Heavy Metal Atoms Research Articles

Full spin polarization and pure spin current produced by the photogalvanic effect in penta-PdN2 photodetector

The photogalvanic effects (PGEs) in low-dimensional devices were thought to be an important mechanism to generate pure spin current which was a essential problem in spintronics. Herein, based on non-equilibrium Green’s function combined with density functional theory, we studied linear and elliptical spin dependent PGEs in the photodetector based on the penta-PdN2 monolayer at zero bias. Due to spin-orbit coupling originating from the heavy metal atoms Pd and low symmetry of C2v for the pristine case and Cs for the defect cases, the penta-PdN2 photodetector at pristine, vacancy and substitution-doping situations can produce robust spin dependent PGEs, and the import of defects were able to strengthen the linear and elliptical PGEs, respectively. More importantly, on account of enormous splitting of the DOS for the pristine, Pd-vacancy, N2-vacancy and NN-vacancy cases, spin up and spin down photocurrents accordingly formed spin splitting, which eventually led to full spin polarization and then pure spin currents in the penta-PdN2 photodetector. PdSe2 monolayer has been compounded in experiments, so structurally similar penta-PdN2 monolayer possesses highly possible to be prepared. Therefore, if the penta-PdN2 photodetector can be successful assembled, the spin-generator will be reality, even no need to be doped because the pristine penta-PdN2 photodetector can give rise to pure spin currents. In addtion, the penta-PdN2 photodetector at different situations are highly polarization sensitive. In conclude, our work suggested great potential applications of the penta-PdN2 monolayer on PGE-driven low energy-consumption photodetectors and spin-generators in optoelectronics and spintronics.

Vibrational heavy atom effect on relaxation and solvent shell dynamics in group VIII trimetallic carbonyls.

Infrared pump-probe and two-dimensional infrared (2D-IR) spectroscopies were used to study the vibrational dynamics of a homologous set of trimetallic dodecacarbonyls with increasingly heavy atomic masses in tetrahydrofuran solution. The vibrational lifetimes showed some evidence of the vibrational heavy atom effect (VHAE) but were not consistent across the sample set. Spectral diffusion was measured by 2D-IR spectroscopy to investigate whether the changes produced by the VHAE had influenced other aspects of vibrational dynamics. The triiron species was found to be more dynamic on very fast timescales and may exhibit evidence of a transient bridging CO structure. Centerline slope analysis of the high-frequency CO peak for each complex revealed that the vibrational dynamics were subtly but consistently slowed for the compounds with heavier metal atoms.

Adsorption mechanisms of heavy metal atoms As, Pb, and Zn on thermally activated palygorskite Si–O/Mg–O (200) surfaces: A first-principles calculations

Heavy metal pollution on air, water, and soil is an issue of increasing global concern. Adsorption is widely recognized as one of the most effective methods for removing heavy metal pollution. The adsorption mechanisms of As (Arsenic), Pb (Lead), and Zn (Zinc) atoms on thermally activated palygorskite Si–O (200) and Mg–O (200) surfaces were investigated using first-principles calculations based on DFT. The coverage dependence of the adsorption configurations and energies on the most stable adsorption sites was also analyzed. The bridge site was found to be the most stable adsorption site for As and Pb on the Si–O (200) surface, while the adsorption energy of Zn was ＜ 0.1 eV on the surface. The adsorption capacity order of the surface was As > Pb ≫ Zn. On the Mg–O (200) surface, the hollow site was the most stable site for three heavy metal atoms. The adsorption energies of them gradually decreased with increasing coverage, thus indicating the lower stability of surface adsorption due to the repulsion of neighboring heavy metal atoms. The adsorption capacity of the Mg–O (200) surface followed the order of As > Pb > Zn. Further exploration was performed on the changes in structure and electronic properties within the adsorption process by studying the lattice relaxation, Bader charge, and electronic density of states (DOS) of the thermally activated palygorskite (200)/heavy metal atoms system.

Crystal phase conversion of amorphous Fe−Mn binary oxides promote the sequestration and redistribution of arsenic, cadmium, and lead in the soil: Comparison with crystalline form

Iron and manganese oxides participate in nearly all geochemical processes in soils. The crystal phase conversion of the Fe−Mn oxides is a crucial process that controls the transport and the fate of metal(loid)s (such as Pb, Cd, and As). However, this conversion and its contribution in immobilization are seldom reported. In this study, the phase transition process of amorphous Fe−Mn oxides has been investigated using TEM, HE−XRD and PDF analyses. The role of heavy metal atoms in the Fe−Mn oxides lattice has been revealed through atomic−scale structural characterization, including bond lengths and coordination numbers. In detail, Mn oxides and Fe oxides exhibit synergistic effects. Mn oxides oxidize As(III) to As(V). Meanwhile, the adsorbed As, Cd, and Pb irons were redistributed and incorporated into the lattice of the Fe−Mn oxides during the crystal phase conversion of the Fe oxides. During this process, the proportion of residual fraction of As, Cd, and Pb increased by 30 %, 25 %, and 9 %, respectively, after 28 d. 100 %, 41.8 %, and 60.7 % of decarbonate−extractable As, DTPA−extractable Cd and Pb could be immobilized, respectively. This study provides insight into the contribution of Fe−Mn oxides in controlling the cycling of metals and offers an advanced strategy in remediation of As, Cd, and Pb in contaminated soil.

Atomic-Scale Imaging of Clay Mineral Nanosheets and Their Supramolecular Complexes through Electron Microscopy: A Supramolecular Chemist's Perspective.

Recent advancements in electron microscopy techniques have revolutionized the ability to directly visualize and understand the intricate world of supramolecular chemistry. This paper provides a concise overview of a study delving into the atomic-scale imaging of monolayer clay mineral nanosheets and their associated supramolecular complexes. The imaging is conducted by harnessing the power of aberration-corrected scanning transmission electron microscopy (STEM). Clay mineral nanosheets, with their anionic charge and ultrathin thickness (of 1 nm), serve as a stable Coulombic host material for cationic guest molecules through electrostatic interactions, facilitating exceptional stability and control during observation. By incorporation of heavy-metal atom markers coordinated within the target molecules, high-angle annular dark field STEM enables a clear visualization of these supramolecular complexes. This approach helps to overcome the limitations of graphene-based systems and expands the possibilities of atomic-scale imaging of nonperiodic molecular assemblies formed by weak supramolecular interactions. The fusion of electron microscopy techniques with the principles of supramolecular and material chemistry offers exciting opportunities for studying the structure, behavior, and properties of complex supramolecular systems. It sheds light on the intricate molecular architectures and design principles governing these systems. This study showcases the immense potential of electron microscopy in supramolecular chemistry and invites researchers from various disciplines to explore the transformative possibilities of atomic-scale imaging in the field.

Organic ferroelastic enantiomers with high Tc and large dielectric switching ratio triggered by order-disorder and displacive phase transition

Molecular-based ferroelastics with dielectric switching properties are highly desirable for their applications on microelectronic dielectric switches, sensors, data storage, and so on. However, the current reports mostly focus on organic-inorganic hybrids containing toxic heavy metal atoms, and the relatively low phase transition temperature limits their application. In this paper, low-toxic organic salt ferroelastic enantiomers (R/S)-4-fluoro-1-azabicyclo[3.2.1]octonium chloride [(R/S)-F-321] were designed and synthesized under the introducing chirality strategy. They undergo a 432F422-type ferroelastic phase transition with a high Curie temperature (Tc) of 470 K, simultaneously exhibiting excellent dielectric switching characteristics. In addition to the ordered-disordered movement of cations, the significant displacement of anions is also responsible for such high Tc and large dielectric switching ratios, which is very rare in molecular-based switching materials. This work enriches the development of molecular ferroelastic switching materials and gives inspiration for the exploration of environmentally friendly high Tc organic salt ferroelastics with prominent switching performances.

Heavy Metal-Based Nanoparticles as High-Performance X-ray Computed Tomography Contrast Agents.

X-ray computed tomography (CT) contrast agents offer extremely valuable tools and techniques in diagnostics via contrast enhancements. Heavy metal-based nanoparticles (NPs) can provide high contrast in CT images due to the high density of heavy metal atoms with high X-ray attenuation coefficients that exceed that of iodine (I), which is currently used in hydrophilic organic CT contrast agents. Nontoxicity and colloidal stability are vital characteristics in designing heavy metal-based NPs as CT contrast agents. In addition, a small particle size is desirable for in vivo renal excretion. In vitro phantom imaging studies have been performed to obtain X-ray attenuation efficiency, which is a critical parameter for CT contrast agents, and the imaging performance of CT contrast agents has been demonstrated via in vivo experiments. In this review, we focus on the in vitro and in vivo studies of various heavy metal-based NPs in pure metallic or chemical forms, including Au, Pt, Pd, Ag, Ce, Gd, Dy, Ho, Yb, Ta, W, and Bi, and provide an outlook on their use as high-performance CT contrast agents.

Experimental and theoretical-based study of heavy metal capture by modified silica-alumina-based materials during thermal conversion of coal at high temperature combustion

Heavy metals emitted from coal combustion can easily pose many threats. In this study, five modified additives based on kaolin were prepared for reducing the emission of heavy metals from high temperature coal combustion and characterized by XRD, FT-IR, XRF, BET, SEM and zeta potential. The heavy metal retention characteristics of the additives under high temperature (900–1300 °C) coal combustion were investigated by static and dynamic experiments, and the results showed that pseudo-boehmite-metakaolin (BMK) was the most effective additive, and the ability of heavy metal capture was Cr > Zn > Pb > Cd, and the dynamic experiments were better than the static experiments. The quantum chemical models of heavy metals (monomers, oxides and chlorides), kaolin and adsorbent-active substances were developed and optimized, and the adsorption energy was calculated. The morphological changes of the active substances were taken into account in the simulation, and new mathematical models for adsorption energy calculation were proposed, which effectively solved the extreme results of adsorption energy calculation and made a comprehensive evaluation of heavy metal adsorption for the whole studied temperature range system. The mechanism of heavy metal adsorption on the active substance was further investigated by the simulations. Heavy metal atoms can form covalent or ionic bonds with O atoms of the active substance, Cl atoms of heavy metal chlorides can be covalently bonded or non-bonded with Al atoms of the active substance, and O atoms of heavy metal oxides can combine with Al atoms of the active substance to form ionic bonds. This study sheds new light on the control of heavy metals in high-temperature coal combustion, the methods for the optimization of simulation and the adsorption mechanism of heavy metals on relevant reactive substances. The method has a promising potential for large-scale application due to its simple preparation, low cost and significant effect.

Experimental Investigation of Thermodynamic Stabilization in Boron Imidazolate Frameworks (BIFs) Synthesized by Mechanochemistry.

This study experimentally explores the energetics for the formation of boron-imidazolate frameworks (BIFs), which are synthesized by mechanochemistry. The topologically similar frameworks employ the same tetratopic linker based on tetrakis(imidazolyl)boric acid but differ in the monovalent cation metal nodes. This permits assessment of the stabilizing effect of metal nodes in frameworks with sodalite (SOD) and diamondoid (dia) topologies. The enthalpy of formation from endmembers (metal oxide and linker), which define thermodynamic stability of the structures, has been determined by use of acid solution calorimetry. The results show that heavier metal atoms in the node promote greater energetic stabilization of denser structures. Overall, in BIFs the relation between cation descriptors (ionic radius and electronegativity) and thermodynamic stability depends on framework topology. Thermodynamic stability increases with the metallic character of the cation employed as the metal node, independent of the framework topology. The results suggest unifying aspects for thermodynamic stabilization across MOF systems.

Experimental and mechanistic study on the enrichment of heavy metals by modified calcium oxide during MSW pyrolysis

ABSTRACT Experimental and density functional theory (DFT) calculations show that NaCl modified can promote the adsorption of heavy metals Cr, Cd, and Pb by CaO in the municipal solid waste (MSW) pyrolysis. CrCl3 (g), CdCl2 (g) and PbCl2 (g) are the main form of Cr, Cd and Pb in MSW pyrolysis gas. The DFT calculations show that the adsorption energy of NaCl modified CaO (NaCl/CaO) increased from 285.37 kJ/mol, 130.58 kJ/mol and 145.72 kJ/mol to 373.80 kJ/mol, 216.03 kJ/mol and 214.67 kJ/mol for Cr, Cd and Pb compared with CaO. Similarly, the experimental average adsorption rates increased from 43.32%, 40.13% and 25.54% to 56.42%, 46.44% and 46.22%. The bondings between CaO and CrCl3, CdCl2, PbCl2 molecules are the outermost 2p orbitals of O in CaO hybridizes with the 3d and 3p orbitals of Cr, the 5s and 4d orbitals of Cd, and the 6p and 6s orbitals of Pb. After the adsorption of NaCl, the total charge change on the CaO surface changed from 0.12e to 0.01e, and the number of electrons obtained by CrCl3, CdCl2 and PbCl2 molecules from the adsorbent increased from 0.51, 0.26 and 0.22 e to 0.94, 0.53 and 0.34 e. NaCl promoting the electron-losing ability of calcium oxide surface. Meanwhile the Cl atom of NaCl form new chemical bonds with heavy metal atoms, increasing adsorption sites of heavy metal molecules with calcium oxide. This study contributes to the adsorption of heavy metals during MSW pyrolysis by CaO and NaCl/CaO.

One-Pot Synthesis of All-Inorganic CsPbClBr2 Blue Perovskite Quantum Dots via Stoichiometric Precursor.

The synthesis of perovskite-based blue light-emitting particles is valuable for several applications as the excellent optical properties and performances of the constituting materials associated with multi-exciton generation can be exploited. However, the preparation of perovskite precursors requires high temperatures, resulting in a complex manufacturing process. This paper proposes a one-pot method to synthesize CsPbClBr2 blue light-emitting quantum dots (QDs). In the case of nonstoichiometric precursor synthesis, the CsPbClBr2 QDs coexisted with additional products. The solvent for synthesizing mixed perovskite nanoparticles (containing chloride) was selected by mixing dimethylformamide (DMF) and/or dimethyl sulfoxide (DMSO) in different ratios. When only DMF was used with the stoichiometric CsBr and PbX2 (X = Cl, Br) ratio, the quantum yield was 70.55%, and superior optical properties were achieved. Moreover, no discoloration was observed for 400 h, and a high photoluminescence intensity was maintained. When deionized water was added to form a double layer with hexane, the luminescence was maintained for 15 days. In other words, the perovskite did not easily decompose even when in contact with water, which suppressed the release of Pb2+, which are heavy metal atoms in the structure. Overall, the proposed one-pot method for all-inorganic-based perovskite QDs provides a platform for synthesizing superior blue light-emitting materials.

The ability of zinc oxide nanostructures for removal of Pb2+, Cu2+, Ag2+ and Cd2+ ions from wastewater: computational perspective

In the heavy metal removal industry, adsorption is a famous and commonplace procedure well-recognized for its flexibility and utility. It is also a cost-effective procedure. Moreover, there are several adsorption procedures that are reversible on the one hand, and adsorbents may be reused after passing different desorption techniques on the other. The foundation of this research is to apply the calculations of the density functional theory (DFT) based on ab initio with an aim to explore the heavy metal atoms’ adsorption properties on ZnO–graphene resembling structure sheets and zinc oxide (ZnO) nanotubes. The heavy metals considered in this study include (Cu2+), (Pb2+), (Cd2+), and (Ag2+). In the initial stage, this study optimises both nanostructures. In the next phase, this study computes the steadiest configuration, the energy of adsorption, and the distance of equilibrium for each heavy metal with nanostructures utilising the mentioned DFT method. The findings were analyzed and compared. According to our case-by-case findings, ZnO-nanotubes exhibited better adsorption behaviour than ZnO–graphene sheets due to a smaller distance for equilibrium and higher adsorption energy. we’ve created the diagrams of the electronic density of states (DOS) in order to analyze the molecule adsorption electrical properties.

Ag(111) and its doped surfaces for heavy metal atoms removal from wastewater: DFT calculation analysis

Some toxic and harmful water pollutants like Cd, Cr, Pb and other heavy metals are inevitably produced during daily industrial and agricultural productions. In the context of green, environmental protection and sustainable development, the study on how to efficiently remove or recycle these heavy metals and give full play to their commercial potential has become the focus of researchers in recent years. There have been some experimental research results on the removal or recycle of heavy metals, but theoretical researches on metal doping adsorption are not deep enough. Based on density functional theory (DFT), the interactions of heavy metal Cd, Cr and Pb atoms with pure, Mo-doped, Pt-doped and Au-doped Ag(111) surfaces were studied by a first-principles calculation. It was found that Cr and Pb atoms shown chemisorption at all adsorption sites, while Cd atom shown physical adsorption (top and bridge sites) and chemisorption (hollow site). Among them, Mo doping, Pt doping and Au doping did not significantly improve the adsorption properties of Cd atom, but help the adsorption of Cr atom and Pb atom on doped substrates. The most stable adsorption surface for three types of heavy metal atoms is Mo-doped Ag(111) surface, and the most stable adsorption site (adsorption energies are −2.13 eV, −9.57 eV, −4.94 eV, respectively) is hollow site. This research enriches the design of Ag-based catalysts for wastewater treatment.

The advanced characterization, post-irradiation examination, and materials informatics for the development of ultra high-burnup annular U-10Zr metallic fuel

U-Zr metallic fuel is a promising fuel candidate for Gen Ⅳ fast spectrum reactors. Previous experimental irradiation campaigns showed that the sodium thermal bonded U-10Zr fuel design can achieve a burnup of 10% fissions per initial heavy metal atom (FIMA). Advanced metallic fuel designs are pushing the burnup limit to 20% or even 30% FIMA. To achieve the higher burnup and eliminate the pyrophoric sodium, a prototypical annular fuel has been designed, fabricated, clad with HT-9 in the Materials and Fuels Complex, and irradiated in the Advanced Test Reactors of Idaho National Laboratory (INL) to a peak burnup of 3.3% FIMA. During irradiation, the mechanical contact between fuel and cladding acts as a thermal bond. The irradiation lasted for 132 days in the reactor. Recently, the archived fresh and irradiated fuel samples were characterized using advanced characterization capabilities in the Irradiated Materials Characterization Laboratory (IMCL) of INL. This article summarizes the results of advanced characterization and computer vision-based materials informatics to reveal the irradiation effects on U-Zr metallic fuel. Future work will focus on further implementation of advanced characterization and statistical data mining to improve the fidelity of fuel performance modeling and support U-Zr metallic fuel qualification for fast spectrum reactors.

Periodic DFT study on heavy metals Cu(II) and Pb(II) atoms adsorption on Na-montmorillonite (010) edge surface

Heavy metal (HM) pollution is of great concern currently because it has been recognized as a potential threat to air, water,and soil. Adsorption is one of the most effective strategies for removing heavy metals. Montmorillonite as the adsorbent with a low cost and high thermal stability has received much attention. The adsorption of heavy metal Copper [Cu(II)] and Plumbum [Pb(II)] atoms on Na-montmorillonite hydroxylated (010) edge surface was analyzed using the generalized gradient approximation and density functional theory in the supercell technique. The coverage dependence of the adsorption structure and energetics was systematically investigated for a wide range of coverage from 0 to 1.0 monolayer (ML). Among all the possible adsorption sites, the most stable adsorption site for Cu(II) atom was a three-fold hollow site while the most favorable adsorption site for Pb(II) atom was a three-fold hollow site and followed by a two-fold bridge site. The adsorption energy increased with increasing coverage of Pb(II) atoms, indicating higher stability of surface adsorption and a tendency for the formation of adsorbate island clusters with increasing coverage. However, the adsorption energy of Cu(II) atoms decreased with increasing coverage. In the coverage range of 0 < Θ ≤ 0.5 ML the recovery capacity of the Na-montmorillonite for the heavy metal atoms was in the order of Cu(II)>Pb(II), while the recovery capacity of the Na-montmorillonite in the coverage range of 0.5 < Θ ≤ 1 ML was in the order of Pb(II)>Cu(II). The other aspects of the Cu(II) and Pb(II)/Na-montmorillonite (010) systems, including adsorption geometry, differential charge distribution, and electronic density of states were also studied and discussed in detail.

Effect of reprocessing on neutrons of a molten chloride salt fast reactor

Due to their unique features, such as the inherent safety, simplified fuel cycle, and continuous on-line reprocessing, molten salt reactors (MSRs) are regarded as one of the six reference reactors in the Generation IV International Forum (GEN-IV). Molten chloride salt fast reactors (MCFRs) are a type of MSR. Compared to molten fluoride salt reactors (MFSRs), MCFRs have a higher solubility of heavy metal atoms, a harder neutron spectrum, lower accumulation of fission products (FPs), and better breeding and transmutation performance. Thus, MCFRs have been recognized as a type of MSR with great prospects for future development. However, as the most important feature for MSRs, the effect of different reprocessing modes on MCFRs must be researched in depth. As such, this study investigated the effect of different isotopes, especially FPs, on the neutronic performance of an MCFR, such as its breeding performance. Furthermore, the characteristics of the different reprocessing modes and MCFR rates were analyzed in terms of safety, radioactivity level, neutron economy, and breeding capacity. In the end, a reprocessing method suitable for MCFRs was determined through calculation and analysis, which provides a reference for the further research of MCFRs.

Evaluating Quantities of Interest Other Than Nuclide Densities in the Bateman Equations

Traditionally, analysts solve the Bateman depletion equations to calculate the nuclide number density (NND) of each nuclide since these densities impact other reactor parameters, such as reactivity, as they change. Many quantities of interest, such as radiation damage, are calculated using simple integration methods, assuming that the NNDs are constant over a given depletion interval. However, the NNDs are time dependent, which can be accurately represented only by the Bateman depletion equations. We propose that these quantities can be calculated simultaneously with the NNDs within the Bateman depletion equations, preserving the coupled nature of these quantities to the time-dependent NNDs. We implemented this functionality in Griffin, demonstrating that only minor code modifications were necessary in order to accommodate an evaluation of these quantities in the Bateman depletion equations. The Chebyshev Rational Approximation Method was used to successfully solve for these additional quantities in the Bateman depletion equations. For radiation damage, the results calculated by Griffin were very accurate, differing by less than 2.5% from an analytical benchmark. For other quantities, the discrepancy between quantities calculated by the Bateman depletion equations versus those calculated by the Forward Euler method exceeded 10% for decay energy and 2% for fissions per initial heavy metal atom and kinetic energy released per unit mass when few depletion intervals were used. As the number of depletion intervals increased, both methods began to converge as expected.

Large magnetostriction of heavy-metal-element doped Fe-based alloys

Using density functional theory calculation and rigid band model, we investigate the electronic structure and magnetostrictive properties of transition heavy-metal doped Fe-based (Fe–Al, Fe–Si, Fe–B, and Fe–Be) alloys. It is found that a small amount of addition of 4d/5d heavy-metal atoms greatly enhances the coefficient of tetragonal magnetostriction of Fe-based alloys, reaching up to about 1000 ppm in Fe87.5Al6.25Pt6.25 and Fe75Al18.75Rh6.25 alloys. The underlying mechanism is mainly ascribed to combined factors of band narrowing induced by non-bonded states in pure Fe layer, strong spin–orbit coupling effect by heavy metals, and improved mechanical properties, through analysis of the electronic density of states near Fermi level and k-mesh resolved magnetocrystalline anisotropy energy in momentum space. These results provide useful guidance for optimizing the magnetostrictive performance of Fe-based alloys for practical application.

Defining the loading of single-atom catalysts: weight fraction or atomic fraction?

Single-atom catalysts (SACs) with the utmost atom-utilization capability are recently considered as the new frontier in catalysis. Theoretically, each isolated metal atom in SACs constitutes an active site during the catalysis. The single metal loading in SACs plays a significant role in tuning the catalytic activity as each isolated atom in SACs can function as a catalytically active point. Many studies calculated SA in weight fraction (wt%), however, defining SACs loading in wt% is less accurate to represent the number of active sites, due to the difference in the atomic mass between the SA and support, especially for heavy metal atoms and light elements. Compared to the wt%, atomic percentage (at%) can be more representative of the loading of SAs.

Ab initio calculation of the adsorption of As, Cd, Cr, and Hg heavy metal atoms onto the illite(001) surface: Implications for soil pollution and reclamation

Elucidating the mechanisms of heavy metal (HM) adsorption on clay minerals is key to solving HM pollution in soil. In this study, the adsorption of four HM atoms (As, Cd, Cr, and Hg) on the illite(001) surface was investigated using density functional theory calculations. Different adsorption configurations were investigated and the electronic properties (i.e., adsorption energy (Ead) and electron transfer) were analyzed. The Ead values of the four HM atoms on the illite(001) surface were found to be As > Cr > Cd > Hg. The Ead values for the most stable adsorption configurations of As, Cr, Cd, and Hg were −1.8554, −0.7982, −0.3358, and −0.2678 eV, respectively. The As atoms show effective chemisorption at all six adsorption sites, while Cd, Cr, and Hg atoms mainly exhibited physisorption. The hollow and top (O) sites were more favorable than the top (K) sites for the adsorption of HM atoms. The Gibbs free energy results show that the illite(001) surface was energetically favorable for the adsorption of As and Cr atoms under the influence of 298 K and 1 atm. After adsorption, there was a redistribution of positions and reconfiguration of the chemical bonding of the surface atoms, with a non-negligible influence around the upper surface atoms. Bader charge analysis shows electrons were transferred from the surface to the HM atoms, and a strong correlation between the valence electron variations and the adsorption energy was observed. HM atoms had a high electronic state overlap with the surface O atoms near the Fermi energy level, indicating that the surface O atoms, though not the topmost atoms around the surface, significantly influence HM adsorption. The above results show illite(001) preferentially adsorbed As among all four investigated HM atoms, indicating that soils containing a high proportion of illite might be more prone to As pollution.