Amorphous Research Articles

Understanding the role played by Cu nanoparticles embedded in situ in a carbonaceous matrix as sulfur host for lithium-sulfur batteries

The lithium-sulfur (Li-S) battery is a promising alternative to Li-ion batteries as an energy storage system, owing to its higher capacity and specific energy values. To tackle its intrinsic problems, the element copper (Cu) is an attractive option given both its excellent conductivity and its ability to interact with highly reactive polysulfides. Here, we propose the use of a carbon/copper composite (90.5:9.5 wt ratio) obtained by thermal decomposition of a single precursor based on a Cu(II) oleate/oleic acid complex and eliminating the use of H2 as a reducing agent as commonly reported. Cu nanoparticles (mean particle size around 15 nm in diameter) which are highly dispersed on an amorphous carbon matrix derived from an organic framework, enhance both the conductivity and the ability for the chemical adsorption of lithium polysulfides (LiPSs), and thus increasing the reaction efficiency. Poor cycling stability, less specific capacity, and diminished rate capability were observed when the Cu content was reduced to around 70 % through treatment with concentrated nitric acid. This confirms the electrocatalytic role of the metal.

Utilizing molecular simulation, ideal adsorbed solution theory and ensemble learning algorithms to investigate adsorption and separation of sulfides on amorphous nanoporous materials

Using grand canonical Monte Carlo method, we investigated the adsorption of pure H2S and SO2 gases on amorphous materials, and the separation of CH4-H2S and CO2-SO2 mixtures. At 303 K, the optimal adsorbent for both gases was found to be HCP-Colina-id016, with 16 mmol/g. For CH4-H2S mixture, despite aCarbon-Marks-id002 exhibiting the highest selectivity (approximately 80), the H2S adsorption was low (around 1 mmol/g), while Kerogen-Coasne-id013 demonstrated a high H2S adsorption of 12 mmol/g with a selectivity of 20. In the case of CO2-SO2, HCP-Colina-id018 exhibited a SO2 selectivity exceeding 30, with a high SO2 adsorption of 12 mmol/g. The Ideal Adsorbed Solution Theory underestimated the adsorption and selectivity of both mixtures, particularly evident in CO2-SO2. Molecular simulations revealed that, for the CO2-SO2 system, CO2 underwent condensation, resulting in a sudden drop in the SO2 adsorption isotherm. However, IAST accurately predicted this abrupt change. Based on the adsorption data obtained from molecular simulations, we compared the predictive performance of four ensemble learning algorithms, namely Random Forest (RF), Gradient Boosted Decision Trees (GBDT), Extreme Gradient Boosting (XGBoost), and CatBoost, for H2S and SO2 pure gases in amorphous porous materials. The rankings were observed to be XGBoost > GBDT > RF > CatBoost.

Nanocrystallization tuning of structural, thermoelectric and electrical properties of SrTiO3-doped vanadate glasses

Glass-ceramic nanocrystals (GCNs) were obtained by annealing parent SrTiO3-V2O5 (SV) glasses prepared using the melt-quenching technique at the crystallization temperature, Tc. The amorphous nature and glassy behavior of the quenched glasses were confirmed by XRD, DSC and FTIR spectroscopy. In the heat-treated samples, the crystal size was found to range from 40 to 80 nm for all studied samples. It was observed that as the SrTiO3 content in the GCNs increased, density (d) steadily rose. The change of vanadium ions concentration(C) has the predominant role for changing Seebeck coefficient in both glass and GCNs samples. The nanocrystallization process at temperatures close to the onset of Tc, lasting for one hour, notably increased the electronic conductivity of the initial glasses. Consequently, the modification in nanostructure resulted in enhanced conductivity. In comparison to the original glasses, the final materials demonstrated significantly improved electrical conductivity. The accumulation of V4+-V5+ pairs at the formed interlayer zones between nanocrystallites and the glassy phase is accountable for electron hopping in the current system, which is markedly higher than in the glassy matrix. The formed nanocrystallites play a crucial role in augmenting the conductivity of such nanomaterials. The maximum obtained value of the power factor (PF) is 0.9 × 10−4 mW/mk2 for the glass sample (x = 20) reflecting a very low thermoelectric power conversion efficiency while in GCNs, the PF values were well-enhanced to 0.6 mW/m.K2 at x = 20.

Structural mechanism of glass transition uncovered by unsupervised machine learning

Uncovering the structural origins of the ubiquitous dynamic arrest phenomenon at the glass transition has long been a challenge due to the difficulty in identifying a rational structural representation from a disordered medium. To address this challenge, we propose a novel approach based on unsupervised learning to define a set of structural fingerprints. In this approach, complex local atomic environments, ranging from short to medium range, are captured by the discretized radial distribution function and projected onto a simple two-dimensional space using a neural network-based autoencoder. This two-dimensional space is characterized by two static structural indicators, P1 and P2, providing a comprehensive and user-friendly representation of the mysterious “glassy structure”. By employing Gaussian mixture modeling, the structural space is autonomously divided into three sections, each representing a unique cluster with similar environments. These indicators not only elucidate the glass transition but also allow for the quantitative prediction of activation barriers for local structural excitations. Furthermore, the unsupervised clustering technique can distinguish between the structural features of “hard zones” and “soft zones”, as well as recently proposed superfast “liquid-like” atoms in glass. This unsupervised machine learning approach demonstrates the utility of seemingly agnostic local structure in amorphous materials, offering insights into the long-sought structural origins of the glass transition.

Magnesite formation during nesquehonite decomposition in the presence and absence of retained self-generated gases and the role of X-ray amorphous materials as essential stores for CO2

Magnesite formation during nesquehonite decomposition in the presence and absence of retained self-generated gases and the role of X-ray amorphous materials as essential stores for CO2

Nonplanar Nanographene: A Hydrocarbon Hole-Transporting Material That Competes with Triarylamines.

Hole-transporting materials (HTMs) are essential for optoelectronic devices, such as organic light-emitting diodes (OLEDs), dye-sensitized solar cells, and perovskite solar cells. Triarylamines have been employed as HTMs since they were introduced in 1987. However, heteroatoms or side chains embedded in the core skeleton of triarylamines can cause thermal and chemical stability problems. Herein, we report that hexabenzo[a,c,fg,j,l,op]tetracene (HBT), a small nonplanar nanographene, functions as a hydrocarbon HTM with hole transport properties that match those of triarylamine-based HTMs. X-ray structural analysis and theoretical calculations revealed effective multidirectional orbital interactions and transfer integrals for HBT. In-depth experimental and theoretical analyses revealed that the nonplanarity-inducing annulative π-extension can achieve not only a stable amorphous state in bulk films, but also a higher increase in the highest occupied molecular orbital level than conventional linear or cyclic π-extension. Furthermore, an in-house manufactured HBT-based OLED exhibited excellent performance, featuring superior curves for current density-voltage, external quantum efficiency-luminance, and lifetime compared to those of representative triarylamine-based OLEDs. A notable improvement in device lifetime was observed for the HBT-based OLED, highlighting the advantages of the hydrocarbon HTM. This study demonstrates the immense potential of small nonplanar nanographenes for optoelectronic device applications.

Nonplanar Nanographene: A Hydrocarbon Hole‐Transporting Material That Competes with Triarylamines

AbstractHole‐transporting materials (HTMs) are essential for optoelectronic devices, such as organic light‐emitting diodes (OLEDs), dye‐sensitized solar cells, and perovskite solar cells. Triarylamines have been employed as HTMs since they were introduced in 1987. However, heteroatoms or side chains embedded in the core skeleton of triarylamines can cause thermal and chemical stability problems. Herein, we report that hexabenzo[a,c,fg,j,l,op]tetracene (HBT), a small nonplanar nanographene, functions as a hydrocarbon HTM with hole transport properties that match those of triarylamine‐based HTMs. X‐ray structural analysis and theoretical calculations revealed effective multidirectional orbital interactions and transfer integrals for HBT. In‐depth experimental and theoretical analyses revealed that the nonplanarity‐inducing annulative π‐extension can achieve not only a stable amorphous state in bulk films, but also a higher increase in the highest occupied molecular orbital level than conventional linear or cyclic π‐extension. Furthermore, an in‐house manufactured HBT‐based OLED exhibited excellent performance, featuring superior curves for current density–voltage, external quantum efficiency–luminance, and lifetime compared to those of representative triarylamine‐based OLEDs. A notable improvement in device lifetime was observed for the HBT‐based OLED, highlighting the advantages of the hydrocarbon HTM. This study demonstrates the immense potential of small nonplanar nanographenes for optoelectronic device applications.

Heat- and shock-induced pyrolysis of crystalline and amorphous TNT revealed by ReaxFF-lg simulations

The decomposition mechanisms of crystalline and amorphous TNT were studied through ReaxFF-lg simulations under the heat-loaded and shock-loaded. Their differences were elucidated from the initial decay reactions, activation energy, products and the clusters. Results showed that the heat-induced pyrolysis of two systems differed slight, but the shock-induced pyrolysis differed large. The decomposition reactions of amorphous and crystalline models are similar, but the nitro oxidation of TNT is only found in amorphous. Dimerization and intermolecular H-transfer were found at the constant temperature and MSST simulations, and intermolecular O-transfer were only found at the constant temperature simulations. For MSST simulation, products in crystalline formed later than in amorphous, and the number of clusters in crystalline is much larger than in amorphous, which indicating crystalline TNT would be induced early through shock wave. These findings could help to increase the understanding for the thermolysis behavior and safety of crystalline and amorphous energetic materials.

Measuring Oxygen Solubility in Amorphous and Semicrystalline Polyolefins Using Test Particle Insertion: A Comparative Study of Polyethylene and Isotactic Polypropylene.

The test particle insertion method is used to study the solubility of oxygen in two commonly used polymers: polyethylene (PE) and isotactic polypropylene (iPP). Amorphous samples for both polymers were prepared by means of Monte Carlo and molecular dynamics simulations, and the oxygen solubility was measured across different temperatures. The solubility-temperature dependence for iPP proved to be nonmonotonic due to the interplay between binding and reorganizational enthalpy, while for PE, it appeared to be monotonic based on the available data in the studied temperature range. A broad comparison to experiments and simulations is included. Further oxygen insertions were also performed in semicrystalline PE and iPP samples at ambient temperature, and the obtained values were compared to a linear relationship which correlates the solubility in the purely amorphous phase with the solubility in the crystalline phase. The solubility of PE closely follows the linear relationship, while iPP exhibits some divergence. All the semicrystalline samples were previously annealed at elevated temperatures for long periods (a few μs), and a strong effect of annealing was observed on the structure and the solubility of iPP. A well-developed iPP lamellar structure emerged at longer annealing times, while PE develops that structure already in the early crystallization stages. The solubility of semicrystalline iPP samples with lamellar morphology exhibited better agreement with extrapolated solubility values of the amorphous state─the extrapolation was made using a linear relationship connecting solubility in the purely amorphous phase and solubility in mixed phases (amorphous and crystalline). Results on the correlation of the solubility with the local structural ordering are also present.

Precision Self‐Assembly of Supramolecules with Heterogeneous Derivatives

AbstractSupramolecular self‐assembly with well‐defined building blocks like lipids, deoxyribonucleic acid, or ligands relies on accessible molecular structures and predictable interactions. However, assembling heterogeneous, undefined blocks, such as disordered proteins, amorphous solids, and catecholic derivatives, remains challenging due to their unpredictable assembly, leading to irreversible aggregation, severe precipitation, and unreliable performance. Here, the first programmable, sustainable, and durable self‐assembly strategy of supramolecules with heterogenous is presented, derived blocks via harmonizing multiple molecular interactions. This approach achieves reversible assembly/disassembly, ≈73.7% reduced precipitation, and salt‐ and alkaline‐durability under freeze‐thaw cycles in model catecholic derivatives, functioning effectively as robust adhesive primers and hydrogel interfacial strengtheners. Moreover, through molecular force measurements and computational simulations, the first general criterion and benchmark for high precision supramolecular self‐assembly is proposed, applicable to complex derivatives and interactions: with blocks bearing multiple binding sites existing, the co‐assembling blocks should bear at least two binding sites with minimum binding strength (≈17 to ≈37 kJ mol−1) to prevent disassembly. This study paves the way and provides benchmarks for precision self‐assembly of diverse supramolecules using heterogeneous derivatives for adhesion technology, nanomaterial synthesis and bio‐inspired applications.

Nanomechanical Crystalline AlN Resonators with High Quality Factors for Quantum Optoelectromechanics.

High-quality factor (Qm) mechanical resonators are crucial for applications where low noise and long coherence time are required, as mirror suspensions, quantum cavity optomechanical devices, or nanomechanical sensors. Tensile strain in the material enables the use of dissipation dilution and strain engineering techniques, which increase the mechanical quality factor. These techniques have been employed for high-Qm mechanical resonators made from amorphous materials and, recently, from crystalline materials such as InGaP, SiC, and Si. A strained crystalline film exhibiting substantial piezoelectricity expands the capability of high-Qm nanomechanical resonators to directly utilize electronic degrees of freedom. In this work, nanomechanical resonators with Qm up to 2.9 × 107 made from tensile-strained 290 nm-thick AlN are realized. AlN is an epitaxially-grown crystalline material offering strong piezoelectricity. Nanomechanical resonators that exploit dissipation dilution and strain engineering to reach a Qm × fm-product approaching 1013 Hz at room temperature are demonstrated. A novel resonator geometry is realized, triangline, whose shape follows the Al-N bonds and offers a central pad patterned with a photonic crystal. This allows to reach an optical reflectivity above 80% for efficient coupling to out-of-plane light. The presented results pave the way for quantum optoelectromechanical devices at room temperature based on tensile-strainedAlN.

Thermoelastic fracture of two-dimensional hexagonal quasicrystal media weakened by a penny-shaped crack subjected to uniformly antisymmetric heat fluxes

This study focuses on the thermoelastic fracture behavior of quasicrystals, a class of solids that exhibit unique properties between traditional crystals and amorphous materials. The complex atomic structure of quasicrystals poses challenges in understanding their fracture mechanisms under thermoelastic loading conditions. Central to our investigation is an analytical examination of a penny-shaped crack in an infinite three-dimensional body composed of two-dimensional hexagonal quasicrystals, where the upper and lower crack surfaces are applied to a pair of uniformly antisymmetric heat fluxes. This crack problem requires simultaneous consideration of thermal-phason-phonon multiple field coupling. According to the symmetry of field variables with respect to the crack plane, the thermal-phason-phonon coupled crack problem is transformed into a mixed boundary value problem in the upper half space. The extended displacement discontinuities, encompassing both phonon and phason displacement discontinuities, as well as the temperature discontinuity, are chosen as the basic unknown variables to construct the boundary integral-differential equations governing the mixed boundary value problem. Based on these boundary governing equations and Fabrikant's potential theory method, the problem with the crack surface subjected to uniform antisymmetric heat fluxes is solved. The solutions of thermal-phason-phonon fields on the crack plane, and in the full space are given in closed-form. Numerical results are employed to validate the obtained analytical solutions and visually illustrate the spatial distribution of thermal-phonon-phason coupling fields in the vicinity of the crack. The study provides fundamental insights into the behavior of cracks in quasicrystals under thermal loading, with potential implications for the design of new materials and structures.

Nanoporous amorphous carbon nanopillars with lightweight, ultrahigh strength, large fracture strain, and high damping capability

Simultaneous achievement of lightweight, ultrahigh strength, large fracture strain, and high damping capability is challenging because some of these mechanical properties are mutually exclusive. Here, we utilize self-assembled polymeric carbon precursor materials in combination with scalable nano-imprinting lithography to produce nanoporous carbon nanopillars. Remarkably, nanoporosity induced via sacrificial template significantly reduces the mass density of amorphous carbon to 0.66 ~ 0.82 g cm−3 while the yield and fracture strengths of nanoporous carbon nanopillars are higher than those of most engineering materials with the similar mass density. Moreover, these nanopillars display both elastic and plastic behavior with large fracture strain. A reversible part of the sp2-to-sp3 transition produces large elastic strain and a high loss factor (up to 0.033) comparable to Ni-Ti shape memory alloys. The irreversible part of the sp2-to-sp3 transition enables plastic deformation, leading to a large fracture strain of up to 35%. These findings are substantiated using simulation studies. None of the existing structural materials exhibit a comparable combination of mass density, strength, deformability, and damping capability. Hence, the results of this study illustrate the potential of both dense and nanoporous amorphous carbon materials as superior structural nanomaterials.

Mechanical Memories in Solids, From Disorder to Design

Solids are rigid, which means that when left undisturbed, their structures are nearly static. It follows that these structures depend on history—but it is surprising that they hold readable memories of past events. Here, we review the research that has recently flourished around mechanical memory formation, beginning with amorphous solids’ various memories of deformation and mesoscopic models based on particle rearrangements. We describe how these concepts apply to a much wider range of solids and glassy matter, and how they are a bridge to memory and physical computing in mechanical metamaterials. An understanding of memory in all these solids can potentially be the basis for designing or training functionality into materials. Just as important is memory's value for understanding matter whenever it is complex, frustrated, and out of equilibrium.

Electrospun patches to deliver combination drug therapy for fungal infections

Fungal infections, though affecting healthcare globally, receive insufficient attention in clinical and academic settings. Invasive fungal infections, particularly caused by combat wounds, have been identified as a critical threat by the US Department of Defense. Monotherapy with traditional antifungals is often insufficient, and so combination therapies are explored to enhance treatment efficacy. However, systemic combination treatments can result in severe adverse effects, suggesting the need for localised delivery systems, such as drug-loaded electrospun patches, to administer antifungals directly to the infection site. This proof-of-concept study hypothesised that dual amorolfine and terbinafine therapy slowly releasing from electrospun patches would be an effective way of eradicating Candida albicans when the patch was applied directly to the fungal colony. The feasibility of creating electrospun materials loaded with amorolfine and terbinafine for combination antifungal therapy was investigated. Electrospinning was used to fabricate polycaprolactone (PCL) patches with varying drug loadings (2.5%, 5%, and 10% w/w) of amorolfine and terbinafine either individually or in combination. The incorporation of both drugs in the fibres was confirmed, with the drugs predominantly in an amorphous state. Results showed that combination therapy patches had a significantly greater and prolonged antifungal effect compared to monotherapy patches, with larger zones of inhibition and sustained efficacy over at least 7 days. This study therefore demonstrates that PCL-based electrospun patches containing amorolfine and terbinafine provide superior antifungal activity against C. albicans compared to monotherapy patches. This approach could lower required drug doses, reducing adverse effects, and enhance patient compliance due to prolonged drug release, leading to more effective antifungal therapy.

Ferroelastic ionic organic crystals that self-heal to 95%

The realm of self-healing materials integrates chemical and physical mechanisms that prevent wear and fracturing and extend the operational lifetime. Unlike the favorable rheology of amorphous soft materials that facilitates efficient contact between fragments, the efficiency of recovery of atomistically ordered materials is restricted by slower interfacial mass transport and the need for ideal physical alignment, which limits their real-world application. We report drastic enhancements in efficiency and recovery time in the self-healing of anilinium bromide, challenging these limitations. Crystals of this material recovered up to 49% within seconds and up to 95% after 100 min via ferroelastic detwinning. The spatial evolution of strain during cracking and healing was measured in real time using digital image correlation. Favorable alignment and strong ionic bonding across the interface of partially fractured crystals facilitate self-healing. This study elevates organic crystals close to the best-in-class self-healing polymers and sets an approach for durable crystal-based optoelectronics.

Effect of alumina on formation mechanism and structure characteristic of sodium calcium silicate compounds with different stoichiometric coefficients

In order to illustrate the effects of Al2O3 on silicate structure for synthesizing sodium calcium silicate compounds, the formation characteristics, lattice parameters, molecular structure and element chemical state of sodium calcium silicates with different Al2O3 proportions through solid-state reaction were investigated using XRD, SEM-EDS, Raman spectroscopy and XPS analyses. Increasing the Al2O3 content facilitates the formation of Na2CaSiO4 and converts the polymorph of Na2Ca6Si4O15 from γ-type into β-type. The product particles aggregate to form clumps by increasing the Al2O3 content when the molar ratios of Na2O and CaO to SiO2 are 0.5 and 1.5, and the network orderliness of silicates deteriorates to form glassy phase at the low CaO and Na2O contents. Al2O3 can engage in the bonding process with silicate crystals to produce a finite solid solution. Increasing the Al2O3 porportion is advantageous for facilitating the participation of [AlO6] in the Si-O-Al bonding reaction, which leads to the depolymerization of [Si2O7]6-, [Si3O10]8- and [Si6O18]12− and promotes the formation of silicate chains of [SiO4]4- and [Si2O7]6-. Moreover, increasing the contents of Na2O and CaO promote the formation of [AlO4] and the depolymerization within silicate chains, which increases the bonding number of Si-Oter and Al-Oter and then reduces the binding energies of Si2p and Al2p orbits.

Synergistic Effects of Radical Distributions of Soluble and Insoluble Polymers within Electrospun Nanofibers for an Extending Release of Ferulic Acid.

Polymeric composites for manipulating the sustained release of an encapsulated active ingredient are highly sought after for many practical applications; particularly, water-insoluble polymers and core-shell structures are frequently explored to manipulate the release behaviors of drug molecules over an extended time period. In this study, electrospun core-shell nanostructures were utilized to develop a brand-new strategy to tailor the spatial distributions of both an insoluble polymer (ethylcellulose, EC) and soluble polymer (polyvinylpyrrolidone, PVP) within the nanofibers, thereby manipulating the extended-release behaviors of the loaded active ingredient, ferulic acid (FA). Scanning electron microscopy and transmission electron microscopy assessments revealed that all the prepared nanofibers had a linear morphology without beads or spindles, and those from the coaxial processes had an obvious core-shell structure. X-ray diffraction and attenuated total reflectance Fourier transform infrared spectroscopic tests confirmed that FA had fine compatibility with EC and PVP, and presented in all the nanofibers in an amorphous state. In vitro dissolution tests indicated that the radical distributions of EC (decreasing from shell to core) and PVP (increasing from shell to core) were able to play their important role in manipulating the release behaviors of FA elaborately. On one hand, the core-shell nanofibers F3 had the advantages of homogeneous composite nanofibers F1 with a higher content of EC prepared from the shell solutions to inhibit the initial burst release and provide a longer time period of sustained release. On the other hand, F3 had the advantages of nanofibers F2 with a higher content of PVP prepared from the core solutions to inhibit the negative tailing-off release. The key element was the water permeation rates, controlled by the ratios of soluble and insoluble polymers. The new strategy based on core-shell structure paves a way for developing a wide variety of polymeric composites with heterogeneous distributions for realizing the desired functional performances.

Poly(butylene 2,5-thiophenedicarboxylate-co-glycolate) copolyesters with good degradation and barrier properties

In this work, poly(butylene 2,5-thiophenedicarboxylate-co-glycolate) (PBTFGA) copolyesters were synthesized from 2,5-thiophenedicarboxylic acid, 1,4-butanediol and glycolic acid. The influence of the glycolic acid content on thermal properties, mechanical properties and degradation capacity of copolyesters was systematically investigated. The glass transition temperature of copolyesters closely matched that of poly(butylene 2,5-thiophenedicarboxylate) (PBTF). While also demonstrating good thermal stability. When the glycolic acid content was low, the copolyesters exhibited some crystallization capability, but they gradually became fully amorphous as the glycolic acid content increased. The tensile tests revealed that the young's modulus of the PBTFGA copolyesters ranged from 69.2 MPa to 221.4 MPa. With elongation at break exceeding 659%, outperforming most biodegradable packaging materials. Copolyesters exhibited excellent gas barrier properties to both oxygen (PO2 = 0.024 barrer) and carbon dioxide (PCO2 = 0.029 barrer), both of which are superior to poly(butylene 2,5-thiophenedicarboxylate). The incorporation of glycolic acid significantly reduced the crystalline content of the copolyesters, facilitating the interaction of water molecules with ester bonds in the polymer backbone. The weight of poly(butylene 2,5-thiophenedicarboxylate-co-glycolate) was decreased significantly during enzymatic hydrolysis, indicating excellent degradation performance

Low-temperature magnetic refrigeration in Gd20Tb20Er20Al20M20 (M = Fe, Co) high-entropy metallic glasses

This paper focuses on the magnetocaloric effect (MCE) of Gd20Tb20Er20Al20M20 (M = Fe, Co) high-entropy metallic glasses (HE-MGs). XRD and TEM results indicate that both HE-MGs are amorphous. Magnetic studies show that both HE-MGs display spin-glass behavior, undergo a second-order phase transition from ferromagnetic to paramagnetic, and exhibit soft magnetic properties at the Curie temperature (TC). Notable large and broad table-like magnetic entropy change characteristics of Gd20Tb20Er20Al20Fe20 (Gd20Tb20Er20Al20Co20) appear near a TC of 92 (51) K. Hence, under 7 T magnetic field, |-∆SMmax|, ∆ TFWHM, and RCP are 7.83 (10.10) J·kg-1·K-1, 120.07 (71.88) K, and 1008.26 (805.70) J·kg-1, respectively. Furthermore, the modulation of the magnetic and magnetocaloric properties of the samples after substitution of Fe for Co was revealed by the intricate 3d-3d and 3d-4f exchange interactions within the system. The magnetic phase transition critical behaviors in both HE-MGs were analyzed using the scaling law to clarify the deviation of amorphous materials from the mean-field theory. Thus, this study not only highlights the potential of this material for low-temperature magnetic refrigeration applications, but also expands our understanding of its physical properties.