The interaction of hydrogen with alumina-supported copper catalysts: a temperature-programmed adsorption/temperature-programmed desorption/isotopic exchange reaction study

Wilmer, H.; Genger, Thomas; Hinrichsen, Olaf

doi:10.1016/s0021-9517(03)00003-4

Cited by 75 publications

(25 citation statements)

References 38 publications

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“…On the basis of the existing experimental data and DFT calculations available in the literature, we can estimate that the enthalpy of adsorption of methane on Cu is about 3.2 eV [27,36,37], the hydrogen adsorption enthalpy is about −0.3 eV [38][39][40] and the enthalpy of graphene formation from adsorbed carbon is about −2.4 eV [32,34].…”

Section: Model Of Langmuir Adsorption and Two-dimensional Crystallizamentioning

confidence: 98%

Modeling of the self-limited growth in catalytic chemical vapor deposition of graphene

et al. 2013

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The development of wafer-scale continuous single-crystal graphene layers is key in view of its prospective applications. To this end, in this paper, we pave the way towards a graphene growth model in the framework of the Langmuir adsorption theory and two-dimensional crystallization. In particular, we model the nucleation and growth of graphene on copper using methane as a carbon precursor. The model leads to the identification of the range of growth parameters (temperature and gas pressures) that uniquely entails the final surface coverage of graphene. This becomes an invaluable tool to address the fundamental problems of continuity of polycrystalline graphene layers and crystalline grain dimensions. The model shows agreement with the existing experimental data in the literature. On the basis of the 'contour map' for graphene growth developed here and existing evidence of optimized growth of large graphene grains, new insights for engineering wafer-scale continuous graphene films are provided.

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Section: Model Of Langmuir Adsorption and Two-dimensional Crystallizamentioning

confidence: 98%

Modeling of the self-limited growth in catalytic chemical vapor deposition of graphene

et al. 2013

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“…The reaction model was based on DFT reaction rate constants by Kattel et al [13] for Zn/Cu(211) surface and the measured kinetics of H 2 adsorption and desorption on Cu. [38] The full reaction network is included in Supporting information, Table S2. The reaction rate for each pathway and the total species consumption/generation were computed as shown in equations 1 and 2.…”

Section: Multisite Microkinetic Modellingmentioning

confidence: 99%

Reaction Path Analysis of CO2 Reduction to Methanol through Multisite Microkinetic Modelling over Cu/ZnO/Al2O3 Catalysts

Prašnikar

Jurković

2021

Applied Catalysis B: Environmental

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The changing hierarchical structure of the applied heterogeneous Cu/ZnO/Al 2 O 3 material during methanol synthesis reactions hinders an efficient engineered process condition optimization, causing sub-optimal functional performance. A robust literature comparison is conducted to determine that activity is tightly coupled with Cu-Zn interactions. In order to investigate this physical behaviour further, characteristic experimental data is acquired through the catalytic reactor tests with an activated commercial catalyst, aged at different input measurements, monitored and characterized by the Brunauer-Emmett-Teller (BET), Xray diffraction (XRD), scanning transmission electron microscopy (STEM) with energy dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), H 2 transient adsorption (TA) and N 2 O pulsed surface oxidation (PSO) methodologies. It is shown that apparent rate law, exponents and activation energies do not vary significantly by increasing the ZnO X coverage from 7% to 23%, while not all of ZnO X over-layer is catalytically active.For Cu/ZnO/Al 2 O 3 with ZnO X over 7%, a highly-dispersed Al 2 O 3 decreases the measured intrinsic kinetics of the Cu-Zn site, implying a steric hindrance effect. Finally, building on unveiled chemical relations, a thorough multisite system micro-kinetic model, based on systematic contribution analysis, mechanisms and quantitative density functional theory (DFT) constants is developed. Values were optimized using the sequential screening results for an industrially relevant application (the temperatures of 160-260 °C, 50 bar pressure, 12,000-200,000 h -1 gas hourly space velocity (GHSV) flow and relative feed compositions).Designed mathematical relationships can therefore be utilised to accurately predict the turnover, selectivity and stability/deactivation in correspondence to ZnO X over Cu.

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“…As shown in Figure 4, all the reduced CZZ catalysts display a similar desorption pattern, demonstrating that there are two adsorptive forms on the surfaces. According to the literature, the resolved peak (peak α) at low temperature (390-480 K) is attributed to the desorption of atomic hydrogen on Cu sites [39], while the much broader peak (peak β) located at 650 K represents the desorption of strongly-adsorbed hydrogen either on the surface of bulk Cu particles or other metal oxides surfaces, respectively [39][40][41][42]. From the data of peak α, it is found that the amount of H2 desorption decreases slowly with the increase of the Cu/Zn ratio, which might be attributed to the loss of surface area, and it maintains nearly the same value at high temperature.…”

Section: H2 Chemisorptionmentioning

confidence: 99%

Catalytic Hydrogenation of CO2 to Methanol: Study of Synergistic Effect on Adsorption Properties of CO2 and H2 in CuO/ZnO/ZrO2 System

et al. 2015

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A series of CuO/ZnO/ZrO2 (CZZ) catalysts with different CuO/ZnO weight ratios have been synthesized by citrate method and tested in the catalytic hydrogenation of CO2 to methanol. Experimental results showed that the catalyst with the lowest CuO/ZnO weight ratio of 2/7 exhibited the best catalytic performance with a CO2 conversion of 32.9%, 45.8% methanol selectivity, and a process delivery of 193.9 gMeOH·kgcat. A synergetic effect is found by systematic temperature-programmed-desorption (TPD) studies. Comparing with single and di-component systems, the interaction via different components in a CZZ system provides additional active sites to adsorb more H2 and CO2 in the low temperature range, resulting in higher weight time yield (WTY) of methanol.

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The interaction of hydrogen with alumina-supported copper catalysts: a temperature-programmed adsorption/temperature-programmed desorption/isotopic exchange reaction study

Cited by 75 publications

References 38 publications

Modeling of the self-limited growth in catalytic chemical vapor deposition of graphene

Modeling of the self-limited growth in catalytic chemical vapor deposition of graphene

Reaction Path Analysis of CO2 Reduction to Methanol through Multisite Microkinetic Modelling over Cu/ZnO/Al2O3 Catalysts

Catalytic Hydrogenation of CO2 to Methanol: Study of Synergistic Effect on Adsorption Properties of CO2 and H2 in CuO/ZnO/ZrO2 System

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