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The notorious dendrite growth and hydrogen evolution reaction (HER) are considered as main barriers that hinder the stability of the Zn-metal anode. Herein, molecular engineering is conducted to optimize the inner Helmholtz plane with a trace of amphiphilic dibenzenesulfonimide (BBI) in an aqueous electrolyte. Both experimental and computational results reveal that the BBI binds strongly with Zn to form {Zn(BBI)(H O) } in the electrical double layer and reduces the water supply to the Zn anode. During the electroplating process, {Zn(BBI)(H O) } is "compressed" to the Zn anode/electrolyte interface by Zn flow, and accumulated and adsorbed on the surface of the Zn anode to form a dynamic water-poor inner Helmholtz plane to inhibit HER. Meanwhile, the{Zn(BBI)(H O) } on the Zn anode surface possesses an even distribution, delivering uniform Zn flow for smooth deposition without Zn dendrite growth. Consequently, the stability of the Zn anode is largely improved with merely 0.02 M BBI to the common electrolyte of 1 M ZnSO . The assembled Zn||Zn symmetric cell can be cycled for more than 1180 h at 5 mA cm and 5 mA h cm . Besides, the practicability in Zn||NaV O ·1.5 H O full cell is evaluated, which suggests efficient storage even under a high mass loading of 12 mg cm .
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http://dx.doi.org/10.1002/advs.202301785 | DOI Listing |
Adv Mater
August 2025
State Key Laboratory of Silicon and Advanced Semiconductor Materials, School of Materials Science and Engineering, Zhejiang University, Hangzhou, 310027, China.
The capability of sodium-ion batteries (SIBs) to operate under extreme temperatures is highly desirable; however, achieving stable performance remains challenging due to limitations in interfacial dynamics. Here, it is revealed that at low temperatures, linear solvents tend to aggregate within the inner Helmholtz plane (IHP), leading to the formation of a solvent-derived solid-electrolyte interphase (SEI) with sluggish Na diffusion kinetics. To address this issue, it is proposed to leverage the polarization interaction induced by the orbital overlap between the solvent molecules and free radicals as an effective approach to breaking solvent aggregation.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
State Key Laboratory of High-Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200062, P. R. China.
Ions are essential components in the anode-electrolyte interfacial microenvironment that significantly influence both the activity and the pathway of electrocatalytic molecular oxidation reactions. Nevertheless, most anions are generally considered inhibitory on electrocatalytic molecular (such as alcohols and amines) oxidation reactions due to their specific adsorption at the inner Helmholtz layer, negatively impacting the electrocatalytic performance. In contrast, we have found herein that fluorine ion (F) at the outer Helmholtz layer is capable of largely elevating the electrocatalytic activity and promoting the transformation of glyceric acid to lactic acid as the main product by fluorine-hydrogen bonding with water molecules, glycerol reactants, and glyceraldehyde intermediate during the glycerol oxidation reaction.
View Article and Find Full Text PDFJ Am Chem Soc
August 2025
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200438, China.
The electrode/electrolyte interfacial structure is a seminal component that governs the activity of electrocatalytic water splitting, providing alternative approaches to electrocatalyst design. Herein, we demonstrate that a dense interface constituting of zwitterionic betaine could selectively accelerate the alkaline oxygen evolution reaction (OER) by 2 orders of magnitude in current. The hygroscopic betaine molecules not only bind water molecules strongly but also endow the underhydrated characteristics of the hydroxide anions that increase their activity coefficient.
View Article and Find Full Text PDFPhys Rev Lett
August 2025
State Key Laboratory of Particle Detection and Electronics, Beijing 100049, Hefei 230026, People's Republic of China.
Using 20.3 fb^{-1} of e^{+}e^{-} collision data collected at a center-of-mass energy of E_{c.m.
View Article and Find Full Text PDFSmall
August 2025
Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou, 213164, China.
Regulating the electric double layer (EDL) at the Zn/electrolyte interface by adding additives into aqueous electrolyte have received considerable attention because it is cost-effective to enhance the electrochemical performance of aqueous Zinc ion batteries (AZIBs). However, the balance between kinetics and reversibility during the Zn deposition/dissolution process remains challenging. In this work, the Diethoxydimethylsilane (DDS) additive with an appropriate concentration is introduced into 3 mol kg ZnSO (3 m ZSO) electrolyte to regulate the favorable EDL on the Zn surface.
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