Insights into the direct selective oxidation of methane to methanol over ZSM-5 zeolytes in aqueous hydrogen peroxide

Alshihri, Saeed; Richard, C.; Al‐Megren, Hamid A.; Chadwick, David

doi:10.1016/j.cattod.2018.03.031

Cited by 13 publications

(10 citation statements)

References 50 publications

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“…Among the series of catalysts for the elimination of volatile organic chemicals, − noble metal-supported catalysts have received tremendous attention because of their excellent catalytic activities and high reaction rates in methane combustion, ,, especially for Pd-based catalysts. − ,,,− Although noble metal-supported catalysts have high efficiencies, their high price, low availability, and easy sintering at high temperatures limit their large-scale industrial applications. ,, Therefore, transition metal oxide catalysts are fast becoming the focus of researchers due to their lower cost and comparable catalytic activity to noble metal catalysts. − In the reaction course of methane catalytic combustion, the activation of the C–H bond is a key step, and NiO is considered to be one of the potential transition metal oxide nanoparticles capable of replacing noble metal catalysts due to its excellent performance in the activation of C–H bonds. ,,,, Consequently, interest in the fabrication of various NiO nanomaterials as high-efficiency and low-cost catalysts in lean methane catalytic combustion has been growing. , …”

Section: Introductionmentioning

confidence: 99%

Irregularly Shaped NiO Nanostructures for Catalytic Lean Methane Combustion

Ogunbiyi

et al. 2021

ACS Appl. Nano Mater.

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NiO nanomaterials prepared using a solid−liquid NH 3 • H 2 O precipitation method (NiO-NSL) were tested in the catalytic combustion of methane. The NiO-NSL presented a characteristic rodlike nanostructure with a length of about a few hundred nanometers except for a part of the nanoparticles. For comparison, the NiO nanomaterials prepared by the traditional liquid-phase NH 3 •H 2 O precipitation method (NiO-NLL) were tested in the same reaction conditions. NiO-NSL exhibited significantly higher methane combustion activity than NiO-NLL and achieved the complete combustion of methane at 390 °C, which was outstanding in non-noble metal-based catalyst. X-ray photoelectron spectroscopy (XPS) and hydrogentemperature-programmed reduction (H 2 -TPR) results indicate that the surface Ni 2+ content of NiO-NSL was higher than that of NiO-NLL, and the presence of more Ni 2+ might be responsible for the enhanced activity. DFT calculations prove that the energy barrier for C−H bond activation on Ni 2+ was lower than that on Ni 3+ , which was consistent with the higher methane catalytic combustion activity of NiO-NSL. In addition, when the precipitating agent was replaced with NaOH and (NH 4 ) 2 CO 3 , the generalization of the solid−liquid precipitation method in the preparation of the NiO catalysts was also tested. The results show that the solid−liquid precipitation method proposed in this work was still applicable when NaOH was used as a precipitant. However, with the use of (NH 4 ) 2 CO 3 as a precipitant, the methane catalytic activity of the NiO nanoparticles prepared by the solid−liquid precipitation method was reduced to a certain extent compared with the traditional liquid-phase precipitation method. This research can open up a highly efficient and environmentally friendly method for the synthesis of methane combustion catalysts.

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Section: Introductionmentioning

confidence: 99%

Irregularly Shaped NiO Nanostructures for Catalytic Lean Methane Combustion

Ogunbiyi

et al. 2021

ACS Appl. Nano Mater.

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“…The oxidation of C 1 -C 3 alkanes utilising H 2 O 2 in conjunction with HZSM-5 [28][29][30][31][32] in addition to AuPd nanoparticles supported on TiO 2 [33,34] at low temperature have been extensively reported, with the valorisation of methane to methanol in particular an attractive option to produce a versatile chemical feedstock. Indeed, we have previously reported that greater selectivity, at comparable catalytic productivity, towards methane can be achieved when generating H 2 O 2 from H 2 and O 2 compared to preformed, commercially synthesised H 2 O 2 [35].…”

Section: Introductionmentioning

confidence: 99%

The Direct Synthesis of H2O2 and Selective Oxidation of Methane to Methanol Using HZSM-5 Supported AuPd Catalysts

et al. 2019

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In this study we show that using gold palladium nanoparticles supported on a commercial aluminosilicate (HZSM-5) prepared using a wet co-impregnation method it is possible to produce hydrogen peroxide from molecular H 2 and O 2 via the direct synthesis reaction. Furthermore, we investigate the efficacy of these catalysts towards the oxidation of methane to methanol using commercially available H 2 O 2. The effect of SiO 2 : Al 2 O 3 ratio and calcination temperature is evaluated and a direct correlation between support acidity and the catalytic activity towards H 2 O 2 synthesis and methanol production is observed.

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“…This process has high capital and energy requirements, so its implementation is not profitable in many scenarios, particularly when lean methane emissions are used as feedstocks. 14 − 17 For this reason, the search for a cheaper and straightforward process to convert methane into methanol by partial oxidation has been an aim of the scientific community in the last decades. 18 − 21 …”

Section: Introductionmentioning

confidence: 99%

“…The most spread technology used for methanol production consists of a two-step process that uses natural gas as feedstock: first, methane is transformed into syngas via steam reforming and then the syngas is converted into methanol. This process has high capital and energy requirements, so its implementation is not profitable in many scenarios, particularly when lean methane emissions are used as feedstocks. − For this reason, the search for a cheaper and straightforward process to convert methane into methanol by partial oxidation has been an aim of the scientific community in the last decades. − …”

Section: Introductionmentioning

confidence: 99%

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Harnessing of Diluted Methane Emissions by Direct Partial Oxidation of Methane to Methanol over Cu/Mordenite

Álvarez

Marín

Ordóñez

2021

Ind. Eng. Chem. Res.

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The upgrading of diluted methane emissions into valuable products can be accomplished at low temperatures (200 °C) by the direct partial oxidation of methanol over copper-exchanged zeolite catalysts. The reaction has been studied in a continuous fixed-bed reactor loaded with a Cu–mordenite catalyst, according to a three-step cyclic process: adsorption of methane, desorption of methanol, and reactivation of the catalyst. The purpose of the work is the use of methane emissions as feedstocks, which is challenging due to their low methane concentration and the presence of oxygen. Methane concentration had a marked influence on methane adsorption and methanol production (decreased from 164 μmol/g Cu for pure methane to 19 μmol/g Cu for 5% methane). The presence of oxygen, even in low concentrations (2.5%), reduced methane adsorption drastically. However, methanol production was only affected slightly (average decrease of 9%), concluding that methane adsorbed on the active centers yielding methanol is not influenced by oxygen.

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Insights into the direct selective oxidation of methane to methanol over ZSM-5 zeolytes in aqueous hydrogen peroxide

Cited by 13 publications

References 50 publications

Irregularly Shaped NiO Nanostructures for Catalytic Lean Methane Combustion

Irregularly Shaped NiO Nanostructures for Catalytic Lean Methane Combustion

The Direct Synthesis of H2O2 and Selective Oxidation of Methane to Methanol Using HZSM-5 Supported AuPd Catalysts

Harnessing of Diluted Methane Emissions by Direct Partial Oxidation of Methane to Methanol over Cu/Mordenite

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