Ab initioinvestigation of quantum size effects on the adsorption of CO2, CO, H2O, and H2on transition-metal particles

Mendes, Paulo C. D.; Ocampo-Restrepo, Vivianne K.; Silva, Juarez L. F. Da

doi:10.1039/d0cp00880j

Cited by 22 publications

(29 citation statements)

References 69 publications

Supporting

Mentioning

Contrasting

Unclassified

Order By: Relevance

“…However, the amplitude of the quantum size effect becomes smaller when the film area is large enough to reach the semi‐infinite film limit. In addition, there are small oscillations in intermediate sizes and become weaker in the surface limit due to the increasing coordination of atoms with increasing size [23,24]. For CO 2 , the TGNs with n = 7 have the smallest absolute value of adsorption energy and the largest adsorption distance.…”

Section: Resultsmentioning

confidence: 99%

See 1 more Smart Citation

Electronic and adsorption properties of the zigzag‐edged triangle graphene nanosheets

Ding

Jin

Chen

2021

Int J of Quantum Chemistry

View full text Add to dashboard Cite

The electronic and adsorption properties of the zigzag-edged triangle graphene nanosheets with different size are investigated, including the calculation of the adsorption energy, sensitivity and recovery time after adsorbing CO 2 , NO 2 , CH 4 and CO. The results show that the quantum size effect is satisfied in the triangle graphene nanosheets, and its conductivity type can be changed from p to n. In addition, the triangle graphene nanosheets with n = 5 has the highest sensitivity to NO 2 (374.79%), which is more than 300 times as compared to the lowest one. The recovery time of triangle graphene nanosheets with n = 4 is the shortest, and its sensitivity and recovery time are the best at 144 K. These results reveal that the zigzag-edged triangular graphene nanosheets can serve as the fundamental structural unit for the design of high sensitivity gas sensors.

show abstract

Section: Resultsmentioning

confidence: 99%

“…The larger the absolute value of adsorption energy, the more stable the adsorption configuration. According to Equation (1 increasing size [23,24]. For CO 2 , the TGNs with n = 7 have the smallest absolute value of adsorption energy and the largest adsorption distance.…”

Section: Gas Adsorptionmentioning

confidence: 99%

Electronic and adsorption properties of the zigzag‐edged triangle graphene nanosheets

Ding

Jin

Chen

2021

Int J of Quantum Chemistry

View full text Add to dashboard Cite

show abstract

“…For the subsequent chapters of this thesis and articles published while developing this thesis, 145,146,159 all relevant bulk and clean surface properties were recalculated using the conditions established for each self-contained study; for example, using the D3 correction and respecting the specific POTCAR files, cutoff energies and convergence criteria defined for each chapter. Hence, small differences in the properties are possible, but all variations are within expected errors from DFT calculations (order of meV), considering that the computational parameters satisfy the convergence of the properties.…”

Section: Discussionmentioning

confidence: 99%

“…As an exception, for Mol/TM 13 , the starting structures were the non Source: Own study reproduced with permission for the thesis. 145 Reproduced from Ref.…”

Section: Procedures To Obtain Adsorption Atomic Structure Configurationsmentioning

confidence: 99%

See 1 more Smart Citation

>i<Ab Initio>/i< investigation of the adsorption of molecules, involved in carbon dioxide and glycerol utilization, on transition-metal substrates

Mendes¹

View full text Add to dashboard Cite

This study was motivated by technologies involving the utilization of glycerol and carbon dioxide to obtain higher value products, which are economically promising and can benefit the environment. Carbon dioxide is a greenhouse gas, abundant in the atmosphere, that could be converted into monomers, fuels and other moieties, while glycerol is a polyol, accumulated as a byproduct in the production of biodiesel, that can be used to obtain other three-carbon alcohols. The aforementioned technologies could be developed by the use of transition-metal substrates as nanoparticles or extended surfaces to design catalysts with great control over properties, such as particle size, morphology and composition, which can be tuned towards optimal catalytic performance. Our study focused on adsorption, a pivotal step of the catalytic process. In this thesis, we present an extensive ab initio investigation, based on density functional theory, of the adsorption of carbon dioxide, glycerol and additional small model molecules on finite-sized and extended TM substrates. Concerning size effects, we found that the adsorption properties for physisorbed and chemisorbed CO 2 depended significantly on the particle size. For CO and H 2 , there was alternation of the most stable adsorption site for the various substrate sizes, which resulted in small size-induced oscillations of properties, while for H 2 O, the adsorption was almost independent of size effects. We also studied the adsorption of CO 2 on Pt-based nanoalloys and found that for systems containing metals with completely filled d-states, alloying with Pt facilitated the charge transfer to CO 2 ; on the other hand, for metals from groups 8, 9 and 10 of the periodic table, alloying with increasing Pt content either caused small effects on the adsorption properties or impaired charge transfer to CO 2 . Moreover, we explored several stable morphologies and chemical orderings and found that CO 2 tends to bend on low-coordinated and heterogeneous adsorption sites. Concerning glycerol and other three-carbon alcohols, we systematically studied the influence of OH groups on the adsorption on model surfaces and found that increasing the number of OH groups increases the adsorption strength, while changing their relative positions leads to similar adsorption strength, but with distinctions of other properties, such as bond stretching for the molecules, such trends were discussed in terms of the reactivities of the alcohols.

show abstract

Polymer Template Synthesis of CuO_x/Clay Nanocomposites with Controllable CuO_x Formation

Takeuchi,

Ohkubo

2023

ChemistrySelect

View full text Add to dashboard Cite

Metal oxides have the excellent functions including high thermal stability, electrical properties, catalytic performance, and adsorption properties of acid gases such as CO2 via the acid‐base interactions. However, they suffer from low reserves, porosity control, and low adsorption efficiency per weight compared with lightweight materials including carbon and silica. To solve these issues, various methods for supporting metal oxides on porous carriers, such as decomposition‐precipitation and impregnation, have been investigated, but controlling the formation of metal oxide on clay nanosheets remains as a challenge. Herein, we developed a soft‐template method for supporting metal oxide (CuOx) nanoparticles on activated clay nanosheets. The intercalation of polyethyleneimine (PEI)−Cu2+ complexes between the layers of clay nanosheets followed by calcination to construct CuOx and remove the PEI templates afforded CuOx/clay nanocomposites. The constructed CuOx/clay nanocomposites had the close porosity to that of clay. Tuning the Cu2+/PEI ratio in PEI−Cu2+ complex allowed to control CuOx states (loadings, particle sizes, etc.). Tuning of the supporting conditions allowed constructing a structure suitable for CO2 uptake. These findings will contribute to the development of the material science of metal oxide nanoparticles and their hybrid materials in diverse fields including CO2 adsorbents, energy devices, and catalysts.

show abstract

Ab initioinvestigation of quantum size effects on the adsorption of CO₂, CO, H₂O, and H₂on transition-metal particles

Abstract: Adsorption is a crucial preliminary step for the conversion of CO2, then the atomistic understanding of how substrate particle size affects this step could be a key factor to control the catalytic transformations of CO2 into higher-value products.

Cited by 22 publications

References 69 publications

Electronic and adsorption properties of the zigzag‐edged triangle graphene nanosheets

Electronic and adsorption properties of the zigzag‐edged triangle graphene nanosheets

>i<Ab Initio>/i< investigation of the adsorption of molecules, involved in carbon dioxide and glycerol utilization, on transition-metal substrates

Polymer Template Synthesis of CuO_x/Clay Nanocomposites with Controllable CuO_x Formation

Contact Info

Product

Resources

About

Ab initioinvestigation of quantum size effects on the adsorption of CO2, CO, H2O, and H2on transition-metal particles

Abstract: Adsorption is a crucial preliminary step for the conversion of CO2, then the atomistic understanding of how substrate particle size affects this step could be a key factor to control the catalytic transformations of CO2 into higher-value products.

Cited by 22 publications

References 69 publications

Electronic and adsorption properties of the zigzag‐edged triangle graphene nanosheets

Electronic and adsorption properties of the zigzag‐edged triangle graphene nanosheets

>i<Ab Initio>/i< investigation of the adsorption of molecules, involved in carbon dioxide and glycerol utilization, on transition-metal substrates

Polymer Template Synthesis of CuOx/Clay Nanocomposites with Controllable CuOx Formation

Contact Info

Product

Resources

About

Ab initioinvestigation of quantum size effects on the adsorption of CO₂, CO, H₂O, and H₂on transition-metal particles

Polymer Template Synthesis of CuO_x/Clay Nanocomposites with Controllable CuO_x Formation