Strong Electrolytes Research Articles

Highly Selective CO2 Electroreduction to Multi‐Carbon Alcohols via Amine Modified Copper Nanoparticles at Acidic Conditions

AbstractElectroreduction of CO2 into multi‐carbon (C2+) products (e.g. C2+ alcohols) offers a promising way for CO2 utilization. Use of strong alkaline electrolytes is favorable to producing C2+ products. However, CO2 can react with hydroxide to form carbonate/bicarbonate, which results in low carbon utilization efficiency and poor stability. Using acidic electrolyte is an efficient way to solve the problems, but it is a challenge to achieve high selectivity of C2+ products. Here we report that the amine modified copper nanoparticles exhibit high selectivity of C2+ products and carbon utilization at acidic condition. The Faradaic efficiency (FE) of C2+ products reach up to 81.8 % at acidic media (pH=2) with a total current density of 410 mA cm−2 over n‐butylamine modified Cu. Especially the FE of C2+ alcohols is 52.6 %, which is higher than those reported for CO2 electroreduction at acidic condition. In addition, the single‐pass carbon efficiency towards C2+ production reach up to 60 %. Detailed studies demonstrate that the amine molecule on the surface of Cu cannot only enhance the formation, adsorption and coverage of *CO, but also provide a hydrophobic environment, which result in the high selectivity of C2+ alcohols at acidic condition.

Highly Selective CO2 Electroreduction to Multi-Carbon Alcohols via Amine Modified Copper Nanoparticles at Acidic Conditions.

Electroreduction of CO2 into multi-carbon (C2+) products (e.g. C2+ alcohols) offers a promising way for CO2 utilization. Use of strong alkaline electrolytes is favorable to producing C2+ products. However, CO2 can react with hydroxide to form carbonate/bicarbonate, which results in low carbon utilization efficiency and poor stability. Using acidic electrolyte is an efficient way to solve the problems, but it is a challenge to achieve high selectivity of C2+ products. Here we report that the amine modified copper nanoparticles exhibit high selectivity of C2+ products and carbon utilization at acidic condition. The Faradaic efficiency (FE) of C2+ products reach up to 81.8 % at acidic media (pH=2) with a total current density of 410 mA cm-2 over n-butylamine modified Cu. Especially the FE of C2+ alcohols is 52.6 %, which is higher than those reported for CO2 electroreduction at acidic condition. In addition, the single-pass carbon efficiency towards C2+ production reach up to 60 %. Detailed studies demonstrate that the amine molecule on the surface of Cu cannot only enhance the formation, adsorption and coverage of *CO, but also provide a hydrophobic environment, which result in the high selectivity of C2+ alcohols at acidic condition.

Synthesis and physicochemical studies of iron(III) complex compounds with TSC

The authors developed methods for the synthesis of coordination compounds of iron(III) with thiosemicarbazide (TSC).The compounds structure was proved by IR spectroscopy, conductometry, X-ray diffraction, and thermogravimetry. The authors found the bidentate coordination of TSC with iron(III) via sulphur and nitrogen atoms. Thermogravimetrically authors have established the proceeding of the complex decomposition in two stages. The first stage involves thermolysis of organic ligands with the formation of the corresponding iron salts; the second one includes decomposition of iron salts and formation of iron(III) oxide. Conductometrically we have established the synthesised complexes are strong electrolytes. X-ray diffraction shows the crystallisation of the complexes into orthorhombic syngonies. There are two structural units in the cell.

Differentiation of puerarin chelate from salt by phase solubility test

Different from salt, metal chelate is a novel state of drug constructed by more separate coordinate bonds to form a chelating circle. Due to their composition similarity, it is hard to distinguish them except identifying ionic bond (i.e., salt) or coordinate bond (i.e., chelate) in the single crystal structure. In this study, sodium chelate (CDCC No: 1865670) and lithium salt (CDCC No: 2161617) of puerarin (PUE) was prepared. In addition to difference in single crystal structure, it was found that they showed totally different phase solubility behaviors: lithium salt demonstrated a typical inverse proportion curve as other common salts, while sodium chelate exhibited disordered scatters. However, when incorporating the unit PUE-Na complex in solution state and complexation constant K11 in chemical equation, the scatters in phase solubility diagram of chelate could be well fitted and the value of K11 was dramatically higher with orders of magnitude than the dissociation constant Kc; while processing phase solubility curve of lithium salt by incorporating complex item, it could not well match the curve at all. PUE sodium chelate is more likely to be a weak electrolyte with partial dissociation, while PUE lithium salt acted as a strong electrolyte with complete dissociation. The phase solubility test would be served as a surrogate tool for differentiation of chelates from salts when single crystal was not available.

Fluorinated ester additive to regulate nucleation behavior and interfacial chemistry of room temperature sodium-sulfur batteries

Room temperature sodium-sulfur (RT Na-S) batteries are considered as advanced energy storage technology due to their low cost and high theoretical energy density. However, challenges such as the growth of sodium dendrite and dissolution of sodium polysulfides significantly hinder the electrochemical performance. Herein, we developed a propylene carbonate (PC)-based electrolyte with Methyl 2-Fluoroisobutyrate (MFB) as an additive. The ester group in the MFB additive is capable of participating in and reconfiguring the coordination of their Na+ solvated structures, thereby lowering the desolvation barrier and regulating the Na anode’s interfacial reaction and nucleation behavior. The polar C−F bond at the other end helps to reduce the lowest unoccupied molecular orbital (LUMO) energy of the MFB additive, enabling the preferential decomposition of MFB to form the F-rich inorganic phase strong polar solid electrolyte interphase (SEI), contributing to the inhibition of Na dendrite growth, the accumulation of dead Na. In addition, NaF-riched cathode electrolyte interphase (CEI) was also observed on sulfur-based cathode, which can effectively inhibited the shuttle effect. Consequently, the developed RT Na-S battery exhibit excellent electrochemical performance.

Access to Seleno‐Functionalized Thiazolo[3,2‐a]Pyrimidinones and Pyrimido[2,1‐b][1,3]Thiazinones via Selenocyclization of 2‐Alkenylthiopyrimidinones and Their Fused Analogs

AbstractThe methodology of electrophilic selenylation/cyclization of 2‐alkenylthiopyrimidinones and their fused analogs underlies most of the reported synthetic approaches to seleno‐functionalized thiazolo[3,2‐a]pyrimidinones and pyrimido[2,1‐b][1,3]thiazinones. We have developed a novel implementation of this strategy using as reagent phenylselenyl chloride or the visible‐light‐induced radical‐generating (PhSe)2/CBr4 system. The effect of the unsaturated substrate structure and reaction conditions on the selenocyclization regioselectivity has been revealed and analyzed in detail. It has been established that regardless of the conditions used, 2‐allylthiopyrimidinones react with selenylating agents via electrophilic 5‐exo‐trig cyclization mainly involving the N1 nitrogen atom to give selenium‐containing thiazolo[3,2‐a]pyrimidinones as major products. On the contrary, the selenocyclization with 2‐cinnamylthiopyrimidinones is dominated by the 6‐endo‐trig mode: it mostly involves six‐membered ring closure at the N1 or N3 atom thus leading to selenylated pyrimido[2,1‐b][1,3]thiazinones, with the regiochemistry governed by the position and nature of the substituents on the substrate pyrimidine ring. However, some of the fused cinnamylthio‐substituted substrates yield 5‐exo‐trig cyclized products in the LiClO4/МеNO2 system (a sufficiently polar solvent with a strong electrolyte added).

Binary aqueous solutions of choline salts: Determination and modelling of liquid density (298.15 or 313.15 K) and Vapour Pressure Osmometry (313.15 K)

Salts composed of the cholinium cation (such as choline hydroxide and choline chloride) have become one of the main reactants for the synthesis of greener ionic liquids, but, for a proper description of the aqueous solutions of these strong electrolytes by thermodynamic modelling, reliable data on liquid density (ρ) and vapour pressure (p) are needed, which are often unavailable. So, in this work, the liquid density (ρ) of binary aqueous solutions of choline bicarbonate ([Ch][Bic]), choline (2R,3R)-bitartrate ([Ch][Bit]), choline chloride ([Ch]Cl), choline dihydrogen citrate ([Ch][H2Cit]) and choline hydroxide ([Ch]OH) were measured at 298.15 or 313.15 K and 0.1 MPa and correlated using second-degree polynomials with salt molality (m), obtaining determination coefficients (R2) higher than 0.9974. Furthermore, the osmotic coefficients (ϕ) of these binaries were determined using vapour pressure osmometry (VPO), at 313.15 K and 0.1 MPa, being satisfactorily described by the Extended Pitzer Model of Archer, which yielded low values of standard deviation (3.58<σϕ·103<12.86). Then, the mean molal activity coefficients (γ±) and excess Gibbs free energies (GE/RT) were calculated, following the order [Ch][H2Cit] > [Ch][Bit] > [Ch][Bic] > [Ch]OH > [Ch]Cl, which corresponds to the decreasing polarity of the choline salts and agrees with the empirical law of matching water affinities (LMWA).

Improving rate performance of FeC2O4/rGO composites on lithium storage via single-polymerization‐induced electrostatic self‐assembly

Based on the wide interlayer distance for ions diffusion, iron (II) oxalate exhibits excellent lithium storage ability. However, the local deposition of metallic nanoparticles of Fe0 leads to low electrochemical reactivity, which hinders the actual application of FeC2O4 in large current regions (>5C). To solve this problem, a strong cationic polymeric electrolyte, polyelectrolyte diallyl dimethyl ammonium (PDDA), was introduced to construct a [FeC2O4(PDDA)]+ ligand. By single-polymerization‐induced electrostatic self-assembly, the [FeC2O4(PDDA)]+ ligand was combined with the surface-charged rGO to produce a FeC2O4/rGO material. It is proved that the rGO carrier improves the interparticle conductivity, electrochemical activity and structure stability of the iron (II) oxalate particles, ensuring the stability of Li || FeC2O4/rGO battery at a rapid charging rate of 20C (8 A g−1) for more than 500 cycles (with the special capacity of 713 mAh g−1). Compared with FeC2O4 electrode, owning to high reactivity of rGO and continuously activating on the nanoscale Fe metal generated at ∼0.75 V, FeC2O4/rGO shows higher electrochemical activity of conversion reaction in the first 50 cycles and better reversibility in the rate charge–discharge test (the capacity rapidly increased to 1158.8 mAh g−1 after 20C cycles). This work reveals how the structural design of conducting and supporting the carrier can achieve fast charging for iron (II) oxalate lithium-ion batteries.

The temperature of maximum in density of aqueous solutions of nitrate and ammonium salts: Testing the Madrid-2019 force field.

The shift in the temperature of maximum in density (TMD) at room pressure of aqueous solutions of a set of five salts containing NO3- and/or NH4+ groups is studied both through experiments and through molecular dynamics simulations using the Madrid-2019 force field for ions and the TIP4P/2005 model for water. The experiments demonstrate the potential transferability and limitations of the Madrid-2019 force field for nitrate and ammonium ions recently developed by our group at different temperatures and add updated information to the reported datasets of TMDs for strong electrolytes. By using the Despretz law, individual ion contributions are extracted for predictive purposes from the experimental values of the shift in the TMD. Interesting findings for the behavior of the shift in the TMD in nitrate salts expose that this property might be particularly challenging for modelization approaches when dealing with polyatomic species.

Electrolyte Design for Low Temperature Lithium‐Sulfur Battery: From Different Polysulfide Conversion Mechanisms

With the increasing demand for large‐scale energy storage devices, lithium‐sulfur (Li‐S) batteries have emerged as a promising candidate because of their ultrahigh energy density (2600 Wh Kg‐1) and the cost‐effectiveness of sulfur cathodes. However, the notorious shuttle effect derived from lithium polysulfide species (LiPSs) hampers their practical application, especially at low temperature. Therefore, electrolytes with low viscosity and high conductivity are required with the advancement of next‐generation Li‐S batteries. Understanding the interface structure dependent solvent electrochemistry and recognizing the existing issues relating to electrolytes are indispensable prerequisites. This review briefly summarizes the challenges to further develop the new generation of Li‐S batteries, which can operate steadily at subzero temperature, including LiPSs accumulation, Li2S nucleation, lithium deposition, and so on. On the basis of the crucial role of electrolytes in solving these questions, we outline the corresponding electrolyte design strategies from the different mechanisms (solid‐liquid‐solid conversion, all‐solid‐phase conversion, and all‐liquid‐phase conversion) such as lithium salt modification, additive introduction, and introduction of strong cationic electrolytes, as well as the application of solid‐state electrolytes, and so on. Finally, we emphasize promising strategies and solutions to improve low‐temperature performance, pointing the way for the future development of maximizing extreme‐temperature electrolytes toward practical applications.

Self-enhanced localized alkalinity at the encapsulated Cu catalyst for superb electrocatalytic nitrate/nitrite reduction to NH3 in neutral electrolyte.

The electrocatalytic nitrate/nitrite reduction reaction (eNOx-RR) to ammonia (NH3) is thermodynamically more favorable than the eye-catching nitrogen (N2) electroreduction. To date, the high eNOx-RR-to-NH3 activity is limited to strong alkaline electrolytes but cannot be achieved in economic and sustainable neutral/near-neutral electrolytes. Here, we construct a copper (Cu) catalyst encapsulated inside the hydrophilic hierarchical nitrogen-doped carbon nanocages (Cu@hNCNC). During eNOx-RR, the hNCNC shell hinders the diffusion of generated OH- ions outward, thus creating a self-enhanced local high pH environment around the inside Cu nanoparticles. Consequently, the Cu@hNCNC catalyst exhibits an excellent eNOx-RR-to-NH3 activity in the neutral electrolyte, equivalent to the Cu catalyst immobilized on the outer surface of hNCNC (Cu/hNCNC) in strong alkaline electrolyte, with much better stability for the former. The optimal NH3 yield rate reaches 4.0 moles per hour per gram with a high Faradaic efficiency of 99.7%. The strong-alkalinity-free advantage facilitates the practicability of Cu@hNCNC catalyst as demonstrated in a coupled plasma-driven N2 oxidization with eNOx-RR-to-NH3.

Protic ionic Liquids-Water Interactions: A study on 2-Hydroxypropylammonium formate through experimental analysis and computer simulations

In this study, interactions within a mixture of the protic ionic liquid 2-hydroxypropylammonium formate and water were investigated across the entire range of ionic liquid compositions and a wide temperature range from 283.15 K to 333.15 K. This investigation was based on the measurement results of density, viscosity, and electrical conductivity, and was supported by computational simulations. The synthesized ionic liquid was further characterized thermally using Thermogravimetric Analysis (TGA) and Differential Scanning Calorimetry (DSC) techniques. The study focuses on the analysis of excess molar quantities of volume, thermal expansion coefficients, viscosity, and Gibbs energy of viscous flow, aiming to examine the influence of temperature and mixture composition on thermophysical properties. The impact of temperature on the system’s viscosity and Angell’s strength parameter was investigated to assess the influence of the ionic liquid’s content on the system’s structural organization. The dependency of molar conductivity on viscosity was analyzed through the Walden rule. Based on this analysis, the effect of temperature and mixture composition on deviations from the ideal behavior in diluted solutions of strong electrolytes was estimated. Computational molecular dynamics simulations were employed for a more detailed study of the structural organization of the system’s components.

Electro-oxidation of 5-hydroxymethylfurfural in a low-concentrated alkaline electrolyte by enhancing hydroxyl adsorption over a single-atom supported catalyst

Electrocatalytic oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA), a sustainable strategy to produce bio-based plastic monomer, is always conducted in a high-concentration alkaline solution (1.0 mol L−1 KOH) for high activity. However, such high concentration of alkali poses challenges including HMF degradation and high operation costs associated with product separation. Herein, we report a single-atom-ruthenium supported on Co3O4 (Ru1-Co3O4) as a catalyst that works efficiently in a low-concentration alkaline electrolyte (0.1 mol L−1 KOH), exhibiting a low potential of 1.191 V versus a reversible hydrogen electrode to achieve 10 mA cm−2 in 0.1 mol L−1 KOH, which outperforms previous catalysts. Electrochemical studies demonstrate that single-atom-Ru significantly enhances hydroxyl (OH−) adsorption with insufficient OH− supply, thus improving HMF oxidation. To showcase the potential of Ru1-Co3O4 catalyst, we demonstrate its high efficiency in a flow reactor under industrially relevant conditions. Eventually, techno-economic analysis shows that substitution of the conventional 1.0 mol L−1 KOH with 0.1 mol L−1 KOH electrolyte may significantly reduce the minimum selling price of FDCA by 21.0%. This work demonstrates an efficient catalyst design for electrooxidation of biomass working without using strong alkaline electrolyte that may contribute to more economic biomass electro-valorization.

A semi-empirical equation modeling long-range contributions to the activity coefficients of individual ions at high ionic strengths

Molecular thermodynamics is well developed with models like UNIQUAC, UNIFAC and SAFT. These models include robust codes and extensive databases for chemical and petroleum industries through ASPEN, DORTMUND, and others. However, important systems in the pharmaceutical and biotech industries now exist where these codes and their databases are not always sufficient. Cell culture media used to grow mammalian cells are multicomponent aqueous solutions with 50, 100, or more compounds including amino acids, salts, acids or bases, as well as sugars, fatty acids, etc. These components can exhibit both complexation and incomplete dissociation. The thermodynamics of these systems have proven challenging to model, as current solubility descriptions frequently assume complete dissociation in solutions containing a single solute in water at relatively low concentrations. However, not all compounds that are generally considered to be strong electrolytes are completely dissociated even at low concentrations. Further, mixtures of such components can show dramatic changes in dissociation and complexation with concentration, pH, and temperature. In this paper, we present a semi-empirical model for individual ions in aqueous solutions. We use data from 317 compounds to isolate the ionic contribution to a compound’s activity coefficient in aqueous systems from confounding short-range effects. We compare eight robust regression M−estimators with a least-squares estimate and provide a two-parameter equation relating ionic strength, valence, and the activity coefficient not requiring arduous characterization of the solute of interest. We demonstrate that the Fair M−estimator generates an accurate model that can serve as an appropriate reference state for use with a model based on perturbation theory up to 29 molal.

Preparation and Performance of High-Temperature-Resistant, Degradable Inorganic Gel for Steam Applications

Summary To address the problems of steam channeling caused by the nonhomogeneity and fluid compatibility of the reservoir in heavy oil reservoirs and the permanent damage to the reservoir easily caused by traditional plugging agents, this study adopted polyaluminum chloride (PAC) as the main agent, urea as the coagulant promoter, and thiourea as the stabilizer and prepared a high-temperature-resistant (up to 350°C) degradable inorganic aluminum gel with excellent performance. Initially, scanning electron microscope (SEM) tests were conducted on gels with and without urea. Energy-dispersive X-ray spectroscopy (EDS)-mapping analysis of gels immersed in water with different mineralization levels for 5 days was then performed. The results revealed that the addition of urea led to a tighter and more complete crosslinked structure, significantly enhancing the mechanical strength of the gel. As water mineral content increased, the gel’s microstructure became denser and smoother. Metal cations on the cross-sectional surface increased gradually and distributed uniformly, further confirming the mechanism of the synergistic salt effect of soluble strong electrolytes and urea in strengthening the gel. Finally, the plugging and degradable properties of the gel were evaluated, and the results showed that the plugging percentage of the gel could still reach 97.6% after aging at 350°C for 30 days, and the gel had excellent plugging and diversion in dual sandpack experiments where the permeability ratio was less than 44. At 250°C, the degradation percentage of the gel was more than 98% at 5 days under the nonacid degradation system and 94% at 5 days under the acid degradation system. The gel showed good degradability and effectively reduced the damage to the reservoir.

Regulation of Dipolar‐Dipolar and Ion‐Dipolar Interactions Simultaneously in Strong Solvating Electrolytes for All‐Temperature Zinc‐Ion Batteries

AbstractAqueous zinc‐ion batteries (AZIBs) attract attention due to their safety and high specific capacity. However, their practical applications are constrained by Zn anode corrosion, dendritic growth, and poor temperature adaptability induced by a strong hydrogen‐bond network in aqueous electrolytes. Herein, a universal strategy to design strong solvating electrolytes is proposed, in which the hydrogen‐bond network and solvation structures are reconstructed by regulating the dipolar‐dipolar and ion‐dipolar interactions simultaneously. Consequently, the hydrogen‐bond network in free water is largely weakened, and the water content in the Zn2+ solvated sheath is reduced, while the hydrogen‐bond network between solvents is strengthened, which effectively broadens the operating temperature range and suppresses Zn dendrites and corrosion. As a result, Zn anodes exhibit excellent platting/stripping efficiency with an average Coulombic Efficiency up to 99.89% after 2000 cycles at 0.5 mA cm−2, impressive cycling stability (5000 h, 0.5 mA cm−2/0.5 mA h cm−2), and a wide operating temperature range of 140 °C (−50–90 °C). Moreover, the Zn//V2O3 full cells also display enhanced temperature‐resistance, implying that the designed strong solvation electrolyte has practical application potential in extreme environments. This study suggests a promising strategy to design ideal electrolytes for high‐performance AZIBs with safety, ultralong cycling life, and satisfying temperature‐resistance.

Influence of Thermal and Chemical Stresses on Thermal Properties, Crystal Morphology, and Mechanical Strength Development of a Sulfur Polymer Composite

The unique properties and sustainability advantages of sulfur polymer cement have led to efforts to use them as alternatives to traditional Portland cement. The current study explores the impact of environmental stresses on the strength development of polymer composite SunBG90, a material composed of animal and plant fats/oils vulcanized with 90 wt. % sulfur. The environmental stresses investigated include low temperature (−25 °C), high temperature (40 °C), and submersion in water, hexanes, or aqueous solutions containing strong electrolyte, strong acid, or strong base. Samples were analyzed for the extent to which exposure to these stresses influenced the thermo-morphological properties and the compressional strength of the materials compared to identical materials allowed to develop strength at room temperature. Differential scanning calorimetry (DSC) analysis revealed distinct thermos-morphological transitions in stressed samples and the notable formation of metastable γ-sulfur in hexane-exposed specimens. Powder X-ray diffraction confirmed that the crystalline domains identified by DSC were primarily γ-sulfur, with ~5% contribution of γ-sulfur in hexane-exposed samples. Compressive strength testing revealed high strength retention other than aging at elevated temperatures, which led to ~50% loss of strength. These findings reveal influences on the strength development of SunBG90, lending important insight into possible use as an alternative to OPC.

Chemotactic particles as strong electrolytes: Debye-Hückel approximation and effective mobility law.

We consider a binary mixture of chemically active particles that produce or consume solute molecules and that interact with each other through the long-range concentration fields they generate. We analytically calculate the effective phoretic mobility of these particles when the mixture is submitted to a constant, external concentration gradient, at leading order in the overall concentration. Relying on an analogy with the modeling of strong electrolytes, we show that the effective phoretic mobility decays with the square root of the concentration: our result is, therefore, a nonequilibrium counterpart to the celebrated Kohlrausch and Debye-Hückel-Onsager conductivity laws for electrolytes, which are extended here to particles with long-range nonreciprocal interactions. The effective mobility law we derive reveals the existence of a regime of maximal mobility and could find applications in the description of nanoscale transport phenomena in living cells.

Cu microvia filling by pulse-reverse electrodeposition with a single accelerator

Cu electrodeposition processes are widely employed to achieve defect-free interconnections in electronic devices. Typically, combinations of three additives—an accelerator, a suppressor, and a leveler—are used for bottom-up filling of Cu in microscaled features. However, the use of multiple additives adds complexity to electrolyte maintenance and can lead to reliability issues in the process. To address this challenge, we have developed a single-accelerator filling technique using pulse-reverse electrodeposition for microvias. During pulse-reverse electrodeposition, the anodic steps produce a large amount of Cu+ ions near the electrode surface. These Cu+ ions can form complexes with Cl− ions or CuCl layers, thereby enhancing the adsorption of the accelerator, SPS. This phenomenon depends on the electrolyte convection. Under strong forced convection, Cu-Cl species are removed, leading to subsequent deactivation of SPS, whereas Cu-Cl species remain stable under mild convection conditions. Based on this convection-dependent behavior of SPS and Cl, Cu electrodeposition is promoted at the bottom of microvias while the SPS is selectively deactivated outside the microvias where the strong electrolyte motion exists. As a result, without any polymeric suppressor and organic leveler, the microvias are successfully filled with Cu.

Self-adhesive, freeze-tolerant, and strong hydrogel electrolyte containing xanthan gum enables the high-performance of zinc-ion hybrid supercapacitors

Hydrogel electrolyte is an ideal candidate material for flexible energy storage devices due to its excellent softness and conductivity properties. However, challenges such as the inherent mechanical weakness, the susceptibility to be frozen in low-temperature environments, and the insufficiency of hydrogel-electrode contact persist. Herein, a “Multi in One” strategy is employed to effectively conquer these difficulties by endowing hydrogels with high strength, freeze-resistance, and self-adhesive ability. Multiple hydrogen bond networks and ion crosslinking networks are constructed within the hydrogel electrolyte (PVA/PAAc/XG) containing polyvinyl alcohol (PVA), acrylic acid (AAc), and xanthan gum (XG), promoting the enhanced mechanical property, and the adhesion to electrode materials is also improved through abundant active groups. The introduction of zinc ions provides the material with superior frost resistance while also promoting electrical conductivity. Leveraging its multifunction of superior mechanical strength, anti-freeze property, and self-adhesive characteristic, the PVA/PAAc/XG hydrogel electrolyte is employed to fabricate zinc ion hybrid supercapacitors (ZHS). Remarkably, ZHS exhibits outstanding electrochemical performance and cycle stability. A remarkable capacity retention rate of 83.86 % after 10,000 charge-discharge cycles can be achieved at high current densities, even when the operational temperature decreases to −60 °C, showing great potential in the field of flexible energy storage devices.