Strategies for the Direct Catalytic Valorization of Methane Using Heterogeneous Catalysis: Challenges and Opportunities

Suarez, Alma I. Olivos; Szécsényi, Àgnes; Hensen, Emiel Emiel; Ruiz‐Martínez, Javier; Pidko, Evgeny A.; Gascón, Jorge

doi:10.1021/acscatal.6b00428

Cited by 463 publications

(331 citation statements)

References 174 publications

Supporting

Mentioning

321

Contrasting

Unclassified

Order By: Relevance

“…Developing an alternative process to produce value‐added chemicals such as methanol from methane, preferably in one step, has therefore been a research field of increasing interest in recent years. Unfortunately, direct oxidation strategies showed low yields and productivity due to the much higher reactivity of the oxygenated products compared to methane . Efficient activation of methane under milder conditions and control of reaction selectivity toward the desired products are therefore the main challenges in heterogeneous catalysis.…”

Section: Introductionsupporting

confidence: 89%

Stepwise Methane‐to‐Methanol Conversion on CuO/SBA‐15

Parishan

Sagaltchik

et al. 2018

Chemistry A European J

View full text Add to dashboard Cite

The direct partial oxidation of methane to methanol is a challenging scientific and economical objective to expand the application of this abundant fuel gas as a major resource for one-step production of value-added chemicals. Despite substantial efforts to commercialize this synthetic route, to date no heterogeneous catalyst can selectively oxidize methane to methanol by O with an economically acceptable conversion. Cu-exchanged zeolites have been recently highlighted as one of the most promising bioinspired catalysts toward the direct production of methanol from methane under mild conditions. In this work, Cu-based catalysts were prepared using mesoporous silica SBA-15 as an alternative support and their activity for this conversion was investigated. The results demonstrate that highly dispersed CuO species on SBA-15 are able to react with methane and subsequently produce methanol with high selectivity (>84 %) through water-assisted extraction. Furthermore, it was confirmed that the main intermediate formed after interaction of the catalyst with methane is a methoxyl species, which can be further converted to methanol or dimethyl ether on extraction with water or methanol, respectively.

show abstract

Section: Introductionsupporting

confidence: 89%

Stepwise Methane‐to‐Methanol Conversion on CuO/SBA‐15

Parishan

Sagaltchik

et al. 2018

Chemistry A European J

View full text Add to dashboard Cite

show abstract

“…Currently methane is converted into various chemicals indirectly via syngas, a mixture of CO and H 2 , which can be synthesized typically through an energy intensive steam reforming reaction (CH 4 +H 2 O↔CO+3H 2 , ΔH° 298K =206 kJ/mol) at high temperatures. To circumvent this energy‐consuming process, the direct conversion of methane has been sought in different ways but these effects have so far failed to be cost‐competitive with an indirect pathway . In particular, the direct oxidation of methane into methane oxygenates such as methanol, formaldehyde, and formic acid under mild conditions is still challenging …”

Section: Catalytic Performance For the Selective Oxidation Of Methanementioning

confidence: 99%

Aqueous‐Phase Selective Oxidation of Methane with Oxygen over Iron Salts and Pd/C in the Presence of Hydrogen

Kang

Park

2019

ChemCatChem

View full text Add to dashboard Cite

Direct conversion of methane into value‐added chemicals is a challenging but worthwhile subject. In this communication, the direct conversion of methane into methane oxygenates was achieved in an aqueous solution at room temperature using iron salts and Pd/C as catalysts and hydrogen peroxide as an oxidant. The hydrogen peroxide can be directly added or generated in situ from hydrogen and oxygen. The Pd/C catalyst greatly enhanced the reaction rate together with the iron salts. The effect of some parameters such as reaction temperature, reaction time, pH, acid type, and catalyst amount on the yields of the methane oxygenates was also investigated. When hydrogen peroxide was directly added, the turnover frequency (TOF), defined as the moles of methane oxygenates per moles of Fe per unit time, at 293 K was 29 h−1 at pH=2.3. The TOF at 293 K was 42 h−1 at pH=1.3 with in situ generated hydrogen peroxide from hydrogen and oxygen.

show abstract

“…[8] Consequently,w eu se Mo:Al f % 0.25 (ca. [18,19] Raman spectroscopy,H AADF-STEM, and chemical transients (Figure 1a-c) reported herein exhibit evolution of catalyst structure during CH 4 DHA. [18,19] Raman spectroscopy,H AADF-STEM, and chemical transients (Figure 1a-c) reported herein exhibit evolution of catalyst structure during CH 4 DHA.…”

mentioning

confidence: 62%

Absorptive Hydrogen Scavenging for Enhanced Aromatics Yield During Non‐oxidative Methane Dehydroaromatization on Mo/H‐ZSM‐5 Catalysts

et al. 2018

View full text Add to dashboard Cite

Addition of Zr metal particles to MoC x /ZSM-5 in interpellet mixtures (2:1 weight ratio) resulted in maximum single-pass methane conversion of 27 %f or dehydroaromatization at 973 K( in significant excess of the equilibrium prescribed circa 10 %c onversion at these conditions) and ac oncurrent 1.4-5.6-fold increase in aromatic product yields due to circumvention of thermodynamic equilibrium limitations by absorptive H 2 removal by Zr while retaining cumulative aromatic product selectivity.T he absorptive function of the polyfunctional catalyst formulation can be regenerated by thermal treatment in He flowa t9 73 K, yielding above-equilibrium methane conversion in successive regeneration cycles.H 2 uptake experiments demonstrate formation of bulk ZrH 1.75 on hydrogen absorption by Zr at 973 K. Cooperation between absorption and catalytic centers distinct in location and function enables circumvention of persistent thermodynamic challenges in non-oxidative methane dehydrogenation.

show abstract

Strategies for the Direct Catalytic Valorization of Methane Using Heterogeneous Catalysis: Challenges and Opportunities

Cited by 463 publications

References 174 publications

Stepwise Methane‐to‐Methanol Conversion on CuO/SBA‐15

Stepwise Methane‐to‐Methanol Conversion on CuO/SBA‐15

Aqueous‐Phase Selective Oxidation of Methane with Oxygen over Iron Salts and Pd/C in the Presence of Hydrogen

Absorptive Hydrogen Scavenging for Enhanced Aromatics Yield During Non‐oxidative Methane Dehydroaromatization on Mo/H‐ZSM‐5 Catalysts

Contact Info

Product

Resources

About