‐temperature rechargeable SIBs. [ABSTRACT FROM AUTHOR]

Carbon with few active sites and narrow interlayer distance as anode for potassium ion batteries (PIBs) always shows low capacity, sluggish kinetics, and low Columbic efficiency. Herein, poly(2‐aminothiazole) (P2AT) hollow nanospheres are first synthesized as a carbon source for high N, S co‐doped carbon hollow nanospheres (NS‐HCSs). The hollow P2AT nanospheres can be controllably synthesized with an Ostwald ripening process. The unique doping and structure endow the NS‐HCSs with high content of N and S dopants in carbon, mesoporous structure with enlarged interlayer distance, elevated ratio of N‐6 and N‐5 species, enhanced conductivity, abundant surface defects, and large active sites. When evaluated as an anode for PIBs, NS‐HCSs exhibit a high reversible capacity of 422 mAh g‒1 and excellent long‐term cycling performance. Using combined experiment and theoretical computation, including in situ TEM and in situ Raman, the K‐storage mechanism and dynamic evolution processes of NS‐HCSs, including low volume expansion, enhanced K‐ion adsorption, and stable composition and structure evolution during repeating potassiation/de‐potassiation processes is revealed. This quantitative design for highly durable K‐storage and large capacity in carbon can be advantageous for the rational design of anode materials of PIBs with ideal electrochemical performance. [ABSTRACT FROM AUTHOR]

Aqueous zinc ion batteries (AZIBs) with high safety, low cost, and eco‐friendliness advantages show great potential in large‐scale energy storage systems. However, their practical application is hindered by low Columbic efficiency and unstable zinc anode resulting from the side reactions and deterioration of zinc dendrites. Herein, tripropylene glycol (TG) is chosen as a dual‐functional organic electrolyte additive to improve the reversibility of AZIBs significantly. Importantly, ab initio molecular dynamics theoretical simulations and experiments such as in situ electrochemical impedance spectroscopy, and synchrotron radiation‐based in situ Fourier transform infrared spectroscopy confirm that TG participates in the solvation sheath of Zn2+, regulating overpotential and inhibiting side reactions; meanwhile, TG inhibits the deterioration of dendrites and modifies the direction of zinc deposition by constructing an adsorbed layer on the zinc anode. Consequently, a Zn‐MnO2 full cell with TG electrolyte exhibited a specific capacity of 124.48 mAh g‐1 after 1000 cycles at a current density of 4 A g‐1. This quantitative regulation for suitable solvation sheath and adsorbed layer on zinc anode, and its easy scalability of the process can be of immediate benefit for the dendrite‐free, high‐performance, and low‐cost energy storage systems. [ABSTRACT FROM AUTHOR]

The practicality of aqueous zinc ion batteries (AZIBs) for large‐scale energy storage is hindered by challenges associated with zinc anodes. In this study, a low‐cost and multi‐function electrolyte additive, cetyltrimethyl ammonium bromide (CTAB), is presented to address these issues. CTAB adsorbs onto the zinc anode surface, regulating Zn2+ deposition orientation and inhibiting dendrite formation. It also modifies the solvation structure of Zn2+ to reduce water reactivity and minimize side reactions. Additionally, CTAB optimizes key physicochemical parameters of the electrolyte, enhancing the stability of the electrode/electrolyte interface and promoting reversibility in AZIBs. Theoretical simulations combined with operando synchrotron radiation‐based in situ Fourier transform infrared spectra and in situ electrochemical impedance spectra further confirm the modified Zn2+ coordination environment and the adsorption effect of CTAB cations at the anode/electrolyte interface. As a result, the assembled Zn‐MnO2 battery demonstrates a remarkable specific capacity of 126.56 mAh g−1 at a high current density of 4 A g−1 after 1000 cycles. This work highlights the potential of CTAB as a promising solution for improving the performance and practicality of AZIBs for large‐scale energy storage applications. [ABSTRACT FROM AUTHOR]

The reversibility and long‐term cycling stability of aqueous zinc‐ion batteries (AZIBs) in a wide temperature range have rarely been explored. Herein, diethylene glycol monoethyl ether (DG) is introduced as an electrolyte additive to enhance Zn performance within a wide temperature range of −35 to 65 °C. Operando synchrotron Fourier transform infrared spectroscopy analysis combined with molecular dynamics simulations reveal that the introduction of DG disrupts the initial hydrogen bonding network of the aqueous electrolyte, restructuring the solvation structure surrounding Zn2+ ions and mitigating water‐induced parasitic reactions. Adding DG reduces the freezing point of the aqueous electrolyte without compromising its incombustibility. Moreover, operando electrochemical quartz crystal microbalance with dissipation monitoring (EQCM‐D) and X‐ray photoelectron spectroscopy demonstrated that the coordinated DG and OTF− undergo reductive decomposition, forming a self‐healing solid electrolyte interphase comprising an inorganic/organic ZnF2‐ZnS, which can effectively suppress the notorious side reactions and guide the uniform Zn deposition. Consequently, the symmetric Zn/Zn cells demonstrate excellent cycling stability for 3500 h under 1 mA cm−2 at 25 °C, and for 1000 h under 1 mA cm−2 at both −35 and 65 °C. Full batteries with a DG‐containing electrolyte exhibit a long lifespan of 5000 cycles at 2 A g−1. [ABSTRACT FROM AUTHOR]

Assembling molecular proton carriers into crosslinked networks is widely used to fabricate proton conductors, but they often suffer losses in conduction efficiency and stability accompanied by unclear causes. Covalent organic frameworks (COFs), with well‐defined crystal frameworks and excellent stability, offer a platform for exploring the proton transfer process. Herein, a strategy to construct proton conductors that induce conductivity and stability by introducing bottom‐up hierarchical structure, mass transport interfaces, and host–guest interactions into the COFs is proposed. The proton‐transport platforms are designed to possess hierarchically macro–microporous structure for proton storage and mass transport. The protic ionic liquids, with low proton dissociation energies investigated by DFT calculation, are installed at open channel walls for faster proton motion. As expected, the resultant proton conductors based on a covalent organic framework (PIL0.5@m‐TpPa‐SO3H) with hierarchical pores increase conductivity by approximately three orders of magnitude, achieving the value of 1.02 × 10−1 S cm−1 (90 °C, 100% RH), and maintain excellent stability. In addition, molecular dynamics simulations reveal the mechanism of "hydrogen‐bond network" for proton conduction. This work offers a fresh perspective on COF‐based material manufacturing for high‐performance proton conductors via a protocol of macro‐micropores. [ABSTRACT FROM AUTHOR]

Potassium‐ion batteries hold practical potential for large‐scale energy storage owing to their appealing cell voltage and cost‐effective features. The development of anode materials with high rate capability and satisfactory cycle lifespan, however, is one of the key elements for exploiting this electrochemical energy storage system at practical levels. Here, a template‐assisted strategy is reported for acquiring a bimetallic telluride heterostructure which is supported on N‐doped carbon shell (ZnTe/CoTe2@NC) that promotes diffusion of K+ ions for rapid charge transfer. It is shown that in telluride heterojunctions, electron‐rich Te sites and built‐in electric fields contributed by electron transfer from ZnTe to CoTe2 concomitantly provide abundant cation adsorption sites and facilitate interfacial electron transport during potassiation/depotassiation. The relatively fine ZnTe/CoTe2 nanoparticles imparted by the heterojunction result in high structural stability, together with a highly reversible capacity up to 5000 cycles at 5 A g−1. Moreover, using judiciously combined experiment and theoretical computation, it is demonstrated that the energy barrier for K+ diffusion in telluride heterojunctions is significantly lower than that in individual counterparts. This quantitative design for fast and durable charge transfer in telluride heterostructures can be of immediate benefit for the rational design of batteries for low‐cost energy storage and conversion. [ABSTRACT FROM AUTHOR]

The development of effective, stable anhydrous proton‐conductive materials is vital but challenging. Covalent organic frameworks (COFs) are promising platforms for ion and molecule conduction owing to their pre‐designable structures and tailor‐made functionalities. However, their poor chemical stability is due to weak interlayer interactions and intrinsic reversibility of linkages. Herein, we present a strategy for enhancing the interlayer interactions of two‐dimensional COFs via importing planar, rigid triazine units into the center of C3‐symmetric monomers. The developed triazine‐core‐based COF (denoted as TPT‐COF) possesses a well‐defined crystalline structure, ordered nanochannels, and prominent porosity. The proton conductivity was ≈10 times those of non‐triazinyl COFs, even reaching up to 1.27×10−2 S cm−1 at 160 °C. Furthermore, the TPT‐COF exhibited structural ultrastability, making it an effective proton transport platform with remarkable conductivity and long‐term durability. [ABSTRACT FROM AUTHOR]

Pt‐based nanomaterials are now the most reliable catalysts for oxygen reduction reaction (ORR). However, the low atomic utilization efficiency and poor stability severely limit their widespread application. Herein, a facile molten salt approach for synthesizing N‐doped porous carbon embedded with Pt3Fe intermetallic nanoparticles is presented. The Pt loading of the as‐prepared materials is as low at 5.91 wt. %, while exhibiting a half‐wave potential of 0.85 V and diffusion limiting current density of −5.68 mA cm−2 in alkaline condition, which is superior to commercial Pt/C (0.83 V, −5.48 mA cm−2). As cathode for Zn‐air battery, the power density and specific capacity up to 130.0 mW cm−2 and 833 mAh g−1, respectively, are outperforming Pt/C batteries (85.8 mW cm−2, 632 mAh g−1). The theoretical calculations identify the origin of activity on Pt3Fe; the Pt3Fe (111) plane exhibits more positive activity than (200) plane. [ABSTRACT FROM AUTHOR]

Several types of electrode materials have been developed for high–performance supercapacitors. Most of the relevant studies have focused on the discovery of new atomic structures and paid limited attention to the effect of heterostructures in supercapacitor electrodes, which has long hindered the fundamental understanding of the use of hybrid materials in supercapacitors. In this study, a novel heterostructure based on perovskite oxide (LaNiO3) nanosheets and polyazulene was synthesized. The as–prepared heterostructure–based supercapacitor exhibited a specific capacitance of up to 464 F g−1 at a high current density of 2 A g−1 in 1–ethyl–3–methylimidazolium tetrafluoroborate. In a symmetric supercapacitor, this heterostructure delivered an energy density of up to 56.4 Wh kg−1 at a power density of 1100 W kg−1. Both LaNiO3 and polyazulene contributed pseudocapacitance and dominated the performance. Unexpectedly, electric double–layer capacitance was found to contribute in this system. Density functional theory calculations indicated that the advantage of the high electrical conductivity of the heterostructure benefited the supercapacitor operation. Electrochemical quartz crystal microbalance analysis revealed that the fast ion flux and adsorption boosted performance. The high intrinsic electrical conductivity and improved stability make this heterostructure a promising electrode material candidate for supercapacitors. [ABSTRACT FROM AUTHOR]

Hierarchical hybrid heteroarchitectures possess attractive structural/compositional merits for lithium‐ion batteries (LIBs). Herein, a facile yet in situ growth strategy is proposed to scalably synthesize hierarchical porous ZnO/ZnFe2O4 hybrid nanofibers (NFs) with robust core/shell heterostructure toward LIBs. In such hybrids, 2D ZnFe2O4 nanosheets (NSs) are uniformly decorated on single‐crystalline ZnO core NFs, thereby affording more exposed active sites, a fast ion diffusion kinetic, and structural stability of electrodes during repeated cycling. As a result, benefiting from the unique hierarchical porous core/shell architecture and synergistic effects between the stable substrate of ZnO NFs and high‐capacity promoter of ZnFe2O4 NSs, the optimized ZnO/ZnFe2O4 hybrid as an anode for LIBs delivers a large reversible capacity of ≈688 mAh g−1 at 0.1 A g−1, high rate capability (≈288 mAh g−1 at 2.0 A g−1), and remarkable cyclability (≈491 mAh g−1 even over 250 cycles at 0.5 A g−1) for efficient lithium storage. This work highlights the rational design of a hierarchical architecture with a stable substrate and high‐capacity phases for next‐generation energy storage applications. [ABSTRACT FROM AUTHOR]

Among the various semiconductor materials, zinc telluride possesses the lowest electron affinity and ultrafast charge separation capability, facilitating improved charge transfer kinetics. In addition, ZnTe has a relatively high density, contributing to high volumetric capacity. Here, 1D N‐doped carbon‐coated ZnTe core‐shell nanowires (ZnTe@C) are designed and prepared via a facile ion‐exchange and carbonization technique. When evaluated as anode for metal ion batteries, it demonstrates superior electrochemical performance in both Li and Na ion storage, including high gravimetric and volumetric capacities (1119 mA h g−1 and 906 mA h cm−3, respectively, at 100 mA g−1 for Li ion storage), excellent high‐rate capability, and long‐term cycling stability. This remarkable electrochemical performance is attributed to the low electron affinity and high density of ZnTe, and the amorphous nature of the N‐doped carbon layer in the heterostructured ZnTe@C nanowires, which not only provide fast charge transfer paths, but also effectively maintain the structural and electrical integrity of the ZnTe. The strategy of embedding high density and high‐performance active materials in highly conductive nanostructures represents an effective way of achieving electrode materials with excellent gravimetric and volumetric capacities towards superior energy storage systems. [ABSTRACT FROM AUTHOR]

A group of newly reported antiperovskite nitrides CuxIn1−xNNi3 (0≤x≤1) with tunable composition are employed as electrocatalysts for the hydrogen evolution reaction (HER). Cu0.4In0.6NNi3 shows the highest intrinsic performance among all developed catalysts with an overpotential of merely 42 mV at 10 mA cmgeo−2. Stability tests at a high current density of 100 mA cmgeo−2 show its super‐stable performance with only 7 mV increase in overpotential after more than 60 hours of measurement, surpassing commercial Pt/C (increase of 170 mV). By partial substitution, the derived antiperovskite nitride achieves a smaller kinetic barrier of water dissociation compared to the unsubstituted InNNi3 and CuNNi3, revealed by first‐principle calculations. It is found that the partially substituted CuxIn1−xNNi3 possesses a thermal neutral and desirable Gibbs free energy of hydrogen for HER, ascribed to the tailoring of the energy of d‐band center arose by the A‐site (A=Cu or In) substitution and a resulting optimization of adsorbate interactions. [ABSTRACT FROM AUTHOR]

Supercapacitors (SCs) with high power output have attracted increasing attention as efficient and environmentally friendly energy storage devices. Prussian blue and its analogues (PB/PBAs) are simple coordination polymers with tunable chemical compositions and open framework. Prussian blue can act as electrode materials in its pristine form and has also been utilized to derive various metallic nanostructures for electrochemical applications due to their simple fabrication process, non‐toxic characteristics, and low price. Here, we firstly describe the charge storage mechanisms of SCs briefly followed by an introduction of the fabrication methods of PB/PBAs and their derivatives. Then, a comprehensive review on recent studies of the use of PB/PBAs and their derivatives as the electrode materials for SCs are given with a focus on strategies to improve their electrochemical performances. Finally, we discuss critical challenges in this research area and propose some general ideas for future research. [ABSTRACT FROM AUTHOR]

The cost‐efficient ZnMnO3 has attracted increasing attention as a prospective anode candidate for advanced lithium‐ion batteries (LIBs) owing to its resourceful abundance, large lithium storage capacity and low operating voltage. However, its practical application is still seriously limited by the modest cycling and rate performances. Herein, a facile design to scalable synthesize unique one‐dimensional (1D) mesoporous ZnMnO3 nanorods (ZMO‐NRs) composed of nanoscale particles (≈11 nm) is reported. The 1D mesoporous structure and nanoscale building blocks of the ZMO‐NRs effectively promote the transport of ions/electrons, accommodate severe volume changes, and expose more active sites for lithium storage. Benefiting from these appealing structural merits, the obtained ZMO‐NRs anode exhibits excellent rate behavior (≈454 mAh g−1 at 2 A g−1) and ultra‐long term cyclic performance (≈949.7 mAh g−1 even over 500 cycles at 0.5 A g−1) for efficient lithium storage. Additionally, the LiNi0.8Co0.1Mn0.1O2//ZMO‐NRs full cell presents a practical energy density (≈192.2 Wh kg−1) and impressive cyclability with approximately 91 % capacity retention over 110 cycles. This highlights that the ZMO‐NRs product is a highly promising high‐rate and stable electrode candidate towards advanced LIBs in electronic devices and sustainable energy storage applications. [ABSTRACT FROM AUTHOR]

To optimize the cycle life and rate performance of lithium‐ion batteries (LIBs), ultra‐fine Fe2O3 nanowires with a diameter of approximately 2 nm uniformly anchored on a cross‐linked graphene ribbon network are fabricated. The unique three‐dimensional structure can effectively improve the electrical conductivity and facilitate ion diffusion, especially cross‐plane diffusion. Moreover, Fe2O3 nanowires on graphene ribbons (Fe2O3/GR) are easily accessible for lithium ions compared with the traditional graphene sheets (Fe2O3/GS). In addition, the well‐developed elastic network can not only undergo the drastic volume expansion during repetitive cycling, but also protect the bulk electrode from further pulverization. As a result, the Fe2O3/GR hybrid exhibits high rate and long cycle life Li storage performance (632 mAh g−1 at 5 A g−1, and 471 mAh g−1 capacity maintained even after 3000 cycles). Especially at high mass loading (≈4 mg cm−2), the Fe2O3/GR can still deliver higher reversible capacity (223 mAh g−1 even at 2 A g−1) compared with the Fe2O3/GS (37 mAh g−1) for LIBs. Winning ribbon: Graphene ribbon networks can effectively improve electron/ion transfer to enhance the battery performance of hybrids, especially at high mass loading. Ultra‐fine Fe2O3 nanowires uniformly anchored on interconnected graphene ribbon networks are successfully synthesized, and exhibit high rate and long cycle life performance. [ABSTRACT FROM AUTHOR]

We have purposefully developed a smart template-engaged methodology to efficiently fabricate well-defined ternary spinel ZnMn2O4 hollow nanotubes (NTs). The procedure involves coating carbon nanotubes (CNTs) with ZnMn2O4 nanosheets (NSs), followed by heating at high temperature in air to oxidize the CNT template. Physicochemical characterization demonstrated that the formed ZnMn2O4 NTs with a diameter of approximately 100 nm were composed of assembled NSs and/or nanoparticles (NPs) as building blocks and possessed numerous nanopores of several nanometers in the sidewall of the NTs. In favor of the intrinsic structural advantages, the resulting ZnMn2O4 NTs exhibited superior electrochemical lithium-storage performance with a large capacity, good rate behavior, and excellent cyclability when evaluated as promising anodes for lithium-ion batteries (LIBs). The remarkable electrochemical performance was rationally ascribed to the appealing one-dimensional (1D) porous hollow tubular architecture with nanoscale subunits and mesopores in the sidewalls, which decreased the diffusion length for the Li+ ions, improved the kinetic process, and enhanced the structural integrity with sufficient void space to tolerate the volume variation during Li+-ion insertion/extraction. These results highlight the promising application of 1D ZnMn2O4 NTs as anodes for high-performance LIBs. [ABSTRACT FROM AUTHOR]

In the work, a facile yet efficient self-sacrifice strategy is smartly developed to scalably fabricate hierarchical mesoporous bi-component-active ZnO/ZnFe2O4 (ZZFO) sub-microcubes (SMCs) by calcination of single-resource Prussian blue analogue of Zn3[Fe(CN)6]2 cubes. The hybrid ZZFO SCMs are homogeneously constructed from well-dispersed nanocrstalline ZnO and ZnFe2O4 (ZFO) subunites at the nanoscale. After selectively etching of ZnO nanodomains from the hybrid, porously assembled ZFO SMCs with integrate architecture are obtained accordingly. When evaluated as anodes for LIBs, both hybrid ZZFO and ZFO samples exhibit appealing electrochemical performance. However, the as-synthesized ZZFO SMCs demonstrate even better electrochemical Li-storage performance, including even larger initial discharge capacity and reversible capacity, higher rate behavior and better cycling performance, particularly at high rates, compared with the single ZFO, which should be attributed to its unique microstructure characteristics and striking synergistic effect between the bi-component-active, well-dispersed ZnO and ZFO nanophases. Of great significance, light is shed upon the insights into the correlation between the electrochemical Li-storage property and the structure/component of the hybrid ZZFO SMCs, thus, it is strongly envisioned that the elegant design concept of the hybrid holds great promise for the efficient synthesis of advanced yet low-cost anodes for next-generation rechargeable Li-ion batteries. [ABSTRACT FROM AUTHOR]

In this work, we put forward a facile yet efficient room-temperature synthetic methodology for the smart fabrication of mesoporous nanocrystalline ZnMn2O4 in macro-quality from the birnessite-type MnO2 phase. A plausible reduction/ion exchange/re-crystallization mechanism is tentatively proposed herein for the scalable synthesis of the spinel phase ZnMn2O4. When utilized as a high-performance anode for advanced Li-ion battery (LIB) application, the as-synthesized nanocrystalline ZnMn2O4 delivered an excellent discharge capacity of approximately 1288 mAh g−1 on the first cycle at a current density of 400 mA g−1, and exhibited an outstanding cycling durability, rate capability, and coulombic efficiency, benefiting from its mesoporous and nanoscale structure, which strongly highlighted its great potential in next-generation LIBs. Furthermore, the strategy developed here is very simple and of great importance for large-scale industrial production. [ABSTRACT FROM AUTHOR]

One-dimensional (1D) mesoporous ternary Co-Ni-Mn oxide nanowires (CNMO NWs) have been controllably fabricated via a facile yet scalable template-free strategy involving a green hydrothermal route coupled with the following calcination. The composition of the reaction solvent system, i.e., the volume ratio of the ethylene glycol and deionized water, plays a significant role in tuning the specific morphologies and microstructures of the final CNMO products. The as-derived lD CNMO NWs are constructed with numerous nanoparticle subunits with the size of ≈5-10 nm, and possess lots of interparticle mesopores ranged from 2 to 6 nm. The well-defined mesoporous CNMO NWs apparently have appealing structural advantages, such as fast and convenient electron and ion transport, sufficient redox electrochemical centers with multiple valences, and large electroactive surface area. As a result, the as-fabricated mesoporous CNMO NWs manifest exceptional pesudocapacitance and excellent cycling stability at high rates when evaluated as a striking low-cost electrode for next-generation electrochemical capacitors. [ABSTRACT FROM AUTHOR]

In this work, we rationally designed an efficient template-free synthetic strategy to fabricate hierarchical mesoporous hollow ZnMn2O4 sub-microspheres (HZSMs) constructed entirely from nanoparticle (NP) building blocks of size ≈15 nm. The well-known inside-out Ostwald ripening process was tentatively proposed to shed light on the formation mechanism of the mesoporous hollow nano-/microarchitecture. In favor of the intrinsic structural advantages, these resulting HZSMs exhibited superior electrochemical lithium-storage performance with high specific capacity, excellent cyclability, and good rate capability when evaluated as an anode material for advanced Li-ion batteries (LIBs). The excellent electrochemical performance should be reasonably ascribed to the porous and hollow structure of the unique HZSMs with nanoscale subunits, which reduced the diffusion length for Li+ ions, improved the kinetic process and enhanced the structural integrity with sufficient void space for tolerating the volume variation during the Li+ insertion/extraction. These results further revealed that the as-prepared mesoporous HZSMs would be a promising anode for high-performance LIBs. [ABSTRACT FROM AUTHOR]

Small molecule organic materials have been considered promising candidates as cathodes in aqueous zinc‐ion batteries (AZIBs) because of their low cost, environmental friendliness, and sustainable production. However, the rapid capacity fading and sluggish kinetics restrict their practical applications, especially under extremely low temperatures (−50 °C). Here, by the condensation of hexaketocyclohexane octahydrate (HKCO) and 1, 2‐diaminoanthraquinone (DQ), a fully conjugated organic molecule, anthraquinone‐quinoxaline derivative (HATAN) is prepared. With the fully conjugated structure, HATAN possesses enhanced π‐electron delocalization and strong intermolecular interaction, which ensure superior electronic conductivity and physicochemical/electrochemical stability. Additionally, the introduction of multiple redox‐active sites (C═O and C═N) can increase the theoretical capacity of HATAN. Consequently, the HATAN cathode for AZIBs exhibits remarkable capacity, long lifespan, and high‐rate capability. Even at −50  C, an exceptional capacity of 75.4 mAh g−1 and 98% capacity retention over 1500 cycles can be preserved. This study presents valuable insights into the structure design of small molecule organic cathodes for advanced AZIBs which can efficiently operate at −50 °C. [ABSTRACT FROM AUTHOR]

Zn‐I2 batteries suffer from uncontrollable shuttle effects of polyiodine ions (I3− and I5−) at the cathode/electrolyte interface and side reactions induced by reactive H2O at the anode/electrolyte interface. In this study, a hydrated eutectic electrolyte is designed that synergizes the eutectic network and functional interfacial adsorbed layer to develop high‐performance Zn‐I2 batteries. The eutectic network can restrain active H2O molecules in the electrolyte to inhibit the side reaction at the anode/electrolyte interface and shuttle effect at the cathode/electrolyte interface. Additionally, the functional interfacial adsorbed layer guides the nucleation behavior of Zn2+ to inhibit the growth of dendrites and also separates the zinc anode from direct contact with active H2O molecules and polyiodine ions to inhibit corrosion. Theoretical calculation, in situ Ultraviolet–visible spectroscopy (UV‐vis) and Raman characterizations, and visualization experiments demonstrate that the hydrated eutectic electrolyte effectively inhibits the shuttling effect and improves the reversibility of zinc deposition/stripping behavior. Consequently, the Zn‐I2 battery can maintain a capacity of 133 mAh g−1 after 5000 cycles at 5 C. This highly efficient synergistic strategy offers a practical approach to the development of advanced Zn‐I2 batteries. [ABSTRACT FROM AUTHOR]

Sodium‐ion batteries (SIBs) are a promising candidate for large‐scale energy storage due to the low cost and abundant sodium resources. However, the formation of sodium dendrites on the surface of hard carbon (HC) anodes is the most intractable challenge for full cells during charging, leading to severe performance degradation and safety hazards. Here, a robust additive‐induced borate and fluoride‐rich interphase is constructed by introducing sodium difluoro(oxalato)borate (NaDFOB) as additive in the ether‐based electrolyte to relieve the performance deterioration for SIBs. NaDFOB can participate in the passivation process of electrolyte‐electrode interfaces through preferential oxidation and reduction of DFOB− to effectively restrain the growth of sodium dendrites. Moreover, the electrolyte decomposition and dissolution of transition metal ions are effectively inhibited. Benefiting from that, FeMn‐based Prussian blue (FeMnHCF) || HC full cell with a negative/positive capacity ratio (N/P ratio) of 1.09 displays a capacity retention of 82.1%, especially with a low N/P ratio of 0.96 the cell still demonstrates a stable Coulombic efficiency of over 99.9% after 500 cycles via using NaDFOB as additive. As a practical demonstration, the designed 18650 full cells display enhanced cycling stability with NaDFOB additive. The findings provide insights into the additive‐induced inorganic‐rich interfacial layers for dendrite‐free SIBs. [ABSTRACT FROM AUTHOR]

The development of stable electrode materials for sodium‐ion batteries (NIBs) with excellent rate capacity, high volumetric/gravimetric capacity, and ultralong‐term cycling stability still remains a challenge. Herein, a novel strategy for the synthesis of edge‐nitrogen‐rich carbon dots pillared graphene blocks (N‐CDGB) through self‐polymerization of aniline into graphene oxide blocks, and subsequent carbonization is developed. Due to high bulk density (1.5 g cm−3) and integrated lamellar structure with large edge‐interlayer spacing (4.2 Å) pillared by nitrogen‐doped carbon dots (95% edge‐nitrogen content), the dense N‐CDGB shows robust structural stability, fast ion/electron transfer pathways, and more active sites for sodium storage. As a result, the N‐CDGB electrode exhibits ultrahigh reversible volumetric and gravimetric capacities (780 mAh cm−3/520 mAh g−1 at 0.02 A g−1) far exceeding those of graphene (108 mAh cm−3/290 mAh g−1) and hard carbon (297 mAh cm−3/311 mAh g−1), excellent rate capability (118 mAh g−1/177 mAh cm−3 at 10 A g−1), and superior cycling stability up to 10 000 cycles with almost no capacity loss at 10 A g−1. This work signifies the superiority of densely pillared structure in the future development of NIBs with high volumetric/gravimetric capacity and ultralong‐term cycling stability. Edge‐nitrogen‐rich carbon dots pillared graphene blocks synthesized from natural graphite exhibit ultrahigh volumetric/gravimetric capacities (780 mAh cm−3/520 mAh g−1 at 0.02 A g−1), excellent rate performance, and ultralong cycle life. [ABSTRACT FROM AUTHOR]