Theoretical Study of Ripening Mechanisms of Pd Clusters on Ceria

Su, Yaqiong; Liu, J Jinxun; Filot, Ivo A. W.; Hensen, Emiel J. M.

doi:10.1021/acs.chemmater.7b03555

Cited by 70 publications

(94 citation statements)

References 58 publications

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“…Pd, Au and Pt atoms prefer to be adsorbed on oxygen‐bridge site of CeO 2 (111),, while Cu atom preferentially locates on oxygen‐hollow site with a binding energy of 2.89 eV, in coincidence with the reported value of 3.03 eV . Figure shows the optimized configurations of isolated Cu atoms on various sites of CeO 2 (111).…”

Section: Figuresupporting

confidence: 67%

“…Single‐atom catalysts (SACs) abstract much attention due to the maximizing utilization of the precious metal components while offering the high reactivity and selectivity . However, metal single atoms generally have a high mobility and prefer to agglomerate into thermodynamically stable particles via Ostwald ripening . Therefore, the stability of the supported metal single atoms is vital for SACs.…”

Section: Figurementioning

confidence: 99%

“…Pd atom has a high mobility on CeO 2 (111), and the activation energy barrier for atomic diffusion is merely 0.14 eV . Au and Pt atoms also diffuse rapidly on the terrace of CeO 2 (111), and the corresponding diffusion barrier is 0.26 and 0.45 eV ,.…”

Section: Figurementioning

confidence: 99%

“…The chocie of U value has a negligible influence on the thermodynamic or kinetic energy property of CeO 2 system . And U =4.5 eV is extnsively used in the simulation of CeO 2 system ,. For the calculations of Cu 1 /CeO 2 (111), we used a periodic slab with a (4×4) supercell in which one of the surface Ce atoms was substituted by one TM atom.…”

Section: Figurementioning

confidence: 99%

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Highly stable and Active Cu₁/CeO₂ Single‐Atom Catalyst for CO Oxidation: A DFT Study

et al. 2018

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We carried out density functional theory simulations to examine the stability and CO oxidation activity of single Cu atoms supported on CeO2(111). Both the strong binding energy and high activation energy for Cu single atom diffusion indicate a high stability of the Cu1/CeO2 single‐atom catalyst. Electronic structure analysis verifies the formation of Cu+ cation due to electron transfer. The frequency analysis further corroborates that the experimentally observed IR bands around 2114–2130 cm−1 of CO adsorption at the boundary of Cu/CeO2 correspond to Cu+‐carbonyl species. Cu1/CeO2 single‐atom catalyst displays a promising catalytic activity for CO oxidation via Mars van Krevelen mechanism.

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Section: Figuresupporting

confidence: 67%

Section: Figurementioning

confidence: 99%

Section: Figurementioning

confidence: 99%

Section: Figurementioning

confidence: 99%

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Highly stable and Active Cu₁/CeO₂ Single‐Atom Catalyst for CO Oxidation: A DFT Study

et al. 2018

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“…In order to overcome the drawback associated with the conventional Pd/Al 2 O 3 catalysts, both theoretical and experimental investigations have suggested that the incorporation of ceria into Pd-based methane oxidation catalysts can result in improved catalytic activity and stability [21,[58][59][60]. For example Sheedeh and co-workers reported a comparative investigation of the activity of various Pd-based catalysts for application to methane oxidation.…”

Section: Catalytic Activitymentioning

confidence: 99%

Active and Stable Methane Oxidation Nano-Catalyst with Highly-Ionized Palladium Species Prepared by Solution Combustion Synthesis

et al. 2018

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We report on the synthesis and testing of active and stable nano-catalysts for methane oxidation. The nano-catalyst was palladium/ceria supported on alumina prepared via a one-step solution-combustion synthesis (SCS) method. As confirmed by X-ray photoelectron spectroscopy (XPS) and high-resolution transmission electron microscopy (HTEM), SCS preparative methodology resulted in segregating both Pd and Ce on the surface of the Al 2 O 3 support. Furthermore, HTEM showed that bigger Pd particles (5 nm and more) were surrounded by CeO 2 , resembling a core shell structure, while smaller Pd particles (1 nm and less) were not associated with CeO 2 . The intimate Pd-CeO 2 attachment resulted in insertion of Pd ions into the ceria lattice, and associated with the reduction of Ce 4+ into Ce 3+ ions; consequently, the formation of oxygen vacancies. XPS showed also that Pd had three oxidation states corresponding to Pd 0 , Pd 2+ due to PdO, and highly ionized Pd ions (Pd (2+x)+ ) which might originate from the insertion of Pd ions into the ceria lattice. The formation of intrinsic Ce 3+ ions, highly ionized (Pd 2+ species inserted into the lattice of CeO 2 ) Pd ions (Pd (2+x)+ ) and oxygen vacancies is suggested to play a major role in the unique catalytic activity. The results indicated that the Pd-SCS nano-catalysts were exceptionally more active and stable than conventional catalysts. Under similar reaction conditions, the methane combustion rate over the SCS catalyst was~18 times greater than that of conventional catalysts. Full methane conversions over the SCS catalysts occurred at around 400 • C but were not shown at all with conventional catalysts. In addition, contrary to the conventional catalysts, the SCS catalysts exhibited superior activity with no sign of deactivation in the temperature range between~400 and 800 • C.

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Engineering the Coordination Environment of Single‐Rh‐Site with N and S Atoms for Efficient Methanol Carbonylation

Mu,

Long,

Song

et al. 2023

Adv Funct Materials

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The local coordination environment of central active sites plays a critical role in tuning the catalytic properties of heterogeneous single‐metal‐site catalysts (HSMSCs). However, carbon supports with inert surface properties provide weak interaction with the active sites, which hamper the effective modulation of the coordination structure of HSMSCs. Herein, this work shows that introducing N and S atoms into carbon support can modify the coordination environment of single‐Rh‐site and effectively improves the catalytic activity for the methanol carbonylation reaction. The synthesized Rh/AC‐NS with single‐Rh‐site exhibits a high methanol conversion of 88% and a stable acetyl production rate of 2812 h−1, in contrast with 1285 h−1 of Rh/AC without N‐ and S‐ functional groups, and meanwhile remarkably higher than those of Rh/AC‐N and Rh/AC‐S with only N‐ or S‐ functional group under the same mild reaction conditions. As revealed by the experimental result and density functional theory (DFT) calculations, the special combination of N‐ and S‐ functional groups offers favorable coordination configuration and also beneficial electronic structure for facilitated CH3I oxidative addition and CO insertion steps of single‐Rh‐site. This work offers new opportunities for rationally tuning the coordination structure of HSMSCs for heterogeneous catalysis.

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Theoretical Study of Ripening Mechanisms of Pd Clusters on Ceria

Cited by 70 publications

References 58 publications

Highly stable and Active Cu₁/CeO₂ Single‐Atom Catalyst for CO Oxidation: A DFT Study

Highly stable and Active Cu₁/CeO₂ Single‐Atom Catalyst for CO Oxidation: A DFT Study

Active and Stable Methane Oxidation Nano-Catalyst with Highly-Ionized Palladium Species Prepared by Solution Combustion Synthesis

Engineering the Coordination Environment of Single‐Rh‐Site with N and S Atoms for Efficient Methanol Carbonylation

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Theoretical Study of Ripening Mechanisms of Pd Clusters on Ceria

Cited by 70 publications

References 58 publications

Highly stable and Active Cu1/CeO2 Single‐Atom Catalyst for CO Oxidation: A DFT Study

Highly stable and Active Cu1/CeO2 Single‐Atom Catalyst for CO Oxidation: A DFT Study

Active and Stable Methane Oxidation Nano-Catalyst with Highly-Ionized Palladium Species Prepared by Solution Combustion Synthesis

Engineering the Coordination Environment of Single‐Rh‐Site with N and S Atoms for Efficient Methanol Carbonylation

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Highly stable and Active Cu₁/CeO₂ Single‐Atom Catalyst for CO Oxidation: A DFT Study

Highly stable and Active Cu₁/CeO₂ Single‐Atom Catalyst for CO Oxidation: A DFT Study