Preferred Adsorption Sites Research Articles

Effect of Al and Mn substitutions on hydrogen activation performances of La–Ni–Al–Mn alloy

To interpret the effect of Al and Mn substitutions on activation performances of La–Ni–Al–Mn alloy, the initial activation curve has been measured, which shows that the incubation time of activation is prolonged with the increase of Al content in alloy, while shortened duo to Mn substitution. Further, the first-principles calculations are employed. We find that (1) (100)/(010) surface of LaNi5 is the most stable and its stability can be improved by Al substitution for Ni while decreased by Mn substitution; (2) the preferential hydrogen adsorption sites are the hole and Ni (or Mn)-top sites; (3) Al and Mn substitutions can increase the hydrogen adsorption stability, but Al doping decreases the number of available sites, therefore retarding activation, while Mn doping guarantees the number of available sites, making activation easier; (4) H bonds covalently with neighbor Ni (or Mn) and ionically with La, together determining the stability of hydrogen adsorption.

Copper nanoparticles encapsulated in zeolitic imidazolate framework-8 as a stable and selective CO2 hydrogenation catalyst

Metal–organic frameworks have drawn attention as potential catalysts owing to their unique tunable surface chemistry and accessibility. However, their application in thermal catalysis has been limited because of their instability under harsh temperatures and pressures, such as the hydrogenation of CO2 to methanol. Herein, we use a controlled two-step method to synthesize finely dispersed Cu on a zeolitic imidazolate framework-8 (ZIF-8). This catalyst suffers a series of transformations during the CO2 hydrogenation to methanol, leading to ~14 nm Cu nanoparticles encapsulated on the Zn-based MOF that are highly active (2-fold higher methanol productivity than the commercial Cu–Zn–Al catalyst), very selective (>90%), and remarkably stable for over 150 h. In situ spectroscopy, density functional theory calculations, and kinetic results reveal the preferential adsorption sites, the preferential reaction pathways, and the reverse water gas shift reaction suppression over this catalyst. The developed material is robust, easy to synthesize, and active for CO2 utilization.

DFT study on the polyol sacrificial agents for improved clay tolerance of polycarboxylate superplasticizers

With the gradual scarcity of high-quality sand and gravel resources, the increasing mud content in concrete aggregates could strongly adsorb on polycarboxylate superplasticizers (PCE), greatly reducing their working performance. Modifying the molecular structure of PCE or compounding sacrificial agents can effectively improve the tolerance to clay minerals. In this article, using different small molecule polyols and polypropylene glycol (PPG) as examples, density functional theory (DFT) was employed to simulate the adsorption between clay minerals and hydration products. This exploration aims to further understand the anti-clay performance of various sacrificial agents from the perspective of adsorption energy. Ca-montmorillonite (CaMMT) exhibits the lowest adsorption energy among different clay minerals, making it the preferred site for sacrificial agent adsorption. With an increase in hydroxyl number, the adsorption energy between polyol sacrificial agents and montmorillonite decreases. Among polymeric polyols, the adsorption energy between PPG 600 and montmorillonite is the lowest (-10.86 eV), indicating superior anti-clay performance by preferentially occupying active sites on montmorillonite. As the interlayer spacing of montmorillonite increases, the adsorption energy between PPG 600 and montmorillonite initially decreases and then increases, reaching the lowest value at c=15.5 Å. There are more electron transfers (0.858) compared to the electron gain and loss, confirming more interaction between the sacrificial agents and montmorillonite at 15.5Å. This article also provides a crucial theoretical basis for the structural design of anti-clay sacrificial agents, offering insights into addressing compatibility issues between PCEs and clay minerals.

Dinitrogen Activation by Heteronuclear Metal Carbide Cluster Anions Y1‐3CoC1,2−: An Experimental and DFT Study

AbstractMass spectrometry was used to observe the reactions between Y−Co heteronuclear metal carbide cluster anions Y1‐3CoC1,2− and N2 at room temperature. Y2CoC1,2− can produce Co ejection products, in which Y2CoC− also has N2 association products; YCoC2− and Y3CoC− only generate N2 association products, while YCoC− and Y3CoC2− are inert to N2. Detailed reaction pathways were obtained through density functional theory calculations, which reasonably explain the experimental phenomena. Co is superior to Y as the electrophilic reaction site in the clusters and is the preferential initial adsorption site for N2. Some crucial steps were identified, including N−N dissociation, CC−N formation, C−CN dissociation, and C−N formation. The energy barriers of these steps are closely related to the coordination mode of N/N2 and C/C2 in clusters. Two indicators, the N−N bond length and the Mayer bond order, were utilized to describe the activation degree of the N−N bond. Analyses on the density of states and the frontier molecular orbitals reveal the electronic structures of key intermediates for N−N dissociation. The reaction mechanisms of N2 activation on Y−Co carbide clusters obtained may lay a preliminary foundation for the further development of catalysts for nitrogen reduction reaction (NRR).

High throughput screening of pure silica zeolites for CF4 capture from electronics industry gas.

The capture and separation of CF4 from CF4/N2 mixture gas is a crucial issue in the electronics industry, as CF4 is a commonly used etching gas and the ratio of CF4 to N2 directly affects process efficiency. Utilizing high-throughput computational screening techniques and grand canonical Monte Carlo (GCMC) simulations, we comprehensively screened and assessed 247 types of pure silicon zeolite materials to determine their adsorption and separation performance for CF4/N2 mixtures. Based on screening, the relationships between the structural parameters and adsorption and separation properties were meticulously investigated. Four indicators including adsorption selectivity, working capacity, adsorbent performance score (APS), and regenerability (R%) were used to evaluate the performance of adsorbents. Based on the evaluation, we selected the top three best-performing zeolite structures for vacuum swing adsorption (LEV, AWW and ESV) and pressure swing adsorption (AVL, ZON, and ERI) processes respectively. Also, we studied the preferable adsorption sites of CF4 and N2 in the selected zeolite structures through centroid density distributions at the molecule level. We expect the study may provide some valuable guidance for subsequent experimental investigations on adsorption and separation of CF4/N2.

Effect of Chlorine on Copper Electrodissolution

A computational study on the role of adsorbed Cl ions on copper dissolution is presented. Extensive grand canonical Monte Carlo (GCMC) calculations using reactive force-field (ReaxFF) are used to check the formation chlorine (Cl) adlayer structures on Cu (100) surface as a function of the chemical potential (µ). From experimental studies conducted by other researchers it has been observed that Cl adlattice on Cu in c(2X2) at maximum coverage. We observe that at low µ, Cl adlayer is disordered and moves to ordered c(2X2) structure at high µ. The binding energy of Cl, oxygen (O), hydroxide (OH-) and H2O on Cu at different sites is calculated and compared with Density-functional theory (DFT) values. Metal surface is often highly uneven and rough during electrodissolution process. Therefore, we also discuss the adsorption isotherm, disorder-order transformation, and preferential adsorption sites for rough surfaces. Specific anion adsorption (SAA) of Cl involves partial charge transfer to Cu substrate and these effect the type of bond and bond strength which is also briefly discussed. The electrodissolution of Cu in the presence of Cl is modelled using kinetic Monte Carlo simulation to obtain the polarization curve.Keywords: Adsorbed chlorine, electrodissolution, grand canonical monte carlo, molecular dynamics, ReaxFF, kinetic monte carlo.

Effect of Ligand Aromaticity on Cyclohexane and Benzene Sorption in IRMOFs: A Computational Study.

A series of four isoreticular MOFs (IRMOF-1, -10, -14, and -16) were selected for a computational investigation of the effect of ligand aromaticity on the adsorption capacity of an aromatic VOC (benzene) compared to its nonaromatic analog (cyclohexane). The affinity of the adsorbates was evaluated by calculating Henry's constants and adsorption enthalpies. It has been evidenced that while KH values decrease with ligand elongation (IRMOF-10 and -16), inserting a pyrene core into the MOF structure (IRMOF-14) increases both the cyclohexane and benzene adsorption efficiency by ∼290 and 54%, respectively. To elucidate host-guest interactions, we sought to locate preferential adsorption sites in MOF structures for the two VOCs studied by using the GCMC method. It appears that benzene interacts with the metal center (Zn4O clusters) and most of the ligand while cyclohexane tends to localize preferentially only near the Zn4O clusters. Coadsorption isotherms (equimolar mixture of benzene and cyclohexane) demonstrated the preferential adsorption of cyclohexane due to the stronger affinity for the MOF structure. On the other hand, for other isoreticular structures, the ligand elongation leads to a shift of the adsorption curve of cyclohexane caused by pore size increase and therefore less interactions with the walls. This phenomenon is counterbalanced in the case of IRMOF-14 due to stronger interactions between the cyclohexane and pyrene groups. The present results thus open perspectives in the design of promising MOF candidates for high-performing separation and sorption/detection of hydrocarbon VOCs.

Reverse micelle strategy for effective substitutional Fe-doping in small-sized CeO2 nanocrystals: Assessment of adsorption and photodegradation efficiency of ibuprofen under visible light

Reverse micelle nanoreactors were successfully designed to synthesize small-sized ceria nanocrystals (3.5–4.2 nm) with a sizeable amount of substitutional iron. Undoped and doped CeO2 catalysts with an iron content (0.50–10 mol %) compliant with the nominal value were prepared and tested for the first time for the removal of ibuprofen both in the dark and under UV or visible light irradiation.The effective inclusion and distribution of iron in the ceria lattice were ascertained through in-depth physicochemical characterization. In particular, X-ray diffraction suggested the formation of an F-type crystal structure, ruling out the formation of separate iron-containing crystalline phases. On the other hand, substitutional doping of CeO2 with Fe atoms favoured the formation of Ce3+ defects and vacancy sites (VOs) with a maximum for the sample with 2.5 mol % iron (Fe2.5), as evidenced by X-ray photoelectron spectroscopy (XPS) measurements and Raman spectroscopy. UV–Vis spectroscopy showed that the optical properties were successfully modified by the presence of iron, which causes a gradual decrease in band gap as iron content increases. The experimental evidence was further verified and supported by density functional theory calculations. DFT calculations also revealed that the surface iron and oxygen vacancies are the preferential sites for ibuprofen adsorption. Nevertheless, it was found under dark conditions that adsorption capacity does not monotonically increase with iron content, revealing contrasting roles of surface characteristics. Indeed, catalytic experiments have identified a trade-off between adsorption and photodegradation, identifying Fe2.5 as the best-performing catalyst for ibuprofen removal under visible light irradiation. These results were discussed by considering the key properties of the catalysts as well as their different surface charge determined by ζ potential measurements. The best catalyst was tested through reuse experiments that proved its stability over 4 cycles. Finally, an attempt was made to identify the photodegradation by-products, allowing the detection of 1-ethenyl-4-(2-methylpropyl)benzene as the main by-product.

The preferred adsorption sites and catalytic mechanism of FCC_CoFeGaNiZn multi-principal element alloy for oxygen evolution reaction catalysis based on site preference of constituent atom on sublattice

The origin of distinguished oxygen evolution reaction (OER) catalytic properties of multi-principal element alloys (MPEAs) is not clear yet due to the rich surface-active sites may exist in MPEAs composed of multiple types of elements, which may bring complex catalytic environment. In this work, four main steps were carried out using computational materials science. The atom distribution of bulk MPEAs was constructed firstly based on the previously predicted site preference of atoms occupying sublattices, which is beyond the traditional hypothesis that the atom distributing randomly on the whole lattice. Then the (111) close-packed surface slab of CoFeGaNiZn MPEA was obtained by cleaving the bulk structure. Subsequently, the OER processes were systematically explored by calculating the free energy change of intermediates *OH, *O, and *OOH at 171 adsorption sites on the (111) surface. Finally, the oxygen evolution reaction catalytic mechanism and its site preference behavior of FCC_CoFeGaNiZn MPEA were discussed in detail. The results show that atoms have obvious site preference, which deviating the ideal randomly distribution, especially Co, Fe and Zn atoms always prefer to 3c sublattice at all temperature, Ga atoms tend to favor 1a sublattice, and the site preferences of Ni atoms and Ga atoms are affected by the heat treatment temperature. At 1273 K, the site occupying configuration is (Co0.0246Fe0.01680Ga0.4550Ni0.4990Zn0.0046)1a (Co0.2580Fe0.2610Ga0.1150Ni0.1000Zn0.2650)3c. The (111) surface of FCC_CoFeGaNiZn MPEA was based on the site occupying configuration at 1273 K, and it was then supposed to quenched to ground state to simulate the experimental status in the available literature. Since *O at hollow sites transforms into *OOH at a higher overpotential, hollow sites may be poisoning surface sites. Three intermediates are found to primarily participate in the catalytic reaction on top sites. In addition, there are no scaling relationships between ΔE*OH and ΔE*O for CoFeGaNiZn MPEA, even for the same type of top sites. It is noteworthy that an average overpotential of 0.349 V was predicted by considering the combinations of three intermediate-tendency elements, which is in better agreement with the experimental overpotential of 0.37 V at 10 mA/cm2 current density than the overpotential of 0.28 V based on the special quasirandom structures (SQS). Current intensive explorations bring new insights into the OER catalytic mechanism of the preferred adsorption sites of MPEAs based on the reasonable consideration concerning the atoms distributing configuration involving the exact site preference of the constituent metallic atoms on the sublattice.

Effects of surface defects and Bi2 pollution on adsorption of Po on Ag surface

During the operation of accelerator-driver systems, hazardous polonium isotopes are produced and their release affects the safety of the nuclear reactors. Reliable filter systems have been proposed to be developed and silver has been studied as one of candidate filter materials. In this work, the adsorption of atomic polonium on defective silver surface is calculated using first principles and strongly chemisorption was obtained. Vacancy on Ag (100), Ag (110), Ag (111) surfaces and hollow site at the step edge of Ag (211) surface are preferred Po adsorption sites. Effect of Bi2 molecule pollution on adsorption of Po is further considered. The result shows that the existence of Bi2 molecule reduces the capture ability of silver to Po, but strong adsorption was still obtained on the surfaces.

Hydrogen adsorption in Si-LTA and LTA-4A zeolites: A Gibbs Ensemble Monte Carlo simulation study

Storing a targeted amount of hydrogen is one of the most challenging tasks. Several porous materials are being tested for the physisorption of hydrogen. We perform, NPT-Gibbs Ensemble Monte Carlo Simulation of hydrogen storage inside two zeolites: Si-LTA and LTA-4A. Classical three-site Silvera-Goldman potential is used to model hydrogen molecules. Gravimetric densities, radial distribution functions, adsorption enthalpies and specific regions for hydrogen are analyzed in detail in this study. Although number of hydrogen molecules stored in LTA-4A is more compared to Si-LTA, their gravimetric densities are comparable. At 77 K and 200 bar, almost 3 wt% of hydrogen can be stored in these zeolites. Introduction of sodium ions enhance the number of hydrogen molecules adsorbed in LTA-4A. Because of the presence of sodium ions at the windows of the cages, it can store these extra hydrogens inside it. It is also observed that for both these zeolites, preferred adsorption sites are always α-cages compared to the channels or β-cages. Replacement of silicon atoms with aluminium does not have any change on the uptake, but the presence of sodium counter ions increase the uptake. At low loading, enthalpies of adsorption are enhanced by 2 kJ/mol, because of the counter ions. Even though hydrogen uptake is less in these zeolites, we find important aspects of hydrogen adsorption in general which will help to devise porous materials with higher storing capabilities.

Intermetallic based materials for Sabatier reaction: Surface understanding, performance assessment and comparison with commercial catalyst

Ni-based intermetallics and commercial CO2 hydrogenation catalysts have been compared in Sabatier’s reaction. For RENi5 intermetallics (RE = La, Ce), the analysis of the chemical bonding shows a charge transfer from the RE to the Ni species and the formation of polar two- and four-atomic RE-Ni and four-atomic Ni bonds. Surface simulations and chemical understanding based on the ELI-D mapping approach indicate that dangling bonds originate from the multi-atomic ones and they are the preferred adsorption sites for H2 molecules. This leads to H2 dissociation, its reduction to hydrides, Ni QTAIM-anion oxidation to the metallic state, and diffusion toward the surface. LaNi5 is active toward rWGS while the best catalytic activity is obtained over CeNi5 (49% methane yield) at 723 K; the exhaust catalyst is composed of Ni particles supported over CeO2 with a mean size of 10 nm and thus, promising material could be developed on intermetallic based compounds.

First-principles study of electronic structure, sodium diffusion on 2D TiO2 monolayers for sodium-ion battery electrodes

The search for suitable electrode materials is crucial for the development of high-performance Na-ion batteries (NIBs). In recent years, significant attention has been drawn to two-dimensional (2D) oxides as potential NIB electrode materials. In this study, employing the first-principles density functional theory method, we investigate the thermodynamic and kinetic properties of Na adsorption and diffusion behavior on the 2D TiO2 (010) monolayer. Our findings demonstrate that the 2D anatase TiO2 (010) monolayer exhibits enhanced thermodynamic stability. Furthermore, the Na atoms preferentially adsorb on the top of oxygen atoms within the TiO2 (010) monolayer, and their diffusion along the [100] direction is characterized by a low energy barrier of 0.054 eV. This comprehensive analysis sheds light on the structural stability, preferred adsorption sites, and diffusion paths of Na atoms on the 2D anatase TiO2 (010) monolayer, providing valuable insights into the nature of the material’s structure and Na ion transport. Moreover, the 2D structure of the TiO2 matrix facilitates short Na diffusion lengths and a large electrode/electrolyte interface, thereby demonstrating the potential of this material as an NIB electrode material.

Stable Janus monolayer MoSHx (0.5 ≤ x ≤ 2)

MoSH is a representative example of a Janus two-dimensional monolayered system consisting of a molybdenum atomic layer sandwiched between sulfur and hydrogen atomic layers. Extensive experimental and theoretical efforts have suggested the great promise of the MoSH material, but the validity of the MoSH model (with a Mo–S–H ratio of 1:1:1) remains uncertain. While various experiments have established the Mo-to-S ratio to be close to 1:1, the hydrogen content has remained elusive even with the use of state-of-the-art characterization techniques due to its lightweight nature. In this study, we present a theoretical investigation aiming to determine the positions and ratios of the hydrogen atoms on MoSHx (with x ranging from 0 to 3) as well as assess their structural stability. By evaluating the energetic, mechanical, and thermodynamic properties, we confirm the existence of stable MoSHx structures within a critical range of hydrogen atom ratios, specifically 0.5 ≤ x ≤ 2.0. Additionally, as the hydrogen atom ratio increases, we observe a transition in the preferred adsorption sites of hydrogen atoms from the center of the hexagonal ring composed of molybdenum and sulfur atoms to the upper region of the molybdenum atoms. This study offers critical insight into the structural characteristics and stability of Janus monolayer MoSHx, contributing to the advancement and application of Janus MoSHx in various fields.

Exploring hydrogen adsorption on nanocluster systems: Insights from DFT calculations of Au[formula omitted] ([formula omitted] = Sc-Ni)

The superatomic cluster Au102+ is the smallest known replica of the golden pyramid Au20, and its complex analogues, Au9M2+ (M = Sc-Ni), have exhibited stable and intriguing electronic properties. In this study, we employ density-functional theory (DFT) to investigate the interaction between hydrogen molecules and Au9M2+ clusters. Our DFT calculations reveal that the structures of these clusters are influenced by the dissociative adsorption of H2, but not by the molecular adsorption. By conducting a comprehensive analysis, we show that the preferred adsorption configuration is a result of the competition between various factors, including the surface/encapsulated position, relative electronegativity, and coordination number of atoms. Although Au9M2+-2H (M = Sc, Ti, Mn, and Fe) are remarkably more stable than their corresponding Au9M2+-H2 configurations, different activation energies ranging from 0.15 to 0.99 eV are required during the dissociative reaction pathway. The finding results shed light on the mechanisms underlying the preferred adsorption site of hydrogen on the studied species and provide insights into adsorption kinetics that can aid further theoretical and experimental studies of hydrogenation in nanostructured materials.

Molecular Simulation Study Based on Adsorption of Gas (CO2,O2,CH4) on Coal

This study aimed to further explore the adsorption properties of different gases (CO2, O2, and CH4) on the coking coal surface by establishing a molecular model. Changes in the absolute adsorption capacity and the isosteric heat of adsorption of gases under different temperatures, pressures, and compositions were simulated using grand canonical Monte Carlo (GCMC) and molecular dynamics simulations. Interaction energy and energy distribution were used to analyze the adsorption behavior of gases, and the diffusion properties were investigated using the diffusion coefficient and diffusion activation energy. The absolute adsorption results fit well with the Langmuir–Freundlich model. The absolute adsorption capacity had a significant positive correlation with pressure and the corresponding mole fraction, and a significant negative correlation with temperature. The competitiveness, based on binary adsorption selectivity, was in the order of CO2 > O2 > CH4. The isosteric heat of adsorption of CH4 was slightly higher than that of O2, and that of CO2 was 1.49–1.64 times that of O2 and CH4. The isosteric heat of the adsorption of gases was also barely influenced by temperature and pressure. The interaction energy between CO2 and coal was greater than that of O2 or CH4, but the high pressure and high content were not conducive to the adsorption of O2 by CO2. The preferred adsorption site for CO2 was stronger than that for O2 and CH4, and its peak value negatively correlated with the molar fraction. The diffusion coefficient for single component gases initially increased and then decreased with increased pressure, showing a positive correlation with temperature. A close inverse correlation existed between diffusion activation energy and pressure. These results revealed the microscopic adsorption and diffusion regularities of CO2, O2, and CH4 in the coal model, indicating great significance in accurately predicting coal fires.

Electrical field-induced selective adsorption behaviours on graphene/Ni heterostructured surfaces: A theoretical study

Graphene is a promising candidate as an ideal reinforcing phase for metal matrix, but the grain growth mechanism within functional graphene/metal composite is still unclear. In our work, the interface microstructures evolution process of graphene/Ni composites is proposed from a theoretical perspective using the first-principles method based on density functional theory (DFT). Specifically, the adsorption and diffusion behaviours of Ni atoms on the graphene/Ni heterostructured surfaces and the selective adsorption sites under external electrical field are comprehensively investigated. Strong interactions are verified by population analysis and charge difference density. To elucidate the influence from the external electrical field, the intensity and the direction of the external electric field are considered. Moreover, the adsorption behaviours of Ni on the boron-doped graphene are studied. It can be concluded that the preferable adsorption sites are near the edge of graphene, and the presence of graphene is favourable for fine grains, and the introduction of boron will decrease adsorption capability. It is expected that our results could provide the underlying insights to reveal the role of graphene in structural evolution and offer some theoretical guidance to rationally design graphene/metal composites.

First-principle calculation of hydrogen adsorption on the surface of Ni3Al (110)

Nickel-based superalloy has good mechanical properties and corrosion resistance, and is widely used in the oil and natural gas industry. However, hydrogen brittle is a serious problem that the application of nickel-based superalloy must face. In this study, the first principle calculation method based on density functional theory was used to calculate the adsorption energy of the molecules of hydrogen and hydrogen atoms on the Ni3Al (110) surface. The calculated results show that the adsorption of hydrogen molecules on the surface of Ni3Al (110) is physical adsorption. The preferential adsorption site of hydrogen molecules is at the top site of Ni atoms, and Ni can promote the dissociation of hydrogen molecules. Hydrogen atoms tend to adsorb in the bridge, and the Ni-Ni bridge site is the preferential adsorption site.

Robust Hydrogen-Bonded Organic Framework with Four-Fold Interpenetration for Adsorptive Separation of C2H6/C2H4 and Xe/Kr.

Hydrogen-bonded organic frameworks (HOFs) are an emerging class of porous materials that hold promise for the adsorptive separation of industrially relevant gas mixtures. However, developing HOFs with high thermal stability and resistance to water remains a daunting challenge. We report here a microporous HOF (HIAM-103) assembled from a hexacarboxylate linker (2,4,6-trimethylbenzene-1,3,5-triylisophthalic acid, H6TMBTI). The compound crystallizes in the trigonal crystal system, and its structure is a four-fold interpenetrated network. Upon thermal activation, the single crystals remain intact, allowing for precise determination of the activated structure. HIAM-103 exhibits remarkable thermal and hydrothermal stability. Its microporous channels demonstrate selective adsorption of C2H6 over C2H4 and Xe over Kr, and its separation capability toward mixed gases has been validated by column breakthrough experiments under dry and humid conditions. The preferential gas adsorption sites and separation mechanisms have been uncovered through DFT analysis, which suggests that the methyl group decorated 1D channels are the primary reason for the selective adsorption.

Understanding the interaction in cellulose–chitosan composite and its adsorption ability for Nickel (II): a theoretical investigation

ABSTRACT The tight-binding quantum chemical method (GFN2-xTB) was performed to study the nature of the interaction between the two components in a cellulose–chitosan composite (CCS) and its adsorption ability for Ni2+ and NiOH+. The interaction energy, topology of bond paths, frontier molecular orbitals, Fukui functions, and molecular electrostatic potentials were calculated and analysed to figure out the interaction between the components in the CCS. The obtained results show that cellulose and chitosan mainly interact via the formation of hydrogen bonds and van der Waals forces. The CCS shows high adsorption ability for Ni2+ and NiOH+. The preferred adsorption sites of Ni(II) on the CCS were determined and analysed. The improvement in adsorption ability of CCS over pristine cellulose and chitosan was attributed to the changes in structure and electronic properties of the material due to the interaction between the components.