Nanostructured ceria supported Pt and Au catalysts for the reactions of ethanol and formic acid

Çiftçi, Ayşegül; Ligthart, D. A. J. Michel; Pastorino, Pietro; Hensen, Emiel J. M.

doi:10.1016/j.apcatb.2012.10.029

Cited by 54 publications

(38 citation statements)

References 77 publications

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“…The N-doped carbon-supported catalysts with single atoms of Pt-group metals have proven capable of providing a remarkably high rate of formic acid decomposition, along with excellent selectivity 26 to H 2 and CO 2 and the possibility of using low loadings of Pt-group metals. The catalyst support admixtures.…”

Section: Discussionmentioning

confidence: 99%

“…12,25 For the production of hydrogen by formic acid decomposition, catalysis with single-atoms and sub-nanometer clusters was reported for gold catalysts. 24,26,27 Evidently, the properties and 4 catalytic applications of single-atom catalysts should be strongly dependent on the catalyst's support. As a rule, metal oxides are used as supports for the catalysts.…”

Section: Introductionmentioning

confidence: 99%

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Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

et al. 2016

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Formic acid is a valuable chemical derived from biomass, as it has a high hydrogen-storage capacity and appears to be an attractive source of hydrogen for various applications. Hydrogen production via formic acid decomposition is often based on using supported catalysts with Pt-group metal nanoparticles. In the present paper, we show that the decomposition of the acid proceeds more rapidly on single metal atoms (by up to one order of magnitude). These atoms can be obtained by rather simple means through anchoring Pt-group metals onto mesoporous N-functionalized carbon nanofibers. A thorough evaluation of the structure of the active site by aberration-corrected scanning transmission electron microscopy (ac-STEM) in high-angle annular dark field (HAADF) mode, by CO chemisorption, X-ray photoelectron spectroscopy (XPS) and quantum-chemical calculations reveals that the metal atom is coordinated by a pair of pyridinic nitrogen atoms at the edge of graphene sheets. The chelate binding provides an ionic/electron-deficient state of these atoms prevents their aggregation and thereby leads to an excellent stability under the reaction conditions. Catalysts with single atoms have also shown very high selectivity. Evidently, the findings can be extended to hydrogen production from other chemicals and can be helpful for improving other energy-related and environmentally benign catalytic processes.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

et al. 2016

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“…1,2 However, according to our knowledge, only gold species in sub-nm sized state have been reported as active sites for vapor-phase formic acid decomposition. Thus, it was shown [8][9][10][11] that these Au species supported on oxide supports are much more active in this reaction than Au nanoparticles. According to FlytzaniStephanopoulos, 12 the sub-nm species must be assigned to isolated Au-O x (OH) species attached to the oxide support.…”

Section: Introductionmentioning

confidence: 99%

Single Isolated Pd²⁺ Cations Supported on N-Doped Carbon as Active Sites for Hydrogen Production from Formic Acid Decomposition

et al. 2015

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Single-site heterogeneous catalysis with isolated Pd atoms was reported earlier mainly for oxidation reactions and for Pd catalysts supported on oxide surfaces. In the present work, we show that single Pd atoms on nitrogen-functionalized mesoporous carbon, observed by aberration-corrected scanning transmission electron microscopy (ac STEM), contribute significantly to the catalytic activity for hydrogen production from vapor-phase formic acid decomposition providing an increase by 2-3 times as compared to Pd catalysts supported on nitrogen-free carbon or unsupported Pd powder. Some gain in selectivity was also achieved.According to X-ray photoelectron spectroscopy (XPS) and near-edge X-ray absorption fine structure (NEXAFS) studies after ex situ reduction in hydrogen at 573 K, these species exist in a

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“…Indeed the synthesis approach within those papers has become the standard recipe for the preparation of rods and cubes [93,100,[103][104][105][106]. Further, the conclusion from those Catalytic mechanism for CO 2 reforming of methane over Ni-supported CeO 2 rod.…”

Section: Recent Work On the Structure And Reactivity Of Ceria Nanoshapesmentioning

confidence: 97%

“…papers that ceria rods have exposed (100) and (110) surfaces and grow along the {110} direction has been significantly relied on during the past eight years for furthering the field [19,21,76,92,96,[98][99][100]102,104,[106][107][108]. However, discrepancies in the literature do exist.…”

Section: Figurementioning

confidence: 99%

Ceria Nanoshapes—Structural and Catalytic Properties

Agarwal

Mojet

Lefferts

et al. 2015

Catalysis by Materials With Well-Defined Structures

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Nanostructured ceria supported Pt and Au catalysts for the reactions of ethanol and formic acid

Cited by 54 publications

References 77 publications

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

Single Isolated Pd²⁺ Cations Supported on N-Doped Carbon as Active Sites for Hydrogen Production from Formic Acid Decomposition

Ceria Nanoshapes—Structural and Catalytic Properties

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Nanostructured ceria supported Pt and Au catalysts for the reactions of ethanol and formic acid

Cited by 54 publications

References 77 publications

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

Single Atoms of Pt-Group Metals Stabilized by N-Doped Carbon Nanofibers for Efficient Hydrogen Production from Formic Acid

Single Isolated Pd2+ Cations Supported on N-Doped Carbon as Active Sites for Hydrogen Production from Formic Acid Decomposition

Ceria Nanoshapes—Structural and Catalytic Properties

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Single Isolated Pd²⁺ Cations Supported on N-Doped Carbon as Active Sites for Hydrogen Production from Formic Acid Decomposition