Chemische Batterien mit CO<sub>2</sub>

Schlögl, Robert

doi:10.1002/ange.202007397

Cited by 3 publications

(2 citation statements)

References 279 publications

(124 reference statements)

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“…Methanol is a central pivot in the chemical supply chain and an important energy carrier for combustion engines or fuel cells. 1 − 8 The synthetic potential ranges from the production of base chemicals such as propylene or aromatics to application as a C1 building block to produce fine chemicals and pharmaceuticals. 9 − 11 Global methanol production is on the order of 100 million metric tons annually, using mainly coal and natural gas as primary feedstocks.…”

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confidence: 99%

Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts

Kaithal

Werlé

Leitner

2021

JACS Au

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Alcohol-assisted hydrogenation of carbon monoxide (CO) to methanol was achieved using homogeneous molecular complexes. The molecular manganese complex [Mn(CO) 2 Br[HN(C 2 H 4 P i Pr 2 ) 2 ]] ([HN(C 2 H 4 P i Pr 2 ) 2 ] = MACHO- i Pr) revealed the best performance, reaching up to turnover number = 4023 and turnover frequency 857 h –1 in EtOH/toluene as solvent under optimized conditions ( T = 150 °C, p (CO/H 2 ) = 5/50 bar, t = 8–12 h). Control experiments affirmed that the reaction proceeds via formate ester as the intermediate, whereby a catalytic amount of base was found to be sufficient to mediate its formation from CO and the alcohol in situ . Selectivity for methanol formation reached >99% with no accumulation of the formate ester. The reaction was demonstrated to work with methanol as the alcohol component, resulting in a reactive system that allows catalytic “breeding” of methanol without any coreagents.

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confidence: 99%

Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts

Kaithal

Werlé

Leitner

2021

JACS Au

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“…1,2 Moreover, the energy generated from renewable sources has to be stored in certain "chemical batteries" before usage. 3 With a high volumetric energy density (4.33 kW h L −1 ), methanol is an ideal candidate for chemical energy storage, which can be produced by CO 2 hydrogenation with hydrogen derived from water electrolysis. 4 Copper-based systems are the most extensively investigated catalysts for methanol synthesis and are already applied in the industry for the hydrogenation of CO/CO 2 mixtures derived from fossil fuels [eqs 1 and 2] 5 (1)…”

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confidence: 99%

Laser-Generated InO_x/ZrO₂ Catalysts for CO₂ Hydrogenation: Role of In Situ Fragmentation and Ripening Control

Lau

Schühle

Liang

et al. 2021

ACS Appl. Energy Mater.

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It is desirable to reduce the reliance on fossil fuels and to develop alternative methods to yield valuable chemicals. CO2 hydrogenation to methanol is a promising approach, where In2O3/ZrO2 catalysts have attracted increasing attention due to their high selectivity and stability. However, the activity of indium-based catalysts is very susceptible to the preparation method, which is typically wet impregnation. Here, we explore a laser-based synthesis route to prepare InO x /ZrO2 catalysts of varying indium size and load. The respective particle sizes were either adjusted by in situ fragmentation with a more (ns-VIS-laser) or less (ns-IR-laser) efficient laser wavelength or by using micromolar concentrations of phosphate as an electrostatic stabilizer. The InO x colloids were subsequently deposited onto ZrO2 Our results demonstrate that the pulsed laser ablation with ns-IR-laser pulses yielded larger ∼45 nm crystalline cuboid InO x supported on zirconia. The frequency-doubled ns-VIS-pulses on the other hand caused an augmented in situ fragmentation during ablation, which led to catalysts with spherical ∼14 nm InO x particles with a significantly higher degree of amorphousness. Further size quenching and increased amorphous content of the InO x nanoparticles were observed when micromolar concentrations of phosphates were additionally present during ablation. After supporting the InO x nanoparticles onto ZrO2, the laser-generated catalysts were found to perform equally well as their wet-chemically prepared counterparts for methanol synthesis in a slurry phase, although crystalline In species performed slightly better in the catalytic reaction. In conclusion, in situ fragmentation does not only provide opportunities for independent studies of size and composition but also ripening control and structural modifications such as amorphization.

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Acceptorless Dehydrogenation of Methanol to Carbon Monoxide and Hydrogen using Molecular Catalysts

et al. 2021

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The acceptorless dehydrogenation of methanol to carbon monoxide and hydrogen was investigated using homogeneous molecular complexes. Complexes of ruthenium and manganese comprising the MACHO ligand framework showed promising activities for this reaction. The molecular ruthenium complex [RuH(CO)(BH 4 )(HN(C 2 H 4 PPh 2 ) 2 )] (Ru-MACHO-BH) achieved up to 3150 turnovers for carbon monoxide and 9230 turnovers for hydrogen formation at 150 8C reaching pressures up to 12 bar when the decomposition was carried out in a closed vessel. Control experiments affirmed that the metal complex mediates the initial fast dehydrogenation of methanol to formaldehyde and methyl formate followed by subsequent slow decarbonylation. Depending on the catalyst and reaction conditions, the CO/ H 2 ratio in the gas mixture thus varies over a broad range from almost pure hydrogen to the stoichiometric limit of 1:2.

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Chemische Batterien mit CO₂

Abstract: zu finden. 2020 Die Autoren. Verçffentlicht von Wiley-VCH GmbH. Dieser Open Access Beitrag steht unter den Bedingungend er Creative Commons AttributionL icense, die jede Nutzung des Beitragesi n allen Medien gestattet, sofern der ursprüngliche Beitrag ordnungsgemäßzitiert wird.

Cited by 3 publications

References 279 publications

Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts

Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts

Laser-Generated InO_x/ZrO₂ Catalysts for CO₂ Hydrogenation: Role of In Situ Fragmentation and Ripening Control

Acceptorless Dehydrogenation of Methanol to Carbon Monoxide and Hydrogen using Molecular Catalysts

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Chemische Batterien mit CO2

Abstract: zu finden. 2020 Die Autoren. Verçffentlicht von Wiley-VCH GmbH. Dieser Open Access Beitrag steht unter den Bedingungend er Creative Commons AttributionL icense, die jede Nutzung des Beitragesi n allen Medien gestattet, sofern der ursprüngliche Beitrag ordnungsgemäßzitiert wird.

Cited by 3 publications

References 279 publications

Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts

Alcohol-Assisted Hydrogenation of Carbon Monoxide to Methanol Using Molecular Manganese Catalysts

Laser-Generated InOx/ZrO2 Catalysts for CO2 Hydrogenation: Role of In Situ Fragmentation and Ripening Control

Acceptorless Dehydrogenation of Methanol to Carbon Monoxide and Hydrogen using Molecular Catalysts

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Chemische Batterien mit CO₂

Laser-Generated InO_x/ZrO₂ Catalysts for CO₂ Hydrogenation: Role of In Situ Fragmentation and Ripening Control