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1.
iScience ; 25(4): 104011, 2022 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-35340428

RESUMO

For the efficient electrochemical conversion of CO2 into valuable chemical feedstocks, a well-coordinated interaction of all electrolyzer compartments is required. In addition to the catalyst, whose role is described in detail in the part "Electrochemical CO2 Reduction toward Multicarbon Alcohols - The Microscopic World of Catalysts & Process Conditions" of this divided review, the general cell setups, design and manufacture of the electrodes, membranes used, and process parameters must be optimally matched. The authors' goal is to provide a comprehensive review of the current literature on how these aspects affect the overall performance of CO2 electrolysis. To be economically competitive as an overall process, the framework conditions, i.e., CO2 supply and reaction product treatment must also be considered. If the key indicators for current density, selectivity, cell voltage, and lifetime of a CO2 electrolyzer mentioned in the techno-economic consideration of this review are met, electrochemical CO2 reduction can make a valuable contribution to the creation of closed carbon cycles and to a sustainable energy economy.

2.
iScience ; 25(4): 104010, 2022 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-35345454

RESUMO

Tackling climate change is one of the undoubtedly most important challenges at the present time. This review deals mainly with the chemical aspects of the current status for converting the greenhouse gas CO2 via electrochemical CO2 reduction reaction (CO2RR) to multicarbon alcohols as valuable products. Feasible reaction routes are presented, as well as catalyst synthesis methods such as electrodeposition, precipitation, or sputtering. In addition, a comprehensive overview of the currently achievable selectivities for multicarbon alcohols in CO2RR is given. It is also outlined to what extent, for example, modifications of the catalyst surfaces or the use of bifunctional compounds the product distribution is shifted. In addition, the influence of varying electrolyte, temperature, and pressure is described and discussed.

3.
ACS Omega ; 7(47): 42994-43005, 2022 Nov 29.
Artigo em Inglês | MEDLINE | ID: mdl-36467945

RESUMO

The conversion of syngas into value-added hydrocarbons gains increasing attention due to its potential to produce sustainable platform chemicals from simple starting materials. Along this line, the "OX-ZEO" process that combines a methanol synthesis catalyst with a zeolite, capable of catalyzing the methanol-to-hydrocarbon reaction, was found to be a suitable alternative to the classical Fischer-Tropsch synthesis. Hitherto, understanding the mechanism of the OX-ZEO process and simultaneously optimizing the CO conversion and the selectivity toward a specific hydrocarbon remains challenging. Herein, we present a comparison of a variety of ZnCrAl oxides with different metal ratios combined with a H-ZSM-5 zeolite for the conversion of syngas to hydrocarbons. The effect of aluminum on the catalytic activity was investigated for ZnCrAl oxides with a Zn/Cr ratio of 4:1, 1:1, and 1:2. The product distribution and CO conversion were found to be strongly influenced by the Zn/Cr/Al ratio. Although a ratio of Zn/Cr of 1:2 was best to produce lower olefins and aromatics, with aromatic selectivities of up to 37%, catalysts with a 4:1 ratio revealed high paraffin selectivity up to 52%. Notably, a distinct effect of aluminum in the oxide lattice on the catalytic activity and product selectivity was observed, as a higher Al content leads to a lower CO conversion and a changed product spectrum. We provide additional understanding of the influence of different compositions of ZnCrAl oxides on their surface properties and the catalytic activity in the OX-ZEO process. Furthermore, the variation of the zeolite component supports the important role of the channel topology of the porous support material for the hydrocarbon production. In addition, variation of the gas hourly space velocity showed a correlation of contact time, CO conversion, and hydrocarbon selectivity. At a gas hourly space velocity of 4200 mL/gcat h, CO conversion as high as 44% along with a CO2 selectivity of 42% and a lower paraffin (C2 0-C4 0) selectivity of 41% was observed.

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