Adsorption and decomposition of hydrazine on Pd(100)

Dopheide, R.; Schröter, L.; Zacharias, H.

doi:10.1016/0039-6028(91)90782-n

Cited by 24 publications

(15 citation statements)

References 10 publications

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“…The factor analysis including the four species also well explains the spectrum after the heat treatment (the inset of Fig.3c ). Previous studies dealing with N 2 H 4 adsorption on metal surfaces 35 36 37 38 and supported metal clusters 39 have shown the molecule is adsorbed intact at low temperatures but easily dissociates at elevated temperatures to yield N 2 H x ( x = 1~3), NH y ( y = 1~3), N, N 2 and H 2 . The literature suggests the species with the BE of 398.1 eV is NH 33 and there is no sign of nitrides (the BE = 397.6 eV).…”

Section: Resultsmentioning

confidence: 99%

“…It is notable that the peaks due to NH and NH 3 already have substantial intensities before the heating ( Fig.3a inset). This can be explained by immediate decomposition upon adsorption of the N 2 H 4 molecule that arrives first to W 5 , which is a reaction with large exothemicity 37 . Since the decomposition pattern of N 2 H x upon heating mentioned above is similar to that of N 2 H 4 , it is strongly suggested the N 2 H x is due mainly to N 2 H 4 .…”

Section: Resultsmentioning

confidence: 99%

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Reduction of N2 by supported tungsten clusters gives a model of the process by nitrogenase

Murakami

Yamaguchi

2012

Sci Rep

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Metalloenzymes catalyze difficult chemical reactions under mild conditions. Mimicking their functions is a challenging task and it has been investigated using homogeneous systems containing metal complexes. The nitrogenase that converts N2 to NH3 under mild conditions is one of such enzymes. Efforts to realize the biological function have continued for more than four decades, which has resulted in several reports of reduction of N2, ligated to metal complexes in solutions, to NH3 by protonation under mild conditions. Here, we show that seemingly distinct supported small tungsten clusters in a dry environment reduce N2 under mild conditions like the nitrogenase. N2 is reduced to NH3 via N2H4 by addition of neutral H atoms, which agrees with the mechanism recently proposed for the N2 reduction on the active site of nitrogenase. The process on the supported clusters gives a model of the biological N2 reduction.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Reduction of N2 by supported tungsten clusters gives a model of the process by nitrogenase

Murakami

Yamaguchi

2012

Sci Rep

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“…Most of the previous studies of catalytic decomposition of hydrazine have been focused on finding the reaction pathways using various experimental techniques (for examples: [12][13][14][15][16][17][18][19][20]). Unfortunately, despite of those extensive studies, the reaction pathways of hydrazine decomposition are not convincingly established yet.…”

Section: Introductionmentioning

confidence: 99%

Density functional study of hydrazine N–N bond cleaving on 3d metal surfaces

Fathurrahman

Kasai

2015

Surface Science

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Theoretical calculations based on dispersion-corrected density functional theory (DFT-D2) has been performed to investigate hydrazine adsorption and N-N bond cleaving on closed packed surfaces of 3d metals: Fe(110), Co(0001), Ni(111), Cu(111), and Zn (0001). The activation energies of N-N bond cleaving of hydrazine on each surface are estimated using climbing-image nudged elastic band (CINEB) method. The results showed that the activation energies for this process have increasing trend from Fe(110) to Zn(0001). By examining the electronic structure of the adsorbed hydrazine, it is found that this trend is related to occupation of derived 6σ* orbitals. It is also found that approximate linear relationship between reaction energy and activation energy (the Brønsted-Evans-Polanyi (BEP) relationship) holds for those surfaces.

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“…The decomposition of hydrazine was thought to take place mainly by the following two possible paths: (a) N 2 H 4 undergoes intramolecular dehydrogenation by eliminating H atom one by one, finally resulting in the formation of the N 2 and H 2 products (R5), as have been deduced from catalytic decomposition of hydrazine on surfaces of Ni(1 0 0) [7] and Pt(1 1 1) [8]; (b) the N-N bond of hydrazine cleaves firstly (R6), followed by further dehydrogenation of the newly formed NH 2 fragments into atomic N and H, and the latter recombine to form N 2 and H 2 molecules (R7). The formation of N 2 and H 2 is observed for catalytic decomposition on Fe(1 1 1) [6], transition metals (Cr, Mn, Fe, W, Re and Os) [9,10], polycrystalline aluminum [11], Ni(1 1 1) [12], polycrystalline iridium foil [13], and Pd(1 0 0) [14].…”

Section: Introductionmentioning

confidence: 99%