J Am Chem Soc
September 2025
An electrolytic Zn-MnO battery is highly valued due to its cost-effectiveness, environmental friendliness, and abundant resource availability. However, the battery's performance is hindered by the slow kinetics at the poorly conductive MnO cathode and hydrogen evolution at the Zn anode. Here, a strategy of P-O-M (M = Mn, Zn) d-pπ backbonding design is proposed for phosphorus-oxygen electrolyte additives, which can be realized by tuning the atomic dipole moment-corrected Hirshfeld (ADCH) population charge of the P/O atom.
View Article and Find Full Text PDFAdv Sci (Weinh)
July 2025
Aqueous zinc-manganese oxide (Zn-MNO) batteries represent a compelling solution for grid-scale energy storage due to their inherent safety, cost-effectiveness and ecological compatibility. However, the commercialization of this technology faces critical challenges including insufficient electrode durability, limited areal capacity output, and fundamentally ambiguous charge storage principles, which collectively hinder practical implementation. Through systematic mechanistic investigation, a previously overlooked phase evolution paradigm is revealed.
View Article and Find Full Text PDFThe development of high-performance Zn-ion batteries is hindered by sluggish reaction kinetics and inadequate redox activity in conventional vanadium-based cathodes. Herein, a thermal oxidation phase-engineering strategy is proposed to construct a comprising VSSe core and oxygen-enriched VO and VO interfaces triple-phase heterojunction cathode. This unique architecture leverages a significantly increased specific surface area, which facilitates rapid electrode-electrolyte interactions and boosts pseudocapacitive contributions.
View Article and Find Full Text PDFUncontrollable dendrite growth can jeopardize the cycle life of aqueous Zn batteries. Here, we propose a general strategy of engineering artificial protrusions (APs) on the electrode surface to regulate the distribution of the electrode interface electric field and induce stable Zn plating/stripping for Zn batteries. The junction-free AP-Cu network is constructed on Cu foil by an ultrafast Joule-heating-welding method.
View Article and Find Full Text PDFThe global clean energy transition and carbon neutrality call for developing high-performance batteries. Here we report a rechargeable lithium metal - catalytic hydrogen gas (Li-H) battery utilizing two of the lightest elements, Li and H. The Li-H battery operates through redox of H/H on the cathode and Li/Li on the anode.
View Article and Find Full Text PDFPhys Chem Chem Phys
March 2024
Lithium-sulfur (Li-S) batteries suffer from sluggish kinetics due to the poor conductivity of sulfur cathodes and polysulfide shutting. Current studies on sulfur redox catalysis mainly focus on the adsorption and catalytic conversion of lithium polysulfides but ignore the modulation of the electronic structure of the catalysts which involves spin-related charge transfer and orbital interactions. In this work, bimetallic phosphorus trisulfides embedded in Prussian blue analogue-derived nitrogen-doped hollow carbon nanocubes (FeCoPS/NCs) were elaborately synthesized as a host to reveal the relationship between the catalytic activity and the spin state configuration for Li-S batteries.
View Article and Find Full Text PDFThe development of safe and high-energy metal anodes represents a crucial research direction. Here, the achievement of highly reversible, dendrite-free transition metal anodes with ultrahigh capacities by regulating aqueous electrolytes is reported. Using nickel (Ni) as a model, theoretical and experimental evidence demonstrating the beneficial role of chloride ions in inhibiting and disrupting the nickel hydroxide passivation layer on the Ni electrode is provided.
View Article and Find Full Text PDFThe efficient storage of electrons and the type of conduction in semiconductor materials are important factors in determining their electrochemical performance. However, the interaction between these two factors is often overlooked by researchers. In this study, the effects of Ni doping at Co Ni O nanoparticles on the electronic storage form of the material and resulting changes in the conduction p/n-type are reported.
View Article and Find Full Text PDFAqueous zinc-chlorine battery with high discharge voltage and attractive theoretical energy density is expected to become an important technology for large-scale energy storage. However, the practical application of Zn-Cl batteries has been restricted due to the Cl cathode with sluggish kinetics and low Coulombic efficiency (CE). Here, an aqueous Zn-Cl battery using an inexpensive and effective MnO redox adsorbent (referred to Zn-Cl@MnO battery) to modulate the electrochemical performance of the Cl cathode is developed.
View Article and Find Full Text PDFThe development of Zn-free anodes to inhibit Zn dendrite formation and modulate high-capacity Zn batteries is highly applauded yet very challenging. Here, we design a robust two-dimensional antimony/antimony-zinc alloy heterostructured interface to regulate Zn plating. Benefiting from the stronger adsorption and homogeneous electric field distribution of the Sb/SbZn-heterostructured interface in Zn plating, the Zn anode enables an ultrahigh areal capacity of 200 mAh cm with an overpotential of 112 mV and a Coulombic efficiency of 98.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2022
A rechargeable aqueous electrolytic MnO/Zn battery (EMZB) based on a reversible Mn/MnO two-electron redox reaction in an acidic electrolyte is very attractive for large-scale energy storage due to its high output voltage, large gravimetric capacity, and low cost. However, severe hydrogen evolution corrosion (HEC) of the Zn anode in an acidic electrolyte limits its application. Here, a proton-trapping agent (PTA) is introduced in the electrolyte to improve the electrochemical performance of the EMZB.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2023
Aqueous zinc-ion batteries (AZBs) show promises for large-scale energy storage. However, the zinc utilization rate (ZUR) is generally low due to side reactions in the aqueous electrolyte caused by the active water molecules. Here, we design a novel solvation structure in the electrolyte by introduction of sulfolane (SL).
View Article and Find Full Text PDFRechargeable hydrogen gas batteries (RHGBs) have been attracting much attention as promising all-climate large-scale energy storage devices, which calls for low-cost and high-activity hydrogen evolution/oxidation reaction (HER/HOR) bifunctional electrocatalysts to replace the costly platinum-based catalysts. Based on density functional theory (DFT) computations, herein we report an effective descriptor-driven design principle to govern the HER/HOR electrocatalytic activity of double-atom catalysts (DACs) for RHGBs. We systematically investigate the -band center variation of DACs and their correlations with HER/HOR free energies.
View Article and Find Full Text PDFAqueous electrolytic MnO -Zn batteries are considered as one of the most promising energy-storage devices for their cost effectiveness, high output voltage, and safety, but their electrochemical performance is limited by the sluggish kinetics of cathodic MnO /Mn and anodic Zn/Zn reactions. To overcome this critical challenge, herein, a cationic accelerator (CA) strategy is proposed based on the prediction of first-principles calculations. Poly(vinylpyrrolidone) is utilized as a model to testify the rational design of the CA strategy.
View Article and Find Full Text PDFNano Lett
April 2022
Aqueous Zn batteries are emerging as promising energy storage devices. However, severe dendrite growth and side reactions of Zn anodes restrict their further development. Herein, we develop a nucleophilic interfacial layer (NIL) on Zn to achieve a highly stable Zn anode for rechargeable Zn batteries.
View Article and Find Full Text PDFAn aqueous electrolytic MnO-Zn battery with eye-catching Mn/MnO cathode chemistry has been attracting immense interest for next-generation energy storage devices due to its irreplaceable advantages. However, the limited MnO conductivity restricts its long service life at high areal capacities. Here, we report a high-performance electrolytic MnO-Zn battery via a bromine redox mediator, to enhance its electrochemical performance.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2016
ZnO nanosheet (NS) arrays have been synthesized by a facile ultrathin liquid layer electrodeposition method. The ion concentration and electrode potential play important roles in the formation of ZnO NS arrays. Studies on the structural information indicate that the NSs are exposed with (100) facets.
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