Negligible Volume Research Articles

Intermolecular interaction engineering to enhance Lithium-Ion storage in Two-Dimensional oxidized silicon nanosheet anodes

Unlike conventional Si anodes for use in Li-ion batteries, 2D oxidized Si nanosheets, i.e., siloxene, undergo negligible volume expansion during cycling owing to their unique geometries and chemical structures. Nevertheless, siloxene receives less attention than other Si-based nanostructures, partly because the interactions of siloxene with conventional binders and their effects on charge storage are largely unexplored. Herein, the intermolecular interactions of siloxene with four typical binders (alginate, carboxymethyl cellulose, polyacrylic acid, and α-polyvinylidene fluoride) are investigated to enhance the electrochemical performance using a simple method. The binders are selected using two criteria, i.e., polarity and functional groups, and they exhibit different intermolecular interactions with siloxene. Particularly, alginate forms the strongest intermolecular bonds, which are attributed to dipole–dipole attractions between the H atoms in siloxene and the OH groups in alginate. The trend of the intermolecular binding strengths of the binders is consistent with those of the cycling stabilities and rate performances. The alginate-based siloxene electrode displays an excellent charge capacity retention of 66 % after 500 cycles at 200 mA g−1, which is unprecedented for pristine siloxene anodes. This study provides useful guidelines for designing binders for use in electrode materials with chemical structures similar to that of siloxene.

Dual-salt assisted synergistic synthesis of Prussian white cathode towards high-capacity and long cycle potassium ion battery

Prussian blue analogues (PBAs) are considered as superior cathode materials for potassium-ion batteries (PIBs) because of their three-dimensional open framework structure, high stability, and low cost. However, the intrinsic lattice defects and low potassium content typically results in poor rate and cycling performance, thus limited their practical applications. In this work, high-quality K1.64FeFe(CN)6 (PW-HQ) material with less crystalline water (6.21%) and high potassium content (1.64 mol−1) was successfully synthesized by a novel coprecipitation method with potassium citrate (K-CA) and potassium chloride (KCl) addition. Specifically, the electrode delivers a reversible capacity of 113.1 mA h g−1 at the current rate of 50 mA g−1 with ∼100% coulombic efficiency. Besides, the electrode retained 90% reversible capacity at 500 mA g−1 current density after 1000 cycles, indicating only 0.01% capacity decay per cycle. Moreover, we have revealed that the introduction of K-CA controlled the chelating rate of Fe(II) and the addition of KCl increased the K+ content, hence improving the capacity and stability of the as-prepared electrodes. Structural evolution and potassium storage mechanism were further investigated by detailed ex-situ X-ray diffraction and in-situ Raman measurements, which demonstrated reversible potassiation/depotassiation behavior and negligible volume change during the electrochemical process. In general, this work provides an efficient strategy to eliminate water contents in Prussian blue cathode and improve its electrochemical performance, which plays a key role in promoting the industrialization of potassium ion batteries.

Designing shape-memory-like microstructures in intercalation materials

During the reversible insertion of ions, lattices in intercalation materials undergo structural transformations. These lattice transformations generate misfit strains and volume changes that, in turn, contribute to the structural decay of intercalation materials and limit their reversible cycling. In this paper, we draw on insights from shape-memory alloys, another class of phase transformation materials, that also undergo large lattice transformations but do so with negligible macroscopic volume changes and internal stresses. We develop a theoretical framework to predict structural transformations in intercalation compounds and identify crystallographic design rules necessary for forming shape-memory-like microstructures in intercalation materials. We use our approach to systematically screen open-source structural databases comprising n>5000 pairs of intercalation compounds. We identify candidate compounds, such as LixMn2O4 (Spinel), LixTi2(PO4)3 (NASICON), that approximately satisfy the crystallographic design rules and can be precisely doped to form shape-memory-like microstructures. Throughout, we compare our analytical results with experimental measurements of intercalation compounds. We find a direct correlation between structural transformations, microstructures, and increased capacity retention in these materials. These results, more generally, show that crystallographic designing of intercalation materials could be a novel route to discovering compounds that do not decay with continuous usage.

Soil Strength and Structural Stability Are Mediated by Soil Organic Matter Composition in Agricultural Expansion Areas of the Brazilian Cerrado Biome

A growing demand for resources has led to the expansion of agricultural areas worldwide. However, land conversion associated with poor soil management might lead to soil physical degradation. We investigated the effects of land conversion on soil physical properties in the Brazilian Cerrado region, under native Cerrado vegetation (NV)—pasture (PA) and NV—cropland (CL) conversion scenarios. Soil physical properties related to compaction, pore size distribution, and structure stability were assessed up to a 30 cm depth. Additionally, carbon levels of soil organic matter fractions (particulate and mineral-associated organic matter) were determined. Our results indicate that the compaction process equivalently reduced the soil porosity in PA and CL. However, soil penetration resistance was higher in PA (~2.5 MPa) than in CL (~1.5 MPa), as well as the stable mean weight diameter of soil aggregates. The highest total and labile organic carbon levels were observed in CL, while the lowest levels of total and labile organic carbon occurred in PA (smaller than in CL). These results suggest that the higher structural stability found in PA was mediated by the predominance of stabilized carbon (a decrease in the proportion of soil labile carbon), causing the gaining of soil strength under negligible soil volume variation (in comparison with CL). Our results suggest that the reduction in the soil porosity by compaction due to PA and CL uses can equivalently reduce macropore space and soil hydraulic functioning, and that soil carbon quality alterations (i.e., labile vs. stabilized fractions) are responsible for the gain in soil strength in long-term degraded PA areas. Future research should focus on understanding the magnitude in which soil organic matter controls soil physical attributes, such as soil strength in these expansion areas, and whether this gain in soil strength limits plant development and compromises productivity in the long term.

Evaluating the per site activity of common mesoporous materials as supports for aminosilica catalysts for the aldol reaction and condensation

Mesoporous silicas are regarded as ideal systems; however, they are complex. The materials can be functionalized with aminosilanes to produce highly active catalysts for aldol chemistry. Despite heterogeneous catalysts often having multiple sites, functionalized materials are tested assuming each site contributes equally to catalytic activity. Here, we functionalize common mesoporous silicas (MCM-41, MCM-48, and SBA-15) and determine the per site catalytic activity. The activity of functionalized MCM-41, MCM-48, and SBA-15 are similar if SBA-15 has negligible micropore volume (NMP-SBA-15). Site quantification data reveal that each material has four different types of sites. MCM-41 has the highest fraction of active sites; however, most sites are low activity. Interestingly, NMP-SBA-15 is as active as MCM-41. NMP SBA-15 has a higher fraction of high activity and medium activity sites than both MCM materials. Overall, each material has similar types of sites even though the materials have different pore structures and different pore sizes.

Operando X-ray Studies of Ni-Containing Heteropolyvanadate Electrode for High-Energy Lithium-Ion Storage Applications.

Ni-containing heteropolyvanadate, Na6[NiV14O40], was synthesized for the first time to be applied in high-energy lithium storage applications as a negative electrode material. Na6[NiV14O40] can be prepared via a facile solution process that is suitable for low-cost mass production. The as-prepared electrode provided a high capacity of approximately 700 mAh g-1 without degradation for 400 cycles, indicating excellent cycling stability. The mechanism of charge storage was investigated using operando X-ray absorption spectroscopy (XAS), X-ray diffraction (XRD), transition X-ray microscopy (TXM), and density functional theory (DFT) calculations. The results showed that V5+ was reduced to V2+ during lithiation, indicating that Na6[NiV14O40] is an insertion-type material. In addition, Na6[NiV14O40] maintained its amorphous structure with negligible volume expansion/contraction during cycling. Employed as the negative electrode in a lithium-ion battery (LIB), the Na6[NiV14O40]//LiFePO4 full cell had a high energy density of 300 W h kg-1. When applied in a lithium-ion capacitor, the Na6[NiV14O40]//expanded mesocarbon microbead full cell displayed energy densities of 218.5 and 47.9 W h kg-1 at power densities of 175.7 and 7774.2 W kg-1, respectively. These findings reveal that the negative electrode material Na6[NiV14O40] is a promising candidate for Li-ion storage applications.

Effect of Ti‐Substitution on the Properties of P3 Structure Na2/3Mn0.8Li0.2O2 Showing a Ribbon Superlattice

AbstractOxygen anion redox offers an effective strategy to enhance the energy density of layered oxide positive electrodes for sodium‐ and lithium‐ion batteries. However, lattice oxygen loss and irreversible structural transformations over the first cycle may result in large voltage hysteresis, thereby impeding practical application. Herein, ribbon superstructure ordering of Li/transition‐metal‐ions was applied to suppress the voltage hysteresis combined with Ti‐substitution to improve the cycling stability for P3‐Na0.67Li0.2Ti0.15Mn0.65O2. When both cation and anion redox reactions are utilized, Na0.67Li0.2Ti0.15Mn0.65O2 delivers a reversible capacity of 172 mA h g−1 after 25 cycles at 10 mA g−1 between 1.6–4.4 V vs. Na+/Na. Ex‐situ X‐ray diffraction data reveal that the ribbon superstructure is retained with negligible unit cell volume expansion/contraction upon sodiation/desodiation. The performance as a positive electrode for Li‐ion batteries was also evaluated and P3‐Na0.67Li0.2Ti0.15Mn0.65O2 delivers a reversible capacity of 180 mA h g−1 after 25 cycles at 10 mA g−1 when cycled vs. Li+/Li between 2.0–4.8 V.

Understanding the Structural Phase Transitions in Na3V2(PO4)3 Symmetrical Sodium-Ion Batteries Using Synchrotron Based X-Ray Techniques

Sodium ion batteries (SIBs) are the promising candidate for large scale applications due to their high abundance and low cost.The symmetrical SIBs (similar cathode and anode configuration) are highly promising as they exhibit negligible volume changes during the charge/discharge process and making SIBs highly stable. Several NASICON (sodium superionic conductor) have high potential towards symmetrical SIBs due to presence of multi-redox reactions in both anodic and cathodic regions. Na3V2(PO4)3 (NVP) has been found to be appeal for symmetrical SIB systems due to presence of flat voltage profile, multi-redox with a single transition metal, and a large working voltage difference between anodic and cathodic regions can greatly improve the output of the NVP symmetrical cell. However, the phase transitions associated during the electrochemical reaction in the symmetrical NVP cells are not widely studied. The synchrotron X-ray studies in NVP symmetrical cells confirms the redox reaction involving ≈2 moles of Na+ reaction instead of 1 mole of Na+ reaction. The in-situ X-ray diffraction and X-ray absorption spectroscopy during the electrochemical cycling confirms the reversible formation of Na5V2(PO4)3 phase in the anode and NaV2(PO4)3 phase in the cathode. The charge storage process in NVP cathode region is through V3+/V4+ redox, and charge storage process in NVP anode region is through V3+/V2+ redox. The 2 moles sodium-ion storage process can make a discharge capacity of ≈99 mAh g−1, increasing the energy output of the symmetrical NVP.

Investigating the impact of micropore volume of aminosilica functionalized SBA-15 on catalytic activity for amine-catalyzed reactions

Mesoporous materials such as SBA-15 are used in many applications since the materials are robust and have tunable properties. Whereas these materials are thought to be ideal, the materials are complex with the common synthesis methods producing materials that contain micropores. This work will investigate the impact of micropores on catalytic activity of aminosilica materials. For comparison, materials are formed using a standard method that produces materials with micropores (REG-SBA-15) and using a modified method that produces materials with negligible micropore volume (NMP-SBA-15). After grafting the calcined support with an aminosilane (either (N-methyl amino propyl) trimethoxy silane (denoted as 2°Am) or (N,N-diethyl-3-amino propyl) trimethoxy silane (3°Am)), catalytic testing experiments reveal that NMP-SBA-15 functionalized materials are more active than REG-SBA-15 functionalized materials for a range of reactions. The reactions include (a) glucose isomerization where amines interacting with surface silanols limit catalytic activity and (b) aldol and Knoevenagel chemistry where amine-silanol interactions increase the reaction rate. For aldol chemistry, the observed difference in rate is further investigated using site quantification experiments. Interestingly, the results reveal that three types of sites exist for each material, including sites that are (1) highly active, (2) intermediate active, and (3) inactive. NMR experiments indicate that amines immobilized on REG-SBA-15 supports are less mobile than amines on NMP-SBA-15. For REG-SBA-15, the materials are found to have aminosilanes that have limited mobility and the largest fraction of inactive sites, which suggests that the inactive catalytic sites are in the micropores. Overall, the design of highly active catalytic materials can be achieved using materials that have limited micropore volumes.

Emerging Solid-to-Solid Phase-Change Materials for Thermal-Energy Harvesting, Storage, and Utilization.

Phase-change materials (PCMs) offer tremendous potential to store thermal energy during reversible phase transitions for state-of-the-art applications. The practicality of these materials is adversely restricted by volume expansion, phase segregation, and leakage problems associated with conventional solid-liquid PCMs. Solid-solid PCMs, as promising alternatives to solid-liquid PCMs, are gaining much attention toward practical thermal-energy storage (TES) owing to their inimitable advantages such as solid-state processing, negligible volume change during phase transition, no contamination, and long cyclic life. Herein, the aim is to provide a holistic analysis of solid-solid PCMs suitable for thermal-energy harvesting, storage, and utilization. The developing strategies of solid-solid PCMs are presented and then the structure-property relationship is discussed, followed by potential applications. Finally, an outlook discussion with momentous challenges and future directions is presented. Hopefully, this review will provide a guideline to the scientific community to develop high-performance solid-solid PCMs for advanced TES applications.

Structural Stability and Phase Transitions in Zeolite A: An In Situ High Pressure-High Temperature Investigation.

The high pressure-high temperature structural stability of Zeolite A (ZA) has been studied using the X-ray diffraction (XRD) method. Structural studies at high temperatures show a reduction in the oxygen occupancy, belonging to the water molecule, indicating thermal dehydration and subsequent expulsion of water molecules from the pores of the structure. ZA does not undergo structural phase transition with temperature. However, structural transitions are observed in in situ XRD studies at high pressure and high temperature. At 1.3 GPa and 300 °C, the cubic ZA concomitantly transformed to cubic sodalite (SOD) and tetragonal zeolite NaP (ZNP). This transition was completely forbidden at 2.7 GPa, where a temperature-induced amorphization was favored at 250 °C. The thermal studies at higher pressure reveal the marginal influence of pressure on the thermal expansion coefficients of hydrated ZA. Pressure evolution of the high pressure-high temperature phases indicates no further phase transitions up to 5.9 GPa. The equation of state fit to the pressure-volume data of these phases show that ZNP is less compressible, followed by SOD and ZA. In contrast to the behavior at 0.1 MPa, SOD shows a pressure-induced negative thermal expansion (NTE) at 5.9 GPa. On the other hand, the positive thermal expansion (PTE) observed along the direction of c axis is compensated by the NTE along the a axis leading to a negligible volume thermal expansion for the ZNP structure. The bulk moduli and thermal expansion coefficients of all of the observed phases are reported. The outcomes of this study have been consolidated as a pressure-temperature phase diagram, which provides an insight into the technological and industrial applications of ZA at extreme conditions.

Interfacial Space Charge Enhanced Sodium Storage in a Zero‐Strain Cerium Niobite Perovskite Anode

AbstractIntercalation electrode materials store Na by incorporation into their framework structure without phase transformation and substantial large volume, resulting in the excellent cycling stability during electrochemical cycling. However, challenges arise due to a low capacity of intercalation electrode for sodium‐ion batteries (SIBs). Here, a perovskite oxide (Ce1/3NbO3 (CNO)) as an intercalation anode with dual functions of high capacity and excellent cycling stability is explored. The Na+ storage capacity of CNO (141.3 mAh g‐1) originates from not only sufficient cation vacancies but also the interfacial space charge storage of Na+ in the surface of CNO particles. Additionally, CNO exhibits excellent cycling stability with 90.2% capacity retention after 1000 cycles at 1 C, 99.4% capacity retention after 2000 cycles at 5 C, and 96.5% capacity retention after 10 000 cycles at 10 C. The cycling performance can be explained by the “zero‐stain” Na+ storage characteristic, where the maximal unit cell volume variation induced by Na+ insertion/extraction is calculated to be only 0.38%. Hence, CNO is a promising alternative for long‐life SIBs. The mechanisms that enable the storage of Na+ with negligible volume variation will guide new insights for the rational design of ultra‐stable electrode materials for SIBs.

Near-Zero Volume Expansion Nanoporous Silicon as Anode for Li-ion Batteries

In this work, novel near-zero volume expanding Si-dominant electrodes are presented as promising anodes for next-generation Li-ion batteries. The electrodes contain micrometer-size nano-porous Silicon particles with a carefully tuned morphology and synthesized via a scalable and cost-effective route. Volume expansion during electrochemical Li-Si alloying/de-alloying is found to be almost completely suppressed. Bi-layer pouch cells manufactured with the abovementioned Si-anodes, having industrial relevant areal capacities (≥3 mAh cm−2), and LiNi0.6Mn0.2Co0.2O2 cathodes, show indeed negligible volume expansion as demonstrated by operando dilatometric measurements during galvanostatic cycling and post-mortem SEM cross-sectional analysis.

Rational design of intrinsic and defective BGe monolayer as the anode material for Li-ion batteries

The rational design of high-performance anode materials is an effective strategy to expedite the development of next-generation lithium-ion rechargeable batteries (LIBs). In this work, the first-principles calculation method is applied to systematically investigate the adsorption and diffusion behaviors of Li ions on the intrinsic and defective BGe monolayer, as well as the application prospects of such materials acting as anode materials for LIBs. Our results show that intrinsic planar BGe monolayer has the advantages of high structural stability, distinct metallic feature and strong interaction with Li. In addition, Li migration on the BGe surface shows a low diffusion barrier (0.32 ​eV), which could guarantee a rapid charging/discharging capability. Interestingly, the presence of the single B vacancy defect weakens the adsorption strength of Li ion in the defective regions due to the charge redistribution. Correspondingly, the defect slightly impedes the diffusion performance, resulting in an increased energy barrier for Li ion (0.44 ​eV) to escape the defective regions. On the other hand, the intrinsic BGe monolayer could be lithiated into BGeLi3 with a theoretical specific capacity of 1927 ​mA ​h ​g−1. The moderate open-circuit voltage and the flexible structural stability with negligible volume change further enhance the reversibility of BGe anode materials. All these results provide a robust foundation for the rational design of BGe monolayer as an efficient anode material for LIBs.

Design of Three-Dimensional Metallic Biphenylene Networks for Na-Ion Battery Anodes with a Record High Capacity.

Na-ion batteries (NIBs) capture intensive research interest in large-scale energy storage applications because of sodium's abundant resources and low cost. However, the low capacity, poor conductivity, and short cycle life of the commonly used anodes are the main challenges in developing advanced NIBs. Here, stimulated by the recent successful synthesis of biphenylene [Science 2021, 372, 852], we show that these problems can be curbed by assembling armchair biphenylene nanoribbons of different widths into three-dimensional architectures, which lead to homogeneously distributed nanopores with robust structural and mechanical stability. Through density functional theory and molecular dynamics calculations combined with the tight-binding model, we find that the assembled 3D biphenylene structures are metallic and thermally stable up to 2500 K, where the metallicity is further identified to originate from the pz-orbitals (π-bonds) of the sp2 carbon atoms. Especially, the optimal assembled structures HexC28 (HexC46) deliver a gravimetric capacity of 956 (1165) mA h g-1 and a volumetric capacity of 1109 (874) mA h mL-1, which are much higher than those of graphite and hard carbon anodes. Moreover, they also show a suitable average potential, negligible volume change, and low diffusion energy barrier. These findings demonstrate that assembling biphenylene nanoribbons is a promising strategy for designing next-generation NIB anodes.

Enhanced Cyclability of Lithium Metal Anodes Enabled by Anti-aggregation of Lithiophilic Seeds.

Constructing 3D skeletons modified with lithiophilic seeds has proven effective in achieving dendrite-free lithium metal anodes. However, these lithiophilic seeds are mostly alloy- or conversion-type materials, and they tend to aggregate and redistribute during cycling, resulting in the failure of regulating Li deposition. Herein, we address this crucial but long-neglected issue by using intercalation-type lithiophilic seeds, which enable antiaggregation owing to their negligible volume expansion and high electrochemical stability against Li. To exemplify this, a 3D carbon-based host is built, in which ultrafine TiO2 seeds are uniformly embedded in nitrogen-doped hollow porous carbon spheres (N-HPCSs). The TiO2@N-HPCSs electrode exhibits superior Coulombic efficiency, high-rate capability, and long-term stability when evaluated as compertitive anodes for Li metal batteries. Furthermore, the superiority of intercalation-type seeds is comprehensively revealed through controlled experiments by various in situ/ex situ electron and optical microscopies, which highlights the excellent structural stability and lithiophilicity of TiO2 nanoseeds upon repeated cycling.

MoS2 with high 1T phase content enables fast reversible zinc-ion storage via pseudocapacitance

Zinc-ion batteries (ZIBs) have garnered considerable interest due to their inherent high safety, low cost, and environmental friendliness. However, the reaction mechanism of cathode material in ZIBs is not entirely clear. Herein, Mixed-phase MoS2 with a high proportion (66%) of 1T phase and 2H phase (TH-MoS2), synthesized by the hydrothermal method, is reported as the cathode material for ZIBs. Material characterizations show that TH-MoS2 have obvious two phase MoS2 with different crystal structures causes sulfur vacancies, increases interlayer spacing and intercalation water. TH-MoS2 cathode delivers excellent electrochemical performance, a satisfactory capacity of 156 mAh g−1, and an excellent cycling performance with 97.3% capacity retention after 500 cycles at 1 A g−1. The ex-situ characterizations elucidate that TH-MoS2 achieves highly reversible Zn2+ storage with negligible phase transition, volume change, and lattice distortion upon cycle. Based on kinetic analysis and first-principles calculations results, Zn2+ and H+ can be stored in TH-MoS2 and the energy storage mechanism of TH-MoS2 electrode is dominated by pseudocapacitance. Understanding the MoS2 reaction mechanism will facilitate comprehension of cathode materials for ZIBs.

Finite volume effects in the McLerran–Venugopalan initial condition for the JIMWLK equation

We revisit the numerical construction of the initial condition for the dipole amplitude from the McLerran–Venugopalan model in the context of the JIMWLK evolution equation. We observe large finite volume effects induced by the Poisson equation formulated on a torus. We show that the situation can be partially cured by introducing an infrared regularization. We propose a procedure which has negligible finite volume corrections. The control of the finite volume and finite lattice spacings effects is crucial when considering the numerical solutions of the JIMWLK evolution equation with the collinear improvement.

Non-perturbative thermal QCD at all temperatures: the case of mesonic screening masses

We present a strategy based on the step-scaling technique to study non-perturbatively thermal QCD up to very high temperatures. As a first concrete application, we compute the flavour non-singlet meson screening masses at 12 temperatures covering the range from T ∼ 1 GeV up to ∼ 160 GeV in the theory with three massless quarks. The calculation is carried out by Monte Carlo simulations on the lattice by considering large spatial extensions in order to have negligible finite volume effects. For each temperature we have simulated 3 or 4 values of the lattice spacing, so as to perform the continuum limit extrapolation with confidence at a few permille accuracy. Chiral symmetry restoration manifests itself in our results through the degeneracy of the vector and the axial vector channels and of the scalar and the pseudoscalar ones. In the entire range of temperatures explored, the meson screening masses deviate from the free theory result, 2πT, by at most a few percent. These deviations, however, cannot be explained by the known leading term in the QCD coupling constant g up to the highest temperature, where other contributions are still very relevant. In particular the vector-pseudoscalar mass splitting turns out to be of O(g4) in the entire range explored, and it remains clearly visible up to the highest temperature, where the two screening masses are still significantly different within our numerical precision. The pattern of different contributions that we have found explains why it has been difficult in the past to match non-perturbative lattice results at T ∼ 1 GeV with the analytic behaviour at asymptotically high temperatures.

Swelling-Resistant, Crosslinked Polyvinyl Alcohol Membranes with High ZIF-8 Nanofiller Loadings as Effective Solid Electrolytes for Alkaline Fuel Cells.

The present work investigates the direct mixing of aqueous zeolitic imidazolate framework-8 (ZIF-8) suspension into a polyvinyl alcohol (PVA) and crosslinked with glutaraldehyde (GA) to form swelling-resistant, mechanically robust and conductivity retentive composite membranes. This drying-free nanofiller incorporation method enhances the homogeneous ZIF-8 distributions in the PVA/ZIF-8/GA composites to overcome the nanofiller aggregation problem in the mixed matrix membranes. Various ZIF-8 concentrations (25.4, 40.5 and 45.4 wt.%) are used to study the suitability of the resulting GA-crosslinked composites for direct alkaline methanol fuel cell (DAMFC). Surface morphological analysis confirmed homogeneous ZIF-8 particle distribution in the GA-crosslinked composites with a defect- and crack-free structure. The increased ionic conductivity (21% higher than the ZIF-free base material) and suppressed alcohol permeability (94% lower from the base material) of PVA/40.5%ZIF-8/GA resulted in the highest selectivity among the prepared composites. In addition, the GA-crosslinked composites’ selectivity increased to 1.5–2 times that of those without crosslink. Moreover, the ZIF-8 nanofillers improved the mechanical strength and alkaline stability of the composites. This was due to the negligible volume swelling ratio (<1.4%) of high (>40%) ZIF-8-loaded composites. After 168 h of alkaline treatment, the PVA/40.5%ZIF-8/GA composite had almost negligible ionic conductivity loss (0.19%) compared with the initial material. The maximum power density (Pmax) of PVA/40.5%ZIF-8/GA composite was 190.5 mW cm−2 at 60 °C, an increase of 181% from the PVA/GA membrane. Moreover, the Pmax of PVA/40.5%ZIF-8/GA was 10% higher than that without GA crosslinking. These swelling-resistant and stable solid electrolytes are promising in alkaline fuel cell applications.