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Effect of morphology and size on the thermodynamic stability of cerium oxide nanoparticles: Experiment and molecular dynamics calculation

  • Andrey N. Chibisov EMAIL logo , Maxim A. Pugachevskii , Alexander P. Kuzmenko , Myo Min Than and Alexey I. Kartsev
Published/Copyright: January 27, 2022
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Nanotechnology Reviews
From the journal Nanotechnology Reviews Volume 11 Issue 1

Abstract

Cerium oxide nanoparticles have unique catalytic and oxygen storage capacity properties. In this work, the morphology and size of cerium oxide nanoparticles were experimentally and theoretically investigated. For the synthesis of nanoparticles, the laser ablation method was used. The analysis of the size and morphological characteristics of nanoparticles was performed using transmission electron microscopy. Using the method of molecular dynamics, we reveal the limiting dimensional transition from octahedral morphology to a spherical form in cerium oxide nanoparticles. The results obtained will be relevant for the controlled synthesis of nanostructured materials based on cerium oxide.

Keywords: nanoparticles; cerium oxide; size and morphology; TEM microscopy; molecular dynamics

1 Introduction

Due to its unique properties, nanostructured cerium oxide is commonly used in solid oxide fuel cells [1] and as a catalyst [2]. Understanding its main properties such as high oxygen storage capacity, redox catalytic properties [3], and electronic properties is an important step to creating highly promising nanomaterials based on cerium oxide nanoparticles. For a detailed understanding of these processes, it is necessary to consider the dimensional, morphological, and thermodynamic features of nanostructured compounds based on CeO2. Recent experimental studies show that the lattice parameters increase with a decrease in the size of cerium oxide nanoparticles. The authors explain this lattice expansion as a result of the formation of significant amounts of Ce3+ with corresponding oxygen vacancies [4,5,6]. Our theoretical calculations within the framework of the density functional theory confirm this result [7]. In refs. [8,9], it was shown that the surface energies of cerium oxide are characterized by the relationship (111) < (110) < (100). These surfaces, depending on the size of the CeO2 nanoparticles, determine their morphology according to the Wulff rule [10,11]. The synthesis of the nanocrystalline cerium oxide uses various common physicochemical methods such as the co-precipitation method [3], the solvothermal method [12,13], the hydrothermal method [11], pyrolysis [14], the sol–gel process [15], etc. These methods can produce cubic, octahedral, spherical, and other forms of CeO2 nanoparticles. In particles with a more developed morphology, the physicochemical activity increases significantly. So, for cubic and octahedral particles in comparison with spherical particles of the same volume, the specific surface area increases significantly. In addition, at the boundaries and vertices of the faces, favorable conditions arise for the formation of structural defects, which contribute to a significant increase in the catalytic, nanoelectronic, energy storage, and biomedical properties of particles.

One of the most promising methods for nanostructuring a substance, especially for obtaining nanoparticles, is laser ablation [16,17]. The advantage of this method is the possibility of obtaining metastable condensed phases due to the development of high-temperature gradients in the process of ultrafast heating and cooling of matter. These physical processes are characterized by the accumulation of structural defects in the nanoparticles’ crystal structure that can affect the functional properties of CeO2 when it is used in applied problems, such as photocatalysis [18], thermoelastic stabilization [19], and antioxidant properties [20]. When cerium oxide nanoparticles are obtained using laser ablation [21,22], there is a strong scatter in the particle sizes, and, in general, they are characterized by octahedral and spherical morphology [23,24]. However, at what nanoparticles diameter and why the transition from octahedral to spherical morphology occurs is still unclear. For a more detailed and accurate description of the properties of nanosized systems based on cerium oxide nanoparticles, it is necessary to use computational methods capable of describing the structure and morphology of the nanoparticles for sufficiently large sizes. The molecular dynamics method served such a computational technology.

This work is devoted to the experimental and theoretical study of the morphology of cerium oxide nanoparticles. Here, the cerium oxide nanoparticles were produced by laser ablation; the analysis of the size and morphological characteristics of the nanoparticles was carried out using transmission electron microscopy. Using the method of molecular dynamics, the agglomeration of CeO2 nanoparticles depending on their size has been calculated for the first time. With the help of our studies, we were able to identify the phase transition from octahedral to spherical morphology and determined the limiting size of this transition.

2 Experiments and calculations

2.1 Materials and methods

Cerium dioxide nanoparticles were obtained by pulsed sputtering of the target material using an IPG Photonics diode-pumped ytterbium fibre laser with the HighContrast option (radiation wavelength: 1.06 µm, laser radiation intensity: 1010 W m−2, pulse duration: 200 µs, and pulse repetition rate: up to 1 kHz). The target for laser ablation was a tablet of remelted chemically pure (>99.99%) cerium dioxide powder. Under the action of focused laser radiation, cerium dioxide was explosively sprayed, forming a flow of ablated particles [18,19,25]. Layers of ablated cerium dioxide nanoparticles were deposited onto a silicon wafer. The spraying time was 1–10 min. Then, the resulting particles were dispersed in an ultrasonic bath for at least 40 min. Deionized water was used as a solvent. After dispersion, the nanodispersed solution of cerium dioxide was centrifuged at various spin rates in the range from 800 to 13,400 rpm to minimize the limiting particle size. After centrifugation of the colloidal CeO2 system at 500 rpm, the limiting particle size in the colloidal system is reduced up to 80 nm; at 2,000 rpm, 50 nm; at 5,000 rpm, 40 nm; and, at 12,500 rpm, 30 nm [26]. Cerium dioxide nanoparticles were characterized using transmission electron microscopy (ZEISS LIBRA-120). For size and morphological analysis, several TEM images (more than 10 images for each sample) were used and the data are subsequently summarized.

2.2 Calculation methods

To carry out molecular dynamics calculations for cerium oxide nanoparticles, we used the Desmond package [27] implemented on the basis of “neutral territory” methods with a high degree of computational parallelism [28,29,30]. This software package has previously been successfully used to simulate the behaviour of CeO2 nanoparticles [31]. All calculations were carried out at a constant temperature of 300 K and pressure of 1 bar within the NPT ensemble (a statistical mechanical ensemble that maintains constant temperature T, constant pressure P, and a constant number of particles N). For electrostatic and van der Waals interactions, we used a cut off at 9 Å taking into account the reversible reference system propagator algorithms (RESPA integrator) [32]. To describe the boundary conditions, all particles were placed in a cell with an orthorhombic shape.

3 Results and discussions

The TEM images of cerium oxide nanoparticles obtained by laser ablation are shown in Figure 1a. The results show that ablated nanoparticles have a wide size variation from 5 to 200 nm and can be characterized by both octahedral and spherical morphology. To determine the sphericity degree of the nanoparticles, the characteristic parameter of the sphericity coefficient was chosen:

(1) ℜ = d D ,

where d and D are the diameters of the inscribed and described spheres for a nanoparticle of a certain size. The results of the analysis of TEM images show (Figure 1b) that an octahedral morphology is observed for ablated nanoparticles with sizes less than 23 nm, and a more spherical shape of particles is characteristic for sizes larger than 23 nm (the particle size was characterized by an equivalent spherical diameter for a sphere that has a volume equal to the volume of the particle). To explain this effect, the method of molecular dynamics was used.

Figure 1 (a) Transmission electron microscopy image of cerium oxide nanoparticles obtained by laser ablation. (b) Dependence of the degree of nanoparticles' sphericity on their size.
Figure 1

(a) Transmission electron microscopy image of cerium oxide nanoparticles obtained by laser ablation. (b) Dependence of the degree of nanoparticles' sphericity on their size.

According to transmission electron microscopy, X-ray diffractometry, and electron energy loss spectroscopy studies, it has recently been established that the ablated CeO2 nanoparticles are enriched in oxygen vacancies that stabilize their internal structure. At this, with a decrease in the particle size, the concentration of crystal defects in the ablated particles increases [20]. The methodology of the laser ablation experiment is such that nanoparticles are sprayed in air under the influence of high temperature, and when they are deposited on a substrate (in our experiment on silicon), they quickly cool to room temperature. Therefore, molecular dynamics were simulated at a temperature of 300 K. The purpose of the calculations using molecular dynamics was to reveal the regularities of the agglomeration of CeO2 nanoparticles during their synthesis by laser ablation.

We began our calculations of molecular dynamics by studying the interaction of three nanoparticles with a composition Ce231O448. We studied this nanoparticle size using the electron density functional theory method in our previous work [7]. Unfortunately, these are the largest cerium oxide nanoparticles that we could calculate within the DFT method using the Vasp software package [33,34] and the computational resources at our disposal. Therefore, it is logical that we took the particle data as the objects of the computational experiment. Initially, the particles were positioned randomly with respect to each other. Then, after a specified simulation time of 8,000 ps, three nanoparticles agglomerate into the structure shown in Figure 2a. They form a particle with a size of about 4.7 nm. Moreover, it can be seen that it is more advantageous for the particles to combine with each other, mainly via the (111) faces. The results are in good agreement with the theoretical data of ref. [35], carried out by the density functional theory method. When nine nanoparticles of cerium oxide are combined (Figure 2b), they tend to form an octahedral nanoparticle with a size of 7.3 nm. The total number of atoms in this nanoparticle is 6,111, of which 2,079 are Ce and 4,032 are O atoms. When 27 nanoparticles are combined, the same pattern is observed: the particles agglomerate and try to form an octahedron with an average size of 10 nm (Figure 3a). This particle contains 6,237 Ce and 12,096 O atoms. A further increase in the number of combined nanoparticles leads to an increase in the size of the total agglomerated particle, and a spherical morphology is observed to form beyond 20.6 nm. Thus, our calculations show that with an increase in the size of cerium oxide nanoparticles over 20 nm, spherical nanoparticles become more stable than the octahedral forms. The calculations are in good agreement with the experimental data acquired in this work, where the experimental value of the transition size from octahedral to spherical morphology was 23 nm.

Figure 2 Structure of agglomerated nanoparticles with a size of (a) 4.7 nm and (b) 7.3 nm. The cerium and oxygen atoms are depicted by yellow and red balls, respectively.
Figure 2

Structure of agglomerated nanoparticles with a size of (a) 4.7 nm and (b) 7.3 nm. The cerium and oxygen atoms are depicted by yellow and red balls, respectively.

Figure 3 Structure of agglomerated octahedral and spherical nanoparticles: (a) 10 nm in size and (b) 20.6 nm in size.
Figure 3

Structure of agglomerated octahedral and spherical nanoparticles: (a) 10 nm in size and (b) 20.6 nm in size.

4 Conclusion

In this work, experimental and theoretical studies of the influence of morphological and dimensional parameters on the thermodynamic stability of cerium oxide nanoparticles were carried out. The cerium oxide nanoparticles were synthesized using the laser ablation method, and the size and morphological characteristics of nanoparticles were analysed using transmission electron microscopy. Experimental data have shown that the resulting nanoparticles predominantly have octahedral and spherical morphology with a particle size ranging from 5 to 200 nm. Using the molecular dynamics method, we have shown that with an increase in the size of cerium oxide nanoparticles to more than 20 nm, spherical nanoparticles become more stable than the octahedral forms. This result is in good agreement with our experimental data of the transition size from an octahedral morphology to a spherical one equal to 23 nm. Our novel results will be important for the analysis and planning of controlled synthesis of high-quality nanomaterials based on cerium oxide nanoparticles with the aim of their promising application in catalysis, nanoelectronics, and biomedicine.

  1. Funding information: This study was carried out with the financial support of the Russian Foundation for Basic Research within the framework of scientific project no. 20-02-00599, as well as with the support of the Ministry of Education and Science of the Russian Federation, s/o 2020 no. 0851-2020-0035, prioritet-2030 program. The studies were carried out using the resources of the Center for Shared Use of Scientific Equipment and the Center for Processing and Storage of Scientific Data of the Far Eastern Branch of the Russian Academy of Sciences, funded by the Russian Federation represented by the Ministry of Science and Higher Education of the Russian Federation under project No. 075-15-2021-663. The authors would like to thank them for providing access to the HPC cluster atthe Joint Supercomputer Center of the Russian Academy of Sciences (JSCC RAS).

  2. Author contributions: All authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  3. Conflict of interest: The authors state no conflict of interest.

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Received: 2021-10-21
Revised: 2021-12-05
Accepted: 2022-01-01
Published Online: 2022-01-27

© 2022 Andrey N. Chibisov et al., published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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  104. The effect of graphene nano-powder on the viscosity of water: An experimental study and artificial neural network modeling
  105. Development of a novel heat- and shear-resistant nano-silica gelling agent
  106. Characterization, biocompatibility and in vivo of nominal MnO2-containing wollastonite glass-ceramic
  107. Entropy production simulation of second-grade magnetic nanomaterials flowing across an expanding surface with viscidness dissipative flux
  108. Enhancement in structural, morphological, and optical properties of copper oxide for optoelectronic device applications
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  111. Analysis of pure nanofluid (GO/engine oil) and hybrid nanofluid (GO–Fe3O4/engine oil): Novel thermal and magnetic features
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  113. Mechanisms and influential variables on the abrasion resistance hydraulic concrete
  114. Synergistic reinforcement mechanism of basalt fiber/cellulose nanocrystals/polypropylene composites
  115. Achieving excellent oxidation resistance and mechanical properties of TiB2–B4C/carbon aerogel composites by quick-gelation and mechanical mixing
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  117. Pulsed laser-assisted synthesis of nano nickel(ii) oxide-anchored graphitic carbon nitride: Characterizations and their potential antibacterial/anti-biofilm applications
  118. Effects of nano-ZrSi2 on thermal stability of phenolic resin and thermal reusability of quartz–phenolic composites
  119. Benzaldehyde derivatives on tin electroplating as corrosion resistance for fabricating copper circuit
  120. Mechanical and heat transfer properties of 4D-printed shape memory graphene oxide/epoxy acrylate composites
  121. Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
  122. Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
  123. Gray correlation analysis of factors influencing compressive strength and durability of nano-SiO2 and PVA fiber reinforced geopolymer mortar
  124. Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
  125. Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
  126. Mechanisms of the improved stiffness of flexible polymers under impact loading
  127. Anticancer potential of gold nanoparticles (AuNPs) using a battery of in vitro tests
  128. Review Articles
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  130. Application of Pickering emulsion in oil drilling and production
  131. The contribution of microfluidics to the fight against tuberculosis
  132. Graphene-based biosensors for disease theranostics: Development, applications, and recent advancements
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  134. Contemporary nano-architectured drugs and leads for ανβ3 integrin-based chemotherapy: Rationale and retrospect
  135. State-of-the-art review of fabrication, application, and mechanical properties of functionally graded porous nanocomposite materials
  136. Insights on magnetic spinel ferrites for targeted drug delivery and hyperthermia applications
  137. A review on heterogeneous oxidation of acetaminophen based on micro and nanoparticles catalyzed by different activators
  138. Early diagnosis of lung cancer using magnetic nanoparticles-integrated systems
  139. Advances in ZnO: Manipulation of defects for enhancing their technological potentials
  140. Efficacious nanomedicine track toward combating COVID-19
  141. A review of the design, processes, and properties of Mg-based composites
  142. Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
  143. Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
  144. Recent progress and challenges in plasmonic nanomaterials
  145. Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
  146. Electronic noses based on metal oxide nanowires: A review
  147. Framework materials for supercapacitors
  148. An overview on the reproductive toxicity of graphene derivatives: Highlighting the importance
  149. Antibacterial nanomaterials: Upcoming hope to overcome antibiotic resistance crisis
  150. Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
  151. A review of atomic layer deposition modelling and simulation methodologies: Density functional theory and molecular dynamics
  152. Recent advances in the preparation of PVDF-based piezoelectric materials
  153. Recent developments in tensile properties of friction welding of carbon fiber-reinforced composite: A review
  154. Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
  155. Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
  156. Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
  157. Nanotechnology application on bamboo materials: A review
  158. Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
  159. Nanostructured lipid carrier system: A compendium of their formulation development approaches, optimization strategies by quality by design, and recent applications in drug delivery
  160. 3D printing customized design of human bone tissue implant and its application
  161. Design, preparation, and functionalization of nanobiomaterials for enhanced efficacy in current and future biomedical applications
  162. A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
  163. Nanotechnology interventions as a putative tool for the treatment of dental afflictions
  164. Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
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  166. Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
  167. Latest developments in the upconversion nanotechnology for the rapid detection of food safety: A review
  168. Strategic applications of nano-fertilizers for sustainable agriculture: Benefits and bottlenecks
  169. Molecular dynamics application of cocrystal energetic materials: A review
  170. Synthesis and application of nanometer hydroxyapatite in biomedicine
  171. Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
  172. Biological applications of ternary quantum dots: A review
  173. Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
  174. Application of antibacterial nanoparticles in orthodontic materials
  175. Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
  176. Nanozymes – A route to overcome microbial resistance: A viewpoint
  177. Recent developments and applications of smart nanoparticles in biomedicine
  178. Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
  179. Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
  180. Diamond-like carbon films for tribological modification of rubber
  181. Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
  182. Recent research progress and advanced applications of silica/polymer nanocomposites
  183. Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
  184. Recent advances in perovskites-based optoelectronics
  185. Biogenic synthesis of palladium nanoparticles: New production methods and applications
  186. A comprehensive review of nanofluids with fractional derivatives: Modeling and application
  187. Electrospinning of marine polysaccharides: Processing and chemical aspects, challenges, and future prospects
  188. Electrohydrodynamic printing for demanding devices: A review of processing and applications
  189. Rapid Communications
  190. Structural material with designed thermal twist for a simple actuation
  191. Recent advances in photothermal materials for solar-driven crude oil adsorption
https://doi.org/10.1515/ntrev-2022-0038
Keywords for this article
nanoparticles; cerium oxide; size and morphology; TEM microscopy; molecular dynamics
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BY 4.0

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  116. Microwave-assisted sol–gel template-free synthesis and characterization of silica nanoparticles obtained from South African coal fly ash
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  121. Coupling the vanadium-induced amorphous/crystalline NiFe2O4 with phosphide heterojunction toward active oxygen evolution reaction catalysts
  122. Graphene-oxide-reinforced cement composites mechanical and microstructural characteristics at elevated temperatures
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  124. Preparation of layered gradient Cu–Cr–Ti alloy with excellent mechanical properties, thermal stability, and electrical conductivity
  125. Recovery of Cr from chrome-containing leather wastes to develop aluminum-based composite material along with Al2O3 ceramic particles: An ingenious approach
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  130. Application of Pickering emulsion in oil drilling and production
  131. The contribution of microfluidics to the fight against tuberculosis
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  141. A review of the design, processes, and properties of Mg-based composites
  142. Green synthesis of nanoparticles for varied applications: Green renewable resources and energy-efficient synthetic routes
  143. Two-dimensional nanomaterial-based polymer composites: Fundamentals and applications
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  145. Apoptotic cell-derived micro/nanosized extracellular vesicles in tissue regeneration
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  147. Framework materials for supercapacitors
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  150. Research progress of carbon materials in the field of three-dimensional printing polymer nanocomposites
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  154. Comprehensive review of the properties of fly ash-based geopolymer with additive of nano-SiO2
  155. Perspectives in biopolymer/graphene-based composite application: Advances, challenges, and recommendations
  156. Graphene-based nanocomposite using new modeling molecular dynamic simulations for proposed neutralizing mechanism and real-time sensing of COVID-19
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  158. Recent developments and future perspectives of biorenewable nanocomposites for advanced applications
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  160. 3D printing customized design of human bone tissue implant and its application
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  162. A brief review of nanoparticles-doped PEDOT:PSS nanocomposite for OLED and OPV
  163. Nanotechnology interventions as a putative tool for the treatment of dental afflictions
  164. Recent advancements in metal–organic frameworks integrating quantum dots (QDs@MOF) and their potential applications
  165. A focused review of short electrospun nanofiber preparation techniques for composite reinforcement
  166. Microstructural characteristics and nano-modification of interfacial transition zone in concrete: A review
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  169. Molecular dynamics application of cocrystal energetic materials: A review
  170. Synthesis and application of nanometer hydroxyapatite in biomedicine
  171. Cutting-edge development in waste-recycled nanomaterials for energy storage and conversion applications
  172. Biological applications of ternary quantum dots: A review
  173. Nanotherapeutics for hydrogen sulfide-involved treatment: An emerging approach for cancer therapy
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  175. Effect of natural-based biological hydrogels combined with growth factors on skin wound healing
  176. Nanozymes – A route to overcome microbial resistance: A viewpoint
  177. Recent developments and applications of smart nanoparticles in biomedicine
  178. Contemporary review on carbon nanotube (CNT) composites and their impact on multifarious applications
  179. Interfacial interactions and reinforcing mechanisms of cellulose and chitin nanomaterials and starch derivatives for cement and concrete strength and durability enhancement: A review
  180. Diamond-like carbon films for tribological modification of rubber
  181. Layered double hydroxides (LDHs) modified cement-based materials: A systematic review
  182. Recent research progress and advanced applications of silica/polymer nanocomposites
  183. Modeling of supramolecular biopolymers: Leading the in silico revolution of tissue engineering and nanomedicine
  184. Recent advances in perovskites-based optoelectronics
  185. Biogenic synthesis of palladium nanoparticles: New production methods and applications
  186. A comprehensive review of nanofluids with fractional derivatives: Modeling and application
  187. Electrospinning of marine polysaccharides: Processing and chemical aspects, challenges, and future prospects
  188. Electrohydrodynamic printing for demanding devices: A review of processing and applications
  189. Rapid Communications
  190. Structural material with designed thermal twist for a simple actuation
  191. Recent advances in photothermal materials for solar-driven crude oil adsorption
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