Infrared studies of CO, O2, and CO2 gases and their interaction products, chemically adsorbed on nickel oxide

Courtois, Michel; Teichner, S. J.

doi:10.1016/0021-9517(62)90016-7

Cited by 41 publications

(11 citation statements)

References 8 publications

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“…3a,b, difference FT-IR spectra are shown (that is, where the first spectrum of the series is subtracted from subsequent spectra). These consecutive spectra are focused on the absorption region between 2,250 and 1,400 cm −1 , where among other things intermediate C≡ O to C-O stretching vibrations occur [36][37][38][39] . Furthermore, we also observe C-H stretching vibrations at 3,015 cm −1 for methane (Fig.…”

Section: Two Separate Particle-size-dependent Mechanisms Identifiedmentioning

confidence: 99%

“…10f-h). The former set describes terminally adsorbed CO atop a single Ni atom, for which vibrations can occur anywhere between 2,060 and 2,019 cm −1 depending on the oxidation state of Ni [36][37][38][39] . The band at 1,903 cm −1 is ascribed to bridged carbonyl species; more specifically, a CO species bound to three neighbouring Ni atoms.…”

Section: Two Separate Particle-size-dependent Mechanisms Identifiedmentioning

confidence: 99%

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Unravelling structure sensitivity in CO2 hydrogenation over nickel

et al. 2018

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T he reduction of CO 2 emissions into the Earth's atmosphere is gaining legislative importance in view of its impact on the climate [1][2][3][4][5] . Reduction of the harmful effect of these emissions through reclamation of CO 2 is made attractive because CO 2 can be a zero-or even negative-cost carbon feedstock 6,7 . The conversion of renewably produced hydrogen and CO 2 into methane, or synthetic natural gas, over Ni is a solution that combines the potential to reduce CO 2 emissions with a direct answer to the temporal mismatch in renewable electricity production capacity and demand [8][9][10][11][12][13][14][15][16][17] . Chemical energy storage in the form of hydrogen production by electrolysis is a relatively mature technology; however, the required costly infrastructure, and inefficiencies in distribution and storage deem it inconvenient for large-scale application in the near future. Point-source CO 2 hydrogenation to methane represents an alternative approach with higher energy density. Furthermore, methane is more easily liquefied and can be stored safely in large quantities through infrastructures that already exist 18,19 . Power-to-gas (in this case methane) is thus actively considered as being capable of balancing electric grid stability, which will allow us to increase the renewable energy supply 20 .The search for fossil fuel alternatives, and application of a process such as that described above can arguably be achieved only with the help of advances in catalysis and the closely related field of nanomaterials. Continuous efforts in both fields have allowed us to make increasingly smaller and catalytically more active (metal) particles. However, it is already known that making progressively smaller supported catalyst particles does not necessarily linearly correspond to higher catalytic activity [21][22][23] . This phenomenon, where not all atoms in a supported metal catalyst have the same activity, is called structure sensitivity and is often attributed to the distinctly different chemistries on different lattice planes for π -bond activation in CO 2 , or σ -bond activation in, for example H 2 dissociation and C-H propagation 21,24 . The availability of stepped (less coordinated) versus terrace (more coordinated) sites on the surface of supported catalyst nanoparticles obviously changes with particle size, and atomic geometries become particularly interesting below 2 nm where, for example, π -bond activation is believed to not be able to occur 21 . While particle-size effects have been extensively studied for CO hydrogenation over Co 23,25 , the understanding of such structure sensitivity effects for these critical smaller metal particle sizes is lacking as sub-2-nm particles prove difficult to synthesize for first-row transition metals (Co, Fe and Ni). However, a particle-size effect for CO 2 hydrogenation is much less well established 26 .Here, we used a unique set of SiO 2 -supported Ni nanoparticles with diameters ranging from 1 to 7 nm in size, and show not only the existence of a distinct pa...

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Section: Two Separate Particle-size-dependent Mechanisms Identifiedmentioning

confidence: 99%

Section: Two Separate Particle-size-dependent Mechanisms Identifiedmentioning

confidence: 99%

Unravelling structure sensitivity in CO2 hydrogenation over nickel

et al. 2018

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“…When assessing the FT-IR spectrum of Figure a for SMR and Figure b for DMR, it is clear that panels 1 provide information on the asymmetric stretching vibrations of the C–H bonds. We refer here to Table for an overview of the literature-based FT-IR peak assignments used in this work. ,− The self-supported wafers of catalyst 6, likely due to its relatively high Ni weight loading, always deform during reduction, which causes resonance IR vibrations to occur in the CO stretching vibration region, hindering us from obtaining useful information from the operando FT-IR spectra. This is as shown in the Supporting Information.…”

Section: Resultsmentioning

confidence: 99%

Structure Sensitivity in Steam and Dry Methane Reforming over Nickel: Activity and Carbon Formation

et al. 2019

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Hydrogen is currently mainly produced via steam reforming of methane (SMR: CH 4 + H 2 O → CO + 3H 2 ). An alternative to this process, utilizing carbon dioxide and thus potentially mitigating its environmentally harmful emissions, is dry methane reforming (DMR: CH 4 + CO 2 → 2CO + 2H 2 ). Both of these reactions are structure sensitive, that is, not all atoms in a catalytic metal nanoparticle have the same activity. Mapping this structure sensitivity and understanding its mechanistic workings provides ways to design better, more efficient, and more stable catalysts. Here, we study a range of SiO 2 -supported Ni nanoparticles with varying particle sizes (1.2−6.0 nm) by operando infrared spectroscopy to determine the active mechanism over Ni (carbide mechanism) and its kinetic dependence on Ni particle size. We establish that Ni particle sizes below 2.5 nm lead to a different structure sensitivity than is expected from and implied in literature. Because of the identification of CH x D x species with isotopically labeled experiments, we show that CH 4 activation is not the only rate-limiting step in SMR and DMR. The recombination of C and O or the activation of CO is likely also an important kinetically limiting factor in the production of synthesis gas in DMR, whereas for SMR the desorption of the formed CO becomes more kinetically limiting. Furthermore, we establish the Ni particle size dependence of carbon whisker formation. The optimal Ni particle size both in terms of activity for SMR and DMR, at 500 and 600 °C, and 5 bar, was found to be approximately 2−3 nm, whereas carbon whisker formation was found to maximally occur at approximately 4.5 nm for SMR and for DMR increased with increasing particle size. These results have direct practical applications for tuning of activity and selectivity of these reactions, while providing fundamental understanding of their working.

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“…It indicates that the LDH-Au/CNTs electrode is more stable and poisoning-tolerant electrocatalyst of COE in our system. Ni and Ni oxide surface have strong both O 2 and CO adsorption 73 74 . For the active Ni-oxide catalyst, the structure transformation from NiO to NiOOH was found in the layered Ni(OH) 2 /NiOOH.…”

Section: Resultsmentioning

confidence: 99%

Efficient Dual-Site Carbon Monoxide Electro-Catalysts via Interfacial Nano-Engineering

Liu

Huang

Cheng

et al. 2016

Sci Rep

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Durable, highly efficient, and economic sound electrocatalysts for CO electrooxidation (COE) are the emerging key for wide variety of energy solutions, especially fuel cells and rechargeable metal−air batteries. Herein, we report the novel system of nickel−aluminum double layered hydroxide (NiAl-LDH) nanoplates on carbon nanotubes (CNTs) network. The formulation of such complexes system was to be induced through the assistance of gold nanoparticles in order to form dual-metal active sites so as to create a extended Au/NiO two phase zone. Bis (trifluoromethylsulfonyl)imide (NTf2) anion of ionic liquid electrolyte was selected to enhance the CO/O2 adsorption and to facilitate electro-catalyzed oxidation of Ni (OH)2 to NiOOH by increasing the electrophilicity of catalytic interface. The resulting neutral catalytic system exhibited ultra-high electrocatalytic activity and stability for CO electrooxidation than commercial and other reported precious metal catalysts. The turnover frequency (TOF) of the LDH-Au/CNTs COE catalyst was much higher than the previous reported other similar electrocatalysts, even close to the activity of solid-gas chemical catalysts at high temperature. Moreover, in the long-term durability testing, the negligible variation of current density remains exsisting after 1000 electrochemistry cycles.

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Infrared studies of CO, O2, and CO2 gases and their interaction products, chemically adsorbed on nickel oxide

Cited by 41 publications

References 8 publications

Unravelling structure sensitivity in CO2 hydrogenation over nickel

Unravelling structure sensitivity in CO2 hydrogenation over nickel

Structure Sensitivity in Steam and Dry Methane Reforming over Nickel: Activity and Carbon Formation

Efficient Dual-Site Carbon Monoxide Electro-Catalysts via Interfacial Nano-Engineering

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