Bond Breaking Research Articles

In Situ Growth of Silver Nanoparticles into Reducing-End Carbohydrate-Based Supramolecular Hydrogels for Antimicrobial Applications.

Hydrogels with antibacterial activities have the potential for many biomedical applications, such as wound healing, because of their capacity to maintain a moist environment and prevent infections. In this work, an ultrasound-induced supramolecular hydrogel consisting of easily accessible reducing-end-free glucosaminylbarbiturate-based hydrogelators that serve the in situ fabrication of silver nanoparticles (AgNPs), excluding the addition of any external reducing or stabilizing agents, has been developed. The innovative synthetic approach relied on the use of N,N'-disubstituted barbituric acid derivatives as a versatile chemical platform that site-selectively reacted with the amino function of glucosamine. A series of glucosaminylbarbiturate were synthesized, and we identified one carbohydrate-based hydrogelator that produced a thixotropic supramolecular hydrogel after ultrasound-mediated breaking of an intralocked hydrogen bond. AgNPs@hydrogels were prepared through in situ reduction of silver ions mediated by the reducing properties of carbohydrates. The AgNPs@hydrogel composite revealed good antimicrobial properties toward both Gram-positive and Gram-negative bacteria. These findings contribute to the development of carbohydrate-based supramolecular hydrogels and make them promising efficient and safe soft materials for antimicrobial therapy.

Quantitative assessment of hardened leather artifact deterioration using infrared spectroscopy

This article describes a quantitative assessment method proposed to quickly identify the degree of deterioration of hardened leather artefacts. We used three techniques to artificially age samples, namely, dry-heat ageing (DH), UV-ageing (UV), and alkali-thermal ageing (AT). The deterioration mechanisms were studied via thermogravimetry/derivative thermogravimetry (TG/DTG) and attenuated total reflectance Fourier transform infrared spectroscopy (ATR-FTIR). Combined with amide III band deconvolution and second derivative fitting, we constructed a method for assessing the degree of deterioration by the relative content of random coils (referred to as R) in the secondary structure of the protein. The results show that with increasing ageing time, the macrostructures and microstructures of the leather changed to varying degrees. This study elucidates the differential behaviour of vegetable-tanned leather collagen under oxidative and hydrolytic mechanisms. Based on the deterioration characteristics and fitting results, we divided the hardened leather into the following three levels. Mild deterioration: 0 ≤ R ≤ 5%; leather with reduced pores and slight dryness and hardness but with a stable collagen structure; if the β-sheet content is ≥ 68% at this point, the leather may be recrosslinked by ultraviolet irradiation. Moderate deterioration: 6 ≤ R ≤ 25%; partial hydrogen bond breaking in leather, loosening of the collagen–tan matrix, dry and hard curling of the leather surface, and fibre cementation. Severe deterioration: R ≥ 40%, β-sheet ≤ 24%, and the α-helix is higher; surface reflection, severe macroscopic deformation and embrittlement, and the breakdown and gelatinization of the three-stranded helical structure of leather proteins. The quantitative analysis method was suitable for studying the deterioration mechanisms and assessing the degree of deterioration in Heishanling leather artefacts, which also provides a new practical scheme for assessing the degree of hardened leather.Graphical

Real-Time Quantification of Molecular-Level Dynamic Behaviors Underpinning Shear Thinning in End-Linked Associative Polymer Networks.

Shear thinning of associative polymers is tied to bond breakage under deformation and retraction of dangling chains, as predicted by transient network theories. However, an in-depth understanding of the molecular mechanisms is limited by our ability to measure the molecular states of the polymers during deformation. Herein, utilizing a custom-built rheo-fluorescence setup, bond dissociation in model end-linked associative polymers is quantified in real time with nonlinear shear deformation based on a fluorescence quench transition when phenanthroline ligands bind with Ni2+. All of the networks exhibit shear thinning, and the dangling chain fraction increases with the shear rate. However, the number of broken bonds is smaller than that predicted by transient network theories, indicating additional relaxation modes or topological inhomogeneities in the networks. Through tuning counteranion chemistry, networks with similar relaxation times but varying dissociation and association rate constants (kd and ka) of Ni2+-phenanthroline cross-links are developed. Decreasing ka contributes to more dangling chain formation, while the effect of kd is less pronounced. Following force-accelerated bond dissociation of bridging chains, the dangling ends in networks with higher ka tend to reassociate to form elastically inactive loops, while the dangling chains are preserved in networks with lower ka. This indicates the critical role of bond reassociation kinetics in dictating shear-induced topological interchange of different chain configurations. Besides reaction kinetics, decreasing network junction functionality results in less shear thinning and broken bonds, originating from the lower amount of bond breakage required to flow and the higher tendency of the dissociated bonds to reform bridging chains.

Unveiling Tetrafluoromethane Decomposition over Alumina Catalysts.

Tetrafluoromethane (CF4), the simplest perfluorocompound known as a "forever chemical", presents substantial environmental challenges due to its health risks and contribution to the greenhouse effect. Designing efficient catalysts for CF4 decomposition remains difficult, compounded by limited understanding of the mechanisms. Here, we use constrained ab initio molecular dynamics (cAIMD) simulations and in situ experiments to elucidate the mechanism of alumina-catalyzed CF4 decomposition, highlighting the pivotal role of surface hydroxyl groups. The initial C-F bond breaking is the rate-determining step, with surface hydroxyl groups reducing the reaction free energy from 1.69 to 1.34 eV. These hydroxyl groups also facilitate the self-healing of oxygen vacancies generated during the decomposition. Contrary to the belief that CF4 decomposes directly into CO2, our cAIMD simulations, supported by synchrotron vacuum ultraviolet photoionization mass spectrometry data, reveal significant CF2O and CO byproducts. Experimental data in an anhydrous environment indicate that water primarily replenishes surface hydroxyl groups rather than directly participating in decomposition. We conclude that the relatively high efficiency of Al2O3 catalysts stems from three key properties: (1) the presence of active sites with a specific affinity for CF4 adsorption, ensuring efficient substrate interaction; (2) appropriate metal-oxygen bond strength, enabling the participation of lattice oxygen in the reaction; and (3) a high density of surface hydroxyl groups that facilitate the initial C-F bond cleavage and the self-healing of oxygen vacancies.

Pt-ZnOx Interfacial Effect on the Performance of Propane Dehydrogenation and Mechanism Study.

Bimetallic Pt-based catalysts, for example, PtZn and PtSn catalysts, have gained significant attention for addressing the poor stability and low selectivity of pristine Pt catalysts over propane dehydrogenation (PDH). However, the structures of the active sites and the corresponding catalytic mechanism of PDH are still elusive. Here, we demonstrate a spatially confined Pt-ZnmOx@RUB-15 catalyst (where "m" is the mole ratio of Zn/Pt and RUB-15 is a layered silica), which exhibited high catalytic activity, ultrahigh selectivity (>99%), and resistance to coking at 550 °C for PDH. Significantly different from the preliminary studies over the PtZn catalysts, through the assistance of quasi-in situ X-ray photoelectron spectroscopy (XPS), in situ Fourier transform infrared spectroscopy (CO-FTIR), in situ X-ray absorption spectroscopy (XAS), and CO titration, we discovered that the active sites for PDH were the Pt-ZnOx interfaces, characterized by a structure of Ptδ+-Zn2+-O-Si. Density functional theory (DFT) calculations showed that Pt atoms positioned at Pt-ZnOx interfaces with coordinatively unsaturated ZnOx sites facilitate the C-H bond breaking of propane while concurrently suppressing deep dehydrogenation processes. This study suggests that engineering the interfaces of Pt-metal oxides under spatially confined conditions holds promise for developing highly efficient Pt-based catalysts for light alkane dehydrogenation.

Ultrafast signatures of merocyanine overcoming steric impedance in crystalline spiropyran

Isomerisation through stereochemical changes and modulation in bond order conjugation are processes that occur ubiquitously in diverse chemical systems and for photochromic spirocompounds, it imparts them their functionality as phototransformable molecules. However, these transformations have been notoriously challenging to observe in crystals due to steric hindrance but are necessary ingredients for the development of reversible spiro-based crystalline devices. Here, we report the detection of spectroscopic signatures of merocyanine due to photoisomerisation within crystalline spiropyran following 266 nm excitation. Our femtosecond spectroscopy experiments reveal bond breaking, isomerisation and increase in bond order conjugation towards the formation of merocynine on a sub-2 ps time scale. They further unveil a lifetime of several picoseconds for the initial open ring intermediate with subsequent relaxation to mercocyanine, with established back connversion pathways, which make the system highly reversible in the solid state. Supporting femtosecond electron diffraction studies suggest that lattice strain favours the return of photoproduct to the closed spiroform. Our work thus paves the way for novel ultrafast applications from spiropyran-derived compounds.

Cell Senescence and the DNA Single-Strand Break Damage Repair Pathway

Cellular senescence is a response to endogenous and exogenous stresses, including telomere dysfunction, oncogene activation, and persistent DNA damage. In particular, radiation damage induces oxidative base damage and bond breaking in the DNA double-helix structure, which are treated by dedicated enzymatic repair pathways. In this review, we discuss the correlation between senescence and the accumulation of non-repaired single-strand breaks, as can occur during radiation therapy treatments. Recent in vitro cell irradiation experiments using high-energy photons have shown that single-strand breaks may be preferentially produced at the borders of the irradiated region, inducing senescence in competition with the apoptosis end-point typically induced by double-strand breaks. Such a particular response to radiation damage has been proposed as a possible cause of radiation-induced second primary cancer, as cells with an accumulation of non-repaired single-strand breaks might evade the senescent state at much later times. In addition, we highlight the peculiarities of strand-break repair pathways in relation to the base-excision pathway that repairs several different DNA oxidation defects.

Protonated molecular clusters: promoting molecular complexity

Abstract Molecules identified in Space display a diversity greater than ever, yet the mechanisms responsible for this complexity remain largely unknown. The extreme conditions faced by these molecules under astrophysical conditions raise several questions about their persistence and evolution. In this work, we explore the role of gas-phase protonated molecular dimers, which act both as protectors of existing molecules and as promotors in the emergence of new species. Experiments were conducted using the DIAM irradiation device on four protonated dimers of astrophysical interest, namely the pyridine, methanol, glycine pure dimers and the diglycine-glycine mixed dimer. Analysis of the observed relaxation channels following an energy deposition mimicking cosmic radiation reveals three main mechanisms of evaporation, covalent bond breaking, and unimolecular reaction. Focusing on the latter, our experiments combined with quantum chemical calculations of the relevant pathways shed new light onto the role of the protonation site on the reactants.

Granular metamaterials with dynamic bond reconfiguration.

Biological materials dynamically reconfigure their underlying structures in response to stimuli, achieving adaptability and multifunctionality. Conversely, mechanical metamaterials have fixed interunit connections that restrict adaptability and reconfiguration. This study introduces granular metamaterials composed of discrete bimaterial structured particles that transition between assembled and unassembled states through mechanical compression and thermal stimuli. These materials enable dynamic bond reconfiguration, allowing reversible bond breaking and formation, similar to natural systems. Leveraging their discrete nature, these materials can adaptively reconfigure their shape and respond dynamically to varying conditions. Our investigations reveal that these granular metamaterials can substantially alter their mechanical properties, like compression, shearing, and bending, offering tunable mechanical characteristics across different states. Furthermore, they exhibit collective behaviors like directional movement, object capture, transportation, and gap crossing, showcasing their potential for reprogrammable functionalities. This work highlights the dynamic reconfigurability and robust adaptability of granular metamaterials, expanding their potential in responsive architecture and autonomous robotics.

Computational Insights into Tunable Reversible Network Materials: Accelerated ReaxFF Kinetics of Furan-Maleimide Diels-Alder Reactions for Self-Healing and Recyclability.

In this study, ReaxFF molecular dynamics simulations were benchmarked and used to study the relative kinetics of the retro Diels-Alder reaction between furan and N-methylmaleimide. This reaction is very important for the creation of polymer networks with self-healing and recyclable properties, since they can be used as reversible linkers in the network. So far, the reversible Diels-Alder reaction has not yet been studied by using reactive molecular dynamics simulations. This work is, thus, the first step in simulating a covalent adaptable network (CAN) using Diels-Alder reactions as reversible linkers. For both endo and exo, the bond breaking in 40 product molecules was simulated using the bond boost method and the endo/exo ratio was evaluated. This ratio was benchmarked against density functional theory (DFT) and experimental results for a changing set of bond boost parameters. Given their importance to understand how the CAN performs, the effect of the addition of a polymer backbone and the effect of temperature were successfully simulated using our newly parametrized reactive force field.

Switchable Fluorescence of a Mechanical Stimulus-Responsive Au-P-S Complex.

The reaction of [(3-bdppmapy)(AuCl)2] with NaHmna (3-bdppmapy = N,N'-bis-(diphenylphosphanylmethyl-3-aminopytidine, H2mna = 2-mercaptonicotinic acid)) resulted in a tetranuclear Au-P-S complex [(3-bdppmapy)2(AuHmna)2(AuCl)2] (1) which emitted bright yellow fluorescence at 542 nm under 377 nm excitation (QY = 5.3%, τ = 0.83 ns). Upon grinding, the emission intensity of 1 significantly and rapidly decreased, but could be recovered by exposure to CH2Cl2 vapor. This switchable fluorescence is attributed to the breaking and reforming of intermolecular hydrogen bonds with concomitant collapse and the restoration of the crystalline phase, which is not caused by static pressure or increased temperature.

Hydrogen Production from Formic Acid Using KIT-6 Supported Non-NobleMetal-Based Catalysts.

The aim of this study is to investigate the activity of KIT-6 supported nickel (Ni) and cobalt (Co) catalysts, and the effect of Co incorporation to the Ni@KIT-6 catalyst in the formic acid (FA) dehydrogenation. Ni and Co are inexpensive and readily available non-noble transition metals that are considered ideal for dehydrogenation reactions due to their high activity against C-C and C-H bond breaking. In this study, KIT-6 supported catalysts were tested for hydrogen production from FA in a conventionally heated packed-bed continuous-flow system. N2 adsorption-desorption isotherms of the samples were found to be consistent with Type-IV according to the International Union of Pure and Applied Chemistry (IUPAC) classification. The introduction of metal loading resulted in the preservation of the mesoporous structure of the support material. X-ray diffraction (XRD) patterns of the catalysts exhibited the characteristic amorphous silica structure. Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFT) analysis, Lewis acidity of Co-based catalysts was found to be higher than the Ni-based catalysts. The complete formic acid conversion was observed at 200-350 °C. The highest H2 selectivity was obtained with the 3Ni@KIT-6 catalyst. The Co-based catalysts exhibited relatively lower catalytic activity, which was linked to increased coke formation within these catalysts.

Sustainable Immunomodulatory via Macrophage P2Y12 Inhibition Mediated Bioactive Patche for Peritendinous Antiadhesion.

Persistent anti-inflammatory responses are critical for the prevention of peritendinous adhesion. Although modified anti-adhesion barriers have been studied extensively, the immune response induced by the implants and the unclear mechanism limits their application. In this research, the advantage of the multi-functionalities of CA (caffeic acid) is taken to synthesize biodegradable poly (ester urethane) urea elastomers with ester- and carbamate-bonded CA (PEUU-CA). PEUU-CA is electrospun into bioactive patches that can uniquely present a sustained CA niche, referred to as BPSN. In the early stage of degradation, the breakage of the ester bond from BPSN is the dominant factor contributing to the early release of CA. In the later stage of BPSN degradation, the breakage of the ester and carbamate bonds contributes to the sustained release of CA. In vitro experiments showed that CA, when specifically bound to the P2Y12 receptor, down-regulated the expression and function of active P2Y12, effectively inhibiting the aberrant activation of macrophages and the secretion of inflammatory chemokines. BPSN addresses the foreign body reaction induced by macrophage-dominated biomaterial implantation and the issue of the short-term release of drugs at later stages of adhesion, providing a feasible strategy for the prevention and treatment of tissue adhesion, and more broadly, the well-known implant-derived inflammatory responses.

Quantum Mechanics/Molecular Mechanics Simulations for Chiral-Selective Aminoacylation: Unraveling the Nature of Life

Biological phenomena are chemical reactions, which are inherently non-stopping or “flowing” in nature. Molecular dynamics (MD) is used to analyze the dynamics and energetics of interacting atoms, but it cannot handle chemical reactions involving bond formation and breaking. Quantum mechanics/molecular mechanics (QM/MM) umbrella sampling MD simulations gives us a significant clue about transition states of chemical reactions and their energy levels, which are the pivotal points in understanding the nature of life. To demonstrate the importance of this method, we present here the results of our application of it to the elucidation of the mechanism of chiral-selective aminoacylation of an RNA minihelix considered to be a primitive form of tRNA. The QM/MM MD simulation, for the first time, elucidated the “flowing” atomistic mechanisms of the reaction and indicated that the L-Ala moiety stabilizes the transition state more than D-Ala, resulting in L-Ala preference in the aminoacylation reaction in the RNA. The QM/MM method not only provides important clues to the elucidation of the origin of homochirality of biological systems, but also is expected to become an important tool that will play a critical role in the analysis of biomolecular reactions, combined with the development of artificial intelligence.

Metal-Metalloid Modified C36 Fullerene: A Dual Role in Drug Delivery and Sensing for Anticancer Chlormethine Explored through DFT and MD Simulations.

Spurred by the latest developments and growing utilization of zero-dimensional (0D) drug delivery and drug sensors, this investigation examines the possibilities of the 0D C36 fullerene for drug delivery and the detection of the anticancer drug chlormethine (CHL), the overabundance of which poses a significant threat to living organisms. This study employs density functional theory and ab initio molecular dynamics (AIMD) simulations (AIMD) to evaluate and gain insights into the interaction mechanisms between pristine C36 fullerene, metal-metalloid (MM)-modified C36 fullerene (with Al, Fe, and B), and the anticancer drug CHL. It is observed that in the gas phase, the CHL drug molecule adsorbs onto the fullerenes in the following order: B-C36 > Fe-C36 > Al-C36 > C36. However, when considering the solvent effect, the adsorption energy of the CHL drug molecule on B-C36 increases, indicating chemisorption behavior. This implies that B-C36 could be a promising candidate for drug delivery applications, particularly for the CHL anticancer drug. In contrast, the adsorption energy of the CHL drug molecule on Fe-C36 decreases with the presence of the solvent, resulting in intermediate physisorption. Due to its minimal recovery time, excellent sensing response, intermediate physisorption, and shorter interatomic distance compared to C36 and Al-C36 fullerenes, Fe-C36 is well-suited as a drug sensor for CHL. AIMD simulations demonstrate that the B-C36/CHL and Fe-C36/CHL complexes are well-equilibrated and highly stable in the aqueous phase at 300 and 310 K respectively, with no evidence of bond breakage or formation. The structural stability observed, even with temperature fluctuations, indicates that the electrostatic interactions are robust enough to maintain cohesion of the fragments.

Pressure Effect on Surface Roughness of Gradient Chromium-doped Diamond-like Carbon Coatings under High Temperature

Abstract In this paper, the pressure effect of surface roughness of four gradient chromium-doped diamond-like carbon (GCD-DLC) coating is systemically studied in argon annealing and high pressure annealing under high temperature. After HIPping annealing, the surface roughness of the hydrogen-free group (GCr and GCrSi) decreased slightly. However, for the two hydrogen-containing GCD-DLC coatings (DCr and DCrSi), especially the DCr coating, the roughness increased significantly. The changes in surface roughness of the hydrogen-free group and the hydrogen-containing group after high-pressure annealing are opposite. The surface roughness of the DCr coating increased significantly after 500°C HIP annealing, which is attributed to the pores on the coating surface. Only the surface morphology of the DCr coating exhibited significant changes. Numerous voids appeared on the surface of the DCr5H coating after 500°C HIP annealing. There were significant differences in the size and shape of these voids compared to those after 500°C argon annealing. The voids on the coating after argon annealing were larger than those after HIP annealing. The formation of pores is associated with the breaking of carbon-hydrogen bonds and the subsequent release of hydrogen. This is because high pressure slows down the transformation from sp3 carbon bonds to sp2 carbon bonds. Simultaneously, high pressure also slows down the release of hydrogen within the coatings.

Humic acid promotes pathway of chloronitrobenzene cathodic reduction shunting from atomic H* to direct electron transfer

Progress mechanism of humic acid (HA) interacting with chloronitrobenzenes (ClNBs) and affecting their reduction and degradation was investigated. A two-stage chamber with graphite felt as cathode and anode was constructed, and 2,4-dichloronitrobenzene (2,4-DCNB) was target pollutant. Result showed that HA increased 36.15% of 2,4-DCNB removal efficiency at pH 5.0 after 4-h cathodic reduction, while at pH 7.0 and 10.0, it showed much less effect. Meanwhile, HA reduced cathodic H2 and atomic H* production via competing electron with H+. Combined with result of HA alleviating inhibition of tert-butyl alcohol on 2,4-DCNB removal, it was supposed that HA shunted dominant pathway of cathodic reduction of 2,4-DCNB from atomic H* to direct electron transfer (DET). This was proved by HA increasing electron transfer efficiency (k) of 2,4-DCNB reduction from 0.50±0.01 to 0.63±0.01, which indicated rate-limiting step of 2,4-DCNB reduction changed from electron transfer (ET) to bond breaking kinetics. HA-mediated DET pathway initially reduced nitro group, followed by dechlorination, while atomic H* pathway was randomly dechlorinated and nitro reduced. The pH significantly affected agglomeration of HA and 2,4-DCNB. Molecular dynamics simulation showed that hydrogen bond and Van der Waals force dominated agglomeration of HA and 2,4-DCNB in acidic condition, while electrostatic force was main driving force in alkaline condition. Less effect of HA on 2,4-DCNB removal efficiency at high pH could be related to its reduced conductivity and weaker molecular interactions with 2,4-DCNB. This study provides comprehensive insight into role and impact of HA in remediation of ClNBs-contaminated sediment and water by (bio)electrochemical technology.

Cysteine-induced disulfide cleavage enhances the solubility of alkali-treated pea protein and its elasticity contribution in low-salt hybrid meat gels.

This study investigated the effectiveness of cysteine in improving the functional properties of pea proteins within low-salt myofibrillar protein (MP) gels. Cysteine treatment, at a concentration of 3.3mM/g protein, cleaved 71-82% of the disulfide bonds in native and pH-shifted pea protein isolates (PPIN and PPIpH), which increased the solubility and hydrophobicity of PPIpH. PPIN showed slight changes, primarily an increase in tryptophan fluorescence. The cleavage of disulfide bonds improved the hardness, elastic component (G'), and network integrity of hybrid gels. When combined with transglutaminase, the MP+PPIpH gel reached its maximum hardness (0.38N) at a cysteine concentration of 1.7mM/g protein. SDS-PAGE patterns and gels treated with additional N-ethylmaleimid confirmed the involvement of cysteine-treated PPI in the gel matrix. Consequently, cysteine-mediated disulfide bond disruption effectively modifies pea proteins, rendering them a more suitable functional ingredient for enhancing the texture of low-salt meat products.

Above-Room-Temperature Ferromagnetism Regulation in Two-Dimensional Heterostructures by van der Waals Interfacial Magnetochemistry.

Most methods for regulating physical and chemical properties of materials involve the breaking and formation of chemical bonds, which inevitably change local structures. Two-dimensional (2D) ferromagnets are critical for spintronic memory and quantum devices, but most of them maintain ferromagnetism at low temperature, and multiaspect control of 2D ferromagnetism at room temperature or above is still missing. Here, we report a nondestructive, van der Waals (vdW) interfacial magnetochemistry strategy for above-room-temperature, multiaspect 2D ferromagnetism regulation. By vdW coupling nonmagnetic MoS2, WSe2, or Bi1.5Sb0.5Te1.7Se1.3 with 2D vdW ferromagnet Fe3GaTe2, the Curie temperature is enhanced up to 400 K, best for 2D ferromagnets, with 26.8% tuning of room-temperature perpendicular magnetic anisotropy and an unconventional anomalous Hall effect up to 340 K. These phenomena originate from changes in magnetic exchange interactions and magnetic anisotropy energy by interfacial charge transfer and spin-orbit coupling. This work opens a pathway for engineering multifunctional 2D heterostructures by vdW interfacial magnetochemistry.

Microscopic deformation mechanism of inelasticity in graphene foams under quasi-static tension and compression

The unique porous structure and exceptional elasticity of graphene foams (GrFs) qualify them as prime candidates for various applications. However, the claim of their super-elasticity under compressive strains up to 90% is ambiguous, as the super-elastic behavior is accompanied by inelastic phenomena such as plasticity and microscale damage. This study systematically investigated the microscopic deformation mechanisms underlying the inelasticity of GrFs under both tension and compression using numerical experiments based on the coarse-grained molecular dynamics method. The “non-uniformity of deformation” parameter is proposed, and it revealed a two-stage deformation process characterized by nonlocalized and localized inelasticity. When the GrFs were subjected to tensile strains below a critical threshold, irreversible microstructural deformation resulted in nonlocalized inelasticity. Beyond this threshold, inelasticity was predominantly driven by localized plastic deformation and damage caused by bond breakages at the fracture interface. In contrast, only nonlocalized inelasticity occurred during the compression process. Furthermore, the results indicated that when nonlocalized inelasticity occurred, a negative correlation between the crosslink densities and the number of graphene layers existed. These results can deepen our understanding of the deformation properties of GrFs, which is crucial for their design and application.