The Formation and Properties of Pt&lt;SUB&gt;4&lt;/SUB&gt; Clusters on the Defective Graphene Support

Tang, Yanan; Yang, Zongxian; Dai, Xianqi

doi:10.1166/jnn.2013.6113

Cited by 6 publications

(3 citation statements)

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“…34 The defects or dopants in graphene act as nucleation centers or anchoring sites to limit the catalytic nanoparticle growth and improve the stability of metallic catalysts. [35][36][37] In the current study, the dynamic structural interconversion of Pt clusters, the adsorption behaviors of gas molecules and the reaction mechanisms of CO oxidation on the tetrahedral Pt 4 cluster supported on graphene substrates (Pt 4 -graphene) are studied using the first-principles methods. The graphene substrates include the pri-graphene, defective graphene with a single vacancy (SV-graphene) and O-graphene.…”

Section: Introductionmentioning

confidence: 99%

Geometric stability and reaction activity of Pt clusters adsorbed graphene substrates for catalytic CO oxidation

Tang

Chen

et al. 2015

Phys. Chem. Chem. Phys.

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The geometric stabilities, electronic structures and catalytic properties of tetrahedral Pt4 clusters anchored on graphene substrates are investigated using the first-principles methods. It is found that the small Pt4 clusters adsorbed on pristine graphene substrates easily interconvert between structural isomers by the small energy barriers, while the structural interconversion of Pt4 clusters on the defective graphene and oxygen-doped graphene (O-graphene) have the large energy barriers. Compared to other graphene substrates, the Pt4 clusters supported on the O-graphene substrate (Pt4/O-graphene) have the least geometrical distortion and the high symmetry of the Pt4 cluster can enhance the sensitivity of reactive gases. Moreover, the sequential reactions of CO oxidation on Pt4/O-graphene are investigated for comparison. Compared with the coadsorption reaction of CO and O2 molecules, the dissociative adsorption of O2 as a starting step has a small energy barrier (0.07 eV) and is followed through the Eley-Rideal reaction with an energy barrier of 0.42 eV (CO + Oads → CO2). The results provide valuable guidance for fabricating graphene-based catalysts as anode materials, and explore the microscopic mechanism of the CO oxidation reaction on atomic-scale catalysts.

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Section: Introductionmentioning

confidence: 99%

Geometric stability and reaction activity of Pt clusters adsorbed graphene substrates for catalytic CO oxidation

Tang

Chen

et al. 2015

Phys. Chem. Chem. Phys.

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“…In addition, more recent HAADF-STEM measurements have even observed single Pt atoms dispersed on undoped [15,16] and nitrogendoped [17] graphene, which show high catalytic activities and CO tolerance. Theoretically, on the other hand, firstprinciples calculations based on density functional theory (DFT) have been performed extensively to clarify the properties of graphene-supported Pt clusters from viewpoints of geometric [18][19][20][21][22][23][24][25][26][27][28][29][30][31][32][33][34] and magnetic [35][36][37][38][39][40][41][42][43][44] structures, molecular adsorptions [45][46][47][48][49][50], CO tolerance [51][52][53][54], and catalytic reactions such as CO oxidation [55][56][57][58][59][60], decomposition of O 3…”

Section: Introductionmentioning

confidence: 99%

Enhanced CO tolerance of Pt clusters supported on graphene with lattice vacancies

et al. 2020

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The adsorption of CO on Pt 4 clusters supported on graphene with lattice vacancies is studied theoretically using the first-principles calculation. Our results show that the electronic structure of the graphene-supported Pt 4 clusters is significantly modified by the interaction with carbon dangling bonds. As a result the adsorption energy of CO at a Pt site decreases almost linearly with the lowering of the Pt d-band center, in analogy with the linear law previously reported for CO adsorption on various Pt surfaces. An exceptional behavior is found for Pt 4 supported on graphene with a tetravacancy, where CO adsorption is noticeably weaker than predicted by the shift in the d-band center. Detailed electronic structure analyses reveal that the deviation from the linear scaling can be attributed to lack of Pt d states near the Fermi level that hybridize with CO molecular orbitals. The weakening of CO adsorption on the Pt 4 clusters is considered as a manifestation of the support effect of graphene, and leads to the enhancement of CO poisoning tolerance that is crucial for developing high-performance Pt cluster catalysts.

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“…However, an efficient catalyst that can facilitate the complete oxidation of ethanol to H 2 O and CO 2 is still a great challenge for the wide application of DEFCs. The adsorption of Pt nano or sub‐nanocluster on graphene can be enhanced by introducing defect, doping N, B, or O on graphene, or using bimetallic clusters…”

Section: Introductionmentioning

confidence: 99%

On the Catalytic Activity of Pt Supported by Graphyne in the Oxidation of Ethanol

Wang

2017

ChemistrySelect

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The adsorption of Pt clusters on β- and γ-graphyne (β-GY, γ-GY), graphdiyne (GDY), and graphene (GP) was extensively investigated with density functional theory. Ethanol adsorption and its partial oxidation on the Pt supported by the GY and GP were then explored to address the influence of the supporting materials on the activity of Pt nanoclusters to ethanol oxidation. Among the examined adsorption sites such as the hollow, Csp-Csp, and Csp-Csp2 bonds, the hollow site consisting of multiple triple bonds is the most attractive one to adsorb Pt and Pt4 regardless of β-GY, γ-GY, and GDY. The binding of Pt4 to the GDY is slightly stronger than those of β-GY and γ-GY (binding energy: −3.64, −3.73, and −4.08eV). It is remarkable that the adsorption of Pt4 on GY is 2–3 times stronger than that on GP (−3.6–4.1 vs −1.3 eV), showing that the GY and GDY are better substracts than the GP for the stability of Pt clusters. Furthermore, the potential energy profiles for the oxidation of ethanol show that in spite of the higher energy barrier for the adsorbed ethanol on Pt4 supported by γ-GY than by GP (1.54 vs 1.19eV), the dehydrogenation product and of ethanol on Pt-graphyne is much stabler than that on Pt-graphene, suggesting that graphyne is thermodynamically more favorable than graphene as a subtract for the Pt catalyst.

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The Formation and Properties of Pt<SUB>4</SUB> Clusters on the Defective Graphene Support

Cited by 6 publications

References 0 publications

Geometric stability and reaction activity of Pt clusters adsorbed graphene substrates for catalytic CO oxidation

Geometric stability and reaction activity of Pt clusters adsorbed graphene substrates for catalytic CO oxidation

Enhanced CO tolerance of Pt clusters supported on graphene with lattice vacancies

On the Catalytic Activity of Pt Supported by Graphyne in the Oxidation of Ethanol

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