N<sub>2</sub> Activation by Neutral Ruthenium Clusters

Kerpal, Christian; Harding, Dan J.; Lyon, Jonathan T.; Meijer, Gerard; Fielicke, André

doi:10.1021/jp401876b

Cited by 65 publications

(63 citation statements)

References 42 publications

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“…The weakened triple bond can then be broken with additional energy, in this case, energy provided by NTP. However, the energy provided by NTP is approximately 3-6 eV according to the specific type of discharge, which is insufficient to ionize Ru, which has ionization energy of 7.36 eV [17][18][19][20]. The situation changes when promoter Cs is attached to Ru.…”

Section: Introductionmentioning

confidence: 99%

Atmospheric Pressure Ammonia Synthesis Using Non-thermal Plasma Assisted Catalysis

Peng

Cheng

et al. 2016

Plasma Chem Plasma Process

132

146

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This paper described a novel and green approach on catalytic ammonia synthesis using non-thermal plasma (NTP). The process studied in this paper involves the synthesis and absorption of ammonia under atmospheric pressure and low temperature. The effects of operational parameters including applied voltage, frequency, gas component and flow rate on ammonia synthesis under NTP conditions are studied in this paper. In addition, different selected catalysts and absorbents were investigated under different conditions of NTP treatment and the ammonia efficiency was reported and analyzed. Ru catalyst with carbon nanotube support, along with Cs promoter and micro porous absorbents including Molecular Sieve 13X and Amberlyst 15 yield the highest ammonia efficiency in this process. Results further indicated that frequency and applied voltage of 10,000 Hz and 6000 V, with N 2 :H 2 feed ratio of 3:1 provided the optimized efficiency of ammonia synthesis of 2.3 gNH 3 /kWh.

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Section: Introductionmentioning

confidence: 99%

Atmospheric Pressure Ammonia Synthesis Using Non-thermal Plasma Assisted Catalysis

Peng

Cheng

et al. 2016

Plasma Chem Plasma Process

132

146

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“…12 In the cluster science, the activation and cleavage of the N−N bond caused by adsorption on transition-metal clusters have been reported. 13,14 In the present study, we investigated the interaction between cationic Ta clusters and N 2 in the thermal energy region, especially in terms of the adsorption forms, molecular or dissociative, and we compared the results with those of cationic Rh clusters. Reactions of neutral Ta clusters, Ta n , with N 2 were observed by Hamrick and Morse using a fast-flow reactor at 320 K. 15 They measured the rate constants of adsorption of a N 2 molecule as a function of the cluster size.…”

Section: ■ Introductionmentioning

confidence: 99%

Nitrogen Molecule Adsorption on Cationic Tantalum Clusters and Rhodium Clusters and Desorption from Their Nitride Clusters Studied by Thermal Desorption Spectrometry

2016

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Adsorption and desorption of N2 molecules onto cationic Ta and Rh clusters in the gas phase were investigated in the temperature range of 300-1000 K by using thermal desorption spectrometry in combination with density functional theory (DFT) calculations. For Ta6(+), the first N2 molecule was found to adsorb dissociatively, and it remained adsorbed when Ta6(+)N2 was heated to 1000 K. In contrast, the second and the subsequent N2 molecules adsorbed weakly as a molecular form and were released into the gas phase when heated to 600 K. The difference can be explained in terms of the activation barrier between the molecular and dissociative forms. On the other hand, when Ta clusters were generated in the presence of N2 gas by the laser ablation of a Ta rod, isomeric clusters, TanNm(+), having heat resistivity were formed. For Rh6(+), N2 adsorbed molecularly at 300 K and desorbed totally at 450 K. These results were consistent with the DFT calculations, indicating that the dissociative adsorption of N2 is endothermic.

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“…CO activation and N 2 activation on small neutral as well as singly charged ruthenium clusters have been studied. 8,9 Recently, small Ru cations have been shown to be catalytically active for CO methanation also in gas phase. 10 Several density functional theory (DFT) studies have been carried out to explore the structural properties of ruthenium clusters.…”

Section: Introductionmentioning

confidence: 99%

Structural evolution of small ruthenium cluster anions

Waldt

Hehn

Ahlrichs

et al. 2015

The Journal of Chemical Physics

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The structures of ruthenium cluster anions have been investigated using a combination of trapped ion electron diffraction and density functional theory computations in the size range from eight to twenty atoms. In this size range, three different structural motifs are found: Ru8(-)-Ru12(-) have simple cubic structures, Ru13(-)-Ru16(-) form double layered hexagonal structures, and larger clusters form close packed motifs. For Ru17(-), we find hexagonal close packed stacking, whereas octahedral structures occur for Ru18(-)-Ru20(-). Our calculations also predict simple cubic structures for the smaller clusters Ru4(-)-Ru7(-), which were not accessible to electron diffraction measurements.

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N₂ Activation by Neutral Ruthenium Clusters

Cited by 65 publications

References 42 publications

Atmospheric Pressure Ammonia Synthesis Using Non-thermal Plasma Assisted Catalysis

Atmospheric Pressure Ammonia Synthesis Using Non-thermal Plasma Assisted Catalysis

Nitrogen Molecule Adsorption on Cationic Tantalum Clusters and Rhodium Clusters and Desorption from Their Nitride Clusters Studied by Thermal Desorption Spectrometry

Structural evolution of small ruthenium cluster anions

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N2 Activation by Neutral Ruthenium Clusters

Cited by 65 publications

References 42 publications

Atmospheric Pressure Ammonia Synthesis Using Non-thermal Plasma Assisted Catalysis

Atmospheric Pressure Ammonia Synthesis Using Non-thermal Plasma Assisted Catalysis

Nitrogen Molecule Adsorption on Cationic Tantalum Clusters and Rhodium Clusters and Desorption from Their Nitride Clusters Studied by Thermal Desorption Spectrometry

Structural evolution of small ruthenium cluster anions

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N₂ Activation by Neutral Ruthenium Clusters