Insight into methanol synthesis from CO2 hydrogenation on Cu(111): Complex reaction network and the effects of H2O

Zhao, Ya‐Fan; Yang, Yong; Mims, Charles A.; Peden, Charles H. F.; Li, Jun; Mei, Donghai

doi:10.1016/j.jcat.2011.04.012

Cited by 376 publications

(413 citation statements)

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“…Methanol is one of the main CO2 hydrogenation products 2,6 which can be directly dehydrated to DME in a single batch reaction. Both these molecules are valuable alternative fuels 2,[7][8][9] and they are also used as feedstocks and intermediates for producing various chemicals and as energy carriers for fuel cells 7,[10][11][12] . Methanol can typically be produced from synthesis gas at a pressure between 50-100 bar and at a temperature between 200-300 °C 6,[12][13][14] .…”

Section: Introductionmentioning

confidence: 99%

Time evolution of the CO2 hydrogenation to fuels over Cu-Zr-SBA-15 catalysts

Atakan

Erdtman

Mäkie

et al. 2018

Journal of Catalysis

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The self-archived postprint version of this journal article is available at Linköping University Institutional Repository (DiVA): http://urn.kb.se/resolve?urn=urn:nbn:se:liu:diva-147297 N.B.: When citing this work, cite the original publication.Atakan, A., Erdtman, E., Mäkie, P., Ojamäe, L., Odén, M., (2018) ABSTRACT: Time evolution of catalytic CO2 hydrogenation to methanol and dimethyl ether (DME) has been investigated in a hightemperature high-pressure reaction chamber where products accumulate over time. The employed catalysts are based on a nano-assembly composed of Cu nanoparticles infiltrated into a Zr doped SiOx mesoporous framework (SBA-15): Cu-Zr-SBA-15. The CO2 conversion was recorded as a function of time by gas chromatography-mass spectrometry (GC-MS) and the molecular activity on the catalyst's surface was examined by diffuse reflectance in-situ Fourier transform infrared spectroscopy (DRIFTS). The experimental results showed that after 14 days a CO2 conversion of 25% to methanol and DME was reached when a DME selective catalyst was used which was also illustrated by thermodynamic equilibrium calculations. With higher Zr content in the catalyst, greater selectivity for methanol and a total 9.5 % conversion to methanol and DME was observed, yielding also CO as an additional product. The time evolution profiles indicated that DME is formed directly from methoxy groups in this reaction system. Both DME and methanol selective systems show the thermodynamically highest possible conversion.

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Section: Introductionmentioning

confidence: 99%

Time evolution of the CO2 hydrogenation to fuels over Cu-Zr-SBA-15 catalysts

Atakan

Erdtman

Mäkie

et al. 2018

Journal of Catalysis

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“…It has been suggested, however, by recent calculations [24] that formyl formation by reaction of *CO and *H is unlikely. Zhao et al [19] also suggested that formation of *H 2 CO is much more favored than *HCOH by hydrogenation of *HCO, and *H 2 CO will readily desorb to form formaldehyde, which has not been observed experimentally. Thus, the RWGS mechanism is also questionable.…”

Section: Key Intermediates and Elementary Stepsmentioning

confidence: 98%

“…Formyl is rather unstable and can be readily hydrogenated to form the more stable methoxy species, which can be further hydrogenated to produce methanol [5]. Regarding the elementary steps, three mechanisms, namely the formate mechanism, the reverse water-gas shift reaction (RWGS) mechanism, and the hydrocarboxyl mechanism have been proposed [18] [19], as shown in Figure 3. The formate mechanism suggests that chemisorbed formate on Cu sites can be produced from reaction of dissociated surface hydrogen and weakly bound CO 2 .…”

Section: Key Intermediates and Elementary Stepsmentioning

confidence: 99%

“…Production of ethers such as DME is favored over acidic catalysts and greatly inhibited by water. The catalyst activity towards methanol and higher alcohol synthesis will also be inhibited by water, although Zhao et al [19] suggested that methanol synthesis is strongly favored in the presence of small amount of water at the beginning of the reaction. Formation of higher alcohols is generally found inhibited by increasing CO 2 amount [40].…”

Section: Kinetics Of Ethanol Formationmentioning

confidence: 99%

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Revisiting Catalyst Structure and Mechanism in Methanol Synthesis

Wu¹,

Cole²,

Fang³

et al. 2017

JAN

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Abstract. Methanol synthesis is a mature industrial process, where industrial Cu/ZnO/Al 2 O 3 catalyst is commonly used. Howerver, function of the active catalyst component and reaction mechanism is still vague. In this contribution, the function of each catalyst component including the synergy between Cu and ZnO, reaction mechanism including carbon source of methanol, key intermediates and elementary steps, and kinetics of methanol synthesis and impurities formation are discussed based on the latest literature survey.

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“…Both options create novel demands on stability and productivity of the Cu-ZnO based catalyst. We have good insight into the mechanism of synthesis of MeOH over bare Cu surfaces [94,95] and use this as basis for design and performance estimation of practical catalysts. We have also found optimized synthesis routes to catalysts of technical scalability [96][97][98].…”

Section: The Chemical Toolbox Of Cecmentioning

confidence: 99%

Sustainable Energy Systems: The Strategic Role of Chemical Energy Conversion

Schlögl

2016

Top Catal

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In our globalized economy a multitude of energy systems are in operation. They present quite different structures and targets despite their common goal of supplying the energy needs for all societal activities reflecting the different boundary conditions of respective societies. The common quest for sustainability has given renewable electricity and ''solar fuels'' a high attention. The paper describes some underlying systemic aspects of integrating renewable with fossil energy and makes the point that without chemical energy conversion (CEC) this target will not be possible. A non-exhaustive list of grand challenges in CEC is derived. Some aspects of chemical energy science are discussed.

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Insight into methanol synthesis from CO2 hydrogenation on Cu(111): Complex reaction network and the effects of H2O

Cited by 376 publications

References 59 publications

Time evolution of the CO2 hydrogenation to fuels over Cu-Zr-SBA-15 catalysts

Time evolution of the CO2 hydrogenation to fuels over Cu-Zr-SBA-15 catalysts

Revisiting Catalyst Structure and Mechanism in Methanol Synthesis

Sustainable Energy Systems: The Strategic Role of Chemical Energy Conversion

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