Collapse in Crystalline Structure and Decline in Catalytic Activity of Pt Nanoparticles on Reducing Particle Size to 1 nm

Sun, Yubao; Zhuang, Lin; Lu, Juntao; Hong, Xinlin; Liu, Peifang

doi:10.1021/ja076177b

Cited by 159 publications

(120 citation statements)

References 24 publications

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“…But for particle sizes smaller than 1 nm, the potential remained constant while the activity decreased with decreasing the size (153). 1 nm Pt nanoparticles were also studied in hydrogen oxidation reaction (154). Experimental and computational data showed that upon reducing the diameter of Pt nanoparticles down to 1 nm, a collapse in the crystalline structure occurs spontaneously and this causes a decline in the catalytic activity.…”

Section: Co Oxidationmentioning

confidence: 99%

Recent Advances in the Liquid‐Phase Synthesis of Metal Nanostructures with Controlled Shape and Size for Catalysis

2009

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Section: Co Oxidationmentioning

confidence: 99%

Recent Advances in the Liquid‐Phase Synthesis of Metal Nanostructures with Controlled Shape and Size for Catalysis

2009

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“…3 Thus, these results indicate that metal clusters can contribute to the development of industrial catalysis, 4 however, the challenges to obtain an atomistic understanding are complex. For example, a good cluster catalyst can abruptly turn down its performance upon a small change in the atomic structure, e.g., size change by adding or removing few atoms, 5,6 shape change, 7 ligands, 7 oxide support, which directly affects its reactivity. A large number of studies have been performed (see Refs.…”

Section: Introductionmentioning

confidence: 99%

Transition-metal 13-atom clusters assessed with solid and surface-biased functionals

Piotrowski

Piquini

Odashima

et al. 2011

The Journal of Chemical Physics

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Photoelectron spectroscopic study of iron-pyrene cluster anions J. Chem. Phys. 135, 204301 (2011) Lowest-energy structures and electronic properties of Na-Si binary clusters from ab initio global search J. Chem. Phys. 135, 184305 (2011) Electron interaction with nitromethane embedded in helium droplets: Attachment and ionization measurements J. Chem. Phys. 135, 174504 (2011) Geometry optimization of bimetallic clusters using an efficient heuristic method J. Chem. Phys. 135, 164109 (2011) Solvation effects on angular distributions in H(NH3)n and NH2(NH3)n photodetachment: Role of solute electronic structure J. Chem. Phys. 135, 164301 (2011) Additional information on J. Chem. Phys. First-principles density-functional theory studies have reported open structures based on the formation of double simple-cubic (DSC) arrangements for Ru 13 , Rh 13 , Os 13 , and Ir 13 , which can be considered an unexpected result as those elements crystallize in compact bulk structures such as the face-centered cubic and hexagonal close-packed lattices. In this work, we investigated with the projected augmented wave method the dependence of the lowest-energy structure on the local and semilocal exchange-correlation (xc) energy functionals employed in density-functional theory. We found that the local-density approximation (LDA) and generalized-gradient formulations with different treatment of the electronic inhomogeneities (PBE, PBEsol, and AM05) confirm the DSC configuration as the lowest-energy structure for the studied TM 13 clusters. A good agreement in the relative total energies are obtained even for structures with small energy differences, e.g., 0.10 eV. The employed xc functionals yield the same total magnetic moment for a given structure, i.e., the differences in the bond lengths do not affect the moments, which can be attributed to the atomic character of those clusters. Thus, at least for those systems, the differences among the LDA, PBE, PBEsol, and AM05 functionals are not large enough to yield qualitatively different results.

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“…1 The morphologic effects of Pt nanoparticles, films, and alloys on the oxygen reduction reaction were reported. 1,21 In contrast that the Pt nanoparticles have been formed on various types of controlled C materials, [3][4][5][6][7][8][9][10][11][12][13][14][15][16][17] the electric contact of Pt with C has never been controlled and monitored nanoscopically.…”

Section: Introductionmentioning

confidence: 99%

Synthesis and Site Structure of a Replica Platinum−Carbon Composite Formed Utilizing Ordered Mesopores of Aluminum-MCM-41 for Catalysis in Fuel Cells

et al. 2009

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Platinum nanoparticles have been reported with mean sizes between 1.5 and 7 nm supported on carbon. The contact between Pt nanoparticles and C has never been controlled and monitored nanoscopically. In this paper, stable Pt nanoparticles with a mean size of 1.2 nm were synthesized embedded on/in a C matrix catalytically produced from acetylene over the Pt nanoparticles. The replica Pt-C composite was synthesized inside of the ordered mesopores (2.7 nm) of Al-MCM-41 followed by removal of the template. The contact between the Pt nanoparticle and C was experimentally observed by high-energy resolution Pt L 2 -edge XANES spectra tuned to 11065.7 eV, at a lower energy by 5 eV than the Pt L 1 peak top for the replica Pt-C pressed to electrolyte polymer (Nafion). The spectra were nicely reproduced in a theoretical spectrum using ab initio multiple scattering calculations for the interface Pt site between cuboctahedral Pt 38 and graphite layers. Other Pt sites detected in state-selective Pt L 2 -edge XANES were exclusively metallic for replica Pt-C/Nafion either in air or in H 2 . The thus-characterized replica Pt-C composite was tentatively tested as a cathode of a H 2 -air polymer electrolyte fuel cell in comparison to commercial 20 wt % Pt/Vulcan XC-72 as the cathode. The improvement of Pt dispersion stabilized on/in a C matrix, effective contact of Pt with C, and diffusion of O 2 in a few nanometers of replica Pt-C powder was suggested.

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Collapse in Crystalline Structure and Decline in Catalytic Activity of Pt Nanoparticles on Reducing Particle Size to 1 nm

Cited by 159 publications

References 24 publications

Recent Advances in the Liquid‐Phase Synthesis of Metal Nanostructures with Controlled Shape and Size for Catalysis

Recent Advances in the Liquid‐Phase Synthesis of Metal Nanostructures with Controlled Shape and Size for Catalysis

Transition-metal 13-atom clusters assessed with solid and surface-biased functionals

Synthesis and Site Structure of a Replica Platinum−Carbon Composite Formed Utilizing Ordered Mesopores of Aluminum-MCM-41 for Catalysis in Fuel Cells

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