DFT study on H2O activation by stepped and planar Rh surfaces

Grootel, PW Pieter van; Hensen, Ejm Emiel; Santen, Rutger A. van

doi:10.1016/j.susc.2009.09.013

Cited by 31 publications

(25 citation statements)

References 50 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…2(n 2(p and q). For H 2 O, the plane formed by the three atoms is nearly parallel to the surface; this result is in good agreement with the previous study by van Grootel et al 44 3.2. CH x (x ¼ 1-3) formation from methane For CH x (x ¼ 1-3) formation from methane, the sequential dehydrogenation of CH 4 is investigated.…”

Section: Adsorption Of Reactants Products and Possible Intermediatessupporting

confidence: 93%

Source and major species of CH_x(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study

et al. 2014

View full text Add to dashboard Cite

Density functional calculations have been carried out to investigate the source and major species of CH x (x ¼ 1-3) involved in acetic acid synthesis from methane-syngas on the Rh(111) surface. All possible formation pathways of CH x (x ¼ 1-3) from methane and syngas have been systematically investigated. For CH x formation from methane, our results show that CH is the most abundant species; for CH x formation from syngas, all CH x (x ¼ 1-3) species form from CHO by CO hydrogenation, and the optimal formation routes of CH x show that CH and CH 3 are the most abundant species rather than CH 2 and CH 3 OH. On the other hand, CH formed by methane is more favourable than CH and CH 3 formed by syngas; meanwhile, CO insertion into CH x species to form C 2 oxygenates as acetic acid precursors is more favourable than CO hydrogenation to CH and CH 3 . As a result, in acetic acid synthesis from methanesyngas, CH x (x ¼ 1-3) species come from methane rather than syngas, and the corresponding primary species is CH. In addition, the CO in syngas is predominantly responsible for insertion reactions that produce CHCO, which is a C 2 oxygenate precursor leading to the formation of acetic acid. Furthermore, microkinetic modelling analysis shows that the major product of acetic acid synthesis from methanesyngas on the Rh(111) surface is CH 3 COOH, and that the production of CH 3 OH cannot compete with that of CH 3 COOH.

show abstract

Section: Adsorption Of Reactants Products and Possible Intermediatessupporting

confidence: 93%

Source and major species of CH_x(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study

et al. 2014

View full text Add to dashboard Cite

show abstract

“…The SMR reaction is widely implemented for production of hydrogen or other useful products [ 34 – 36 ]. The water dissociation is believed to be one of the rate controlling elementary reaction steps in the SMR reaction [ 37 ].…”

Section: Introductionmentioning

confidence: 99%

The Effect of Carbon Monoxide Co-Adsorption on Ni-Catalysed Water Dissociation

Mohsenzadeh

Börjesson

Wang

et al. 2013

IJMS

View full text Add to dashboard Cite

The effect of carbon monoxide (CO) co-adsorption on the dissociation of water on the Ni(111) surface has been studied using density functional theory. The structures of the adsorbed water molecule and of the transition state are changed by the presence of the CO molecule. The water O–H bond that is closest to the CO is lengthened compared to the structure in the absence of the CO, and the breaking O–H bond in the transition state structure has a larger imaginary frequency in the presence of CO. In addition, the distances between the Ni surface and H2O reactant and OH and H products decrease in the presence of the CO. The changes in structures and vibrational frequencies lead to a reaction energy that is 0.17 eV less exothermic in the presence of the CO, and an activation barrier that is 0.12 eV larger in the presence of the CO. At 463 K the water dissociation rate constant is an order of magnitude smaller in the presence of the CO. This reveals that far fewer water molecules will dissociate in the presence of CO under reaction conditions that are typical for the water-gas-shift reaction.

show abstract

“…The first hydrogen abstraction on Rh (111) was 0.02 eV faster than that on Fe (110). 208 However, *H2O and *OH dissociation on Ni (111) surface was 0.28 and 0.13 eV slower than that on Fe (110) surface, respectively. 209 The energy barrier for *H2O dissociation on Cu (111) was higher than 1 eV and the *OH dissociation was even harder with a high energy barrier of 1.51 eV.…”

Section: Resultsmentioning

confidence: 94%

“…0.68, 0.67, and 0.39 eV higher, respectively. [206][207][208]211 This indicated the positive influence of Mo6S8 cluster for the adsorption of H2O. Obviously, H2O adsorption was much stronger than CH4 adsorption, indicating that H2O…”

Section: Resultsmentioning

confidence: 96%

“…Compared with H2O dissociation on metallic surface, the interaction between M and Mo6S8 suppressed this elementary step by 0.16 and 0.37 eV on Co (110) and Rh (111), respectively. 206,208 However, H2O dissociation was accelerated by 0.26 and 0.14 eV on Fe (110) and Ni (111), respectively. 207,211 The energy barrier was the same for the case of Cu.…”

Section: H2o Adsorptionmentioning

confidence: 98%

See 1 more Smart Citation

Mo6s8-Based Single-Metal-Atom Catalysts for Methanol Synthesis From Steam Reforming of Methane

Zhang¹

View full text Add to dashboard Cite

DFT study on H2O activation by stepped and planar Rh surfaces

Cited by 31 publications

References 50 publications

Source and major species of CH_x(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study

Source and major species of CH_x(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study

The Effect of Carbon Monoxide Co-Adsorption on Ni-Catalysed Water Dissociation

Mo6s8-Based Single-Metal-Atom Catalysts for Methanol Synthesis From Steam Reforming of Methane

Contact Info

Product

Resources

About

DFT study on H2O activation by stepped and planar Rh surfaces

Cited by 31 publications

References 50 publications

Source and major species of CHx(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study

Source and major species of CHx(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study

The Effect of Carbon Monoxide Co-Adsorption on Ni-Catalysed Water Dissociation

Mo6s8-Based Single-Metal-Atom Catalysts for Methanol Synthesis From Steam Reforming of Methane

Contact Info

Product

Resources

About

Source and major species of CH_x(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study

Source and major species of CH_x(x = 1–3) in acetic acid synthesis from methane–syngas on Rh catalyst: a theoretical study