Valorization of steel-work off-gases: Influence of impurities on the performance of Cu-based methanol synthesis catalyst

Heracleous, Eleni; Koidi, Vasiliki; Lappas, Angelos A.; Hauser, Alexander; Haag, Stéphane

doi:10.1016/j.cej.2022.136571

Cited by 6 publications

(8 citation statements)

References 43 publications

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“…Cu sintering has also been reported to cause severe deactivation 41,42. Our previous studies43 related thermal sintering with decreased methanol selectivity, due to disruption…”

mentioning

confidence: 87%

“…40 Cu sintering has also been reported to cause severe deactivation. 41,42 Our previous studies 43 related thermal sintering with decreased methanol selectivity, due to disruption of the Cu/ZnO synergy that is crucial for methanol synthesis but less important for the RWGS reaction. 44 Sorbent addition leads to higher activity and product yields in each reaction−regeneration cycle.…”

Section: Cyclic Stability and Effect Of Regenerationmentioning

confidence: 99%

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Experimental Investigation of Sorption-Enhanced CO₂ Hydrogenation to Methanol

Heracleous

Koidi

Lappas

2023

ACS Sustainable Chem. Eng.

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In this work, we investigate experimentally the use of zeolite 13X as an efficient water sorbent in the sorption-enhanced CO2 hydrogenation reaction over Cu/ZnO/Al2O3 under different operating conditions and over multiple reaction–regeneration cycles. Introduction of the solid sorbent along with the catalyst in the reactor leads to a prominent increase in the CO2 conversion and CH3OH yield. As the reaction proceeds, the sorbent gradually becomes saturated, the enhancement effect reduces, and the system eventually reaches the same steady state as with catalyst only. The CH3OH yield increase is higher than that of the CO2 conversion, indicating preferential enhancement of methanol production. This can be attributed to the partial co-adsorption of both methanol and water on zeolite 13X. The effects of reaction and regeneration temperature on the activity, product distribution, enhancement degree, and recyclability are also examined. The highest sorption enhancement occurs at 225 °C, with the methanol yield increasing by 115% compared to the conventional process. The cyclic stability is investigated by consecutive reaction–regeneration cycles. The correlation between activity reduction and textural properties of both the catalyst and sorbent as well as the zeolite’s ability to regenerate are explored. To that end, the effect of regeneration temperature on the products’ desorption is also examined.

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“…Cu sintering has also been reported to cause severe deactivation 41,42. Our previous studies43 related thermal sintering with decreased methanol selectivity, due to disruption…”

mentioning

confidence: 87%

Section: Cyclic Stability and Effect Of Regenerationmentioning

confidence: 99%

Experimental Investigation of Sorption-Enhanced CO₂ Hydrogenation to Methanol

Heracleous

Koidi

Lappas

2023

ACS Sustainable Chem. Eng.

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“…[157] Unlike the promotional effect mentioned above, the addition of Na 2 CO 3 poisoned the Cu/ZnO/Al 2 O 3 in CO 2 hydrogenation to CH 3 OH. [158] In particular, serious activity deterioration was caused by the reluctant desorption of CO 2 tightly bound to the surface basic sites and limited exposure of active sites blocked by Na 2 CO 3 . [159][160] Similar with A promoters, AE compounds are also effective modifier for the surface basicity of Al 2 O 3 .…”

Section: Alkali and Alkali Earth Metal Species (A/ae)mentioning

confidence: 99%

Applications of Al₂O₃‐Based Nano‐Catalysts in Thermocatalytic CO₂ Transformations: Impacts of Surface Acidity and Basicity

Qiu

Tan

et al. 2023

ChemCatChem

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Adsorption and activation of CO2 exert a profound impact on the catalytic conversion and stability in thermocatalytic CO2 transformations. To optimize the surface property of Al2O3‐based nano‐catalysts, various modifications focusing on the surface acidity and basicity have been applied and proven effective in promoting the CO2 adsorption and activation, thus enhancing the catalytic performances. In this Review, the beneficial effects of a series of modifications strategies (e. g., promoters and synthesis/treatment methods) on adjusting the surface acidity and basicity of Al2O3‐based nano‐catalysts were comprehensively summarized, covering nearly all types of thermocatalytic CO2 transformations (e. g., reforming and hydrogenation). Moreover, the structure‐performance relationships were discussed in depth by relating to the adsorption, activation and conversion of CO2, selectivity of targeted products as well as the coke resistance and lifespan of catalysts.

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“…In contrast, CZA-based catalysts are strongly deactivated by H 2 S, which blocks part of the Cu active sites, hence reducing the surface area and therefore leading to a significant decrease of carbon conversion. The extent of the activity loss is proportional to the sulfur molar concentration accumulated on the catalyst [178,179,199]. An impurity level of H 2 S should be lower than 0.1 ppm in order to avoid catalyst poisoning [180].…”

Section: Tolerance Of the Catalyst To Syngas Impuritiesmentioning

confidence: 99%

“…The occurrence of water as a by-product of catalytic methanol synthesis depends, among other things, on the substrate gas. When working with CO 2 -rich syngas, water is formed via both methanol synthesis and reverse WGSR, leading to reduced productivities [199,218]. Further by-products occur at hot reactor zones [12].…”

Section: Intermediates and By-productsmentioning

confidence: 99%

CO_xFixation to Elementary Building Blocks: Anaerobic Syngas Fermentation vs. Chemical Catalysis

Perret

Campos

Delgado

et al. 2022

Chemie Ingenieur Technik

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Heterogeneous catalysis and anaerobic syngas fermentation represent two different approaches for the conversion of synthesis gas into chemicals and fuels. This review provides a unique comparison of different reaction paths for the fixation of CO 2 , CO and H 2 into elementary building blocks such as methanol, acetic acid and ethanol. Operating conditions, reactor engineering, influence of gas impurities, yields, conversion efficiencies as well as downstream product recovery are compared. It was found that mass-specific productivity ranges in the same order of magnitude for both technologies, while space-time yield of heterogeneous catalysis is up to three orders of magnitude higher.

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Valorization of steel-work off-gases: Influence of impurities on the performance of Cu-based methanol synthesis catalyst

Cited by 6 publications

References 43 publications

Experimental Investigation of Sorption-Enhanced CO₂ Hydrogenation to Methanol

Experimental Investigation of Sorption-Enhanced CO₂ Hydrogenation to Methanol

Applications of Al₂O₃‐Based Nano‐Catalysts in Thermocatalytic CO₂ Transformations: Impacts of Surface Acidity and Basicity

CO_xFixation to Elementary Building Blocks: Anaerobic Syngas Fermentation vs. Chemical Catalysis

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Valorization of steel-work off-gases: Influence of impurities on the performance of Cu-based methanol synthesis catalyst

Cited by 6 publications

References 43 publications

Experimental Investigation of Sorption-Enhanced CO2 Hydrogenation to Methanol

Experimental Investigation of Sorption-Enhanced CO2 Hydrogenation to Methanol

Applications of Al2O3‐Based Nano‐Catalysts in Thermocatalytic CO2 Transformations: Impacts of Surface Acidity and Basicity

COxFixation to Elementary Building Blocks: Anaerobic Syngas Fermentation vs. Chemical Catalysis

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Product

Resources

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Experimental Investigation of Sorption-Enhanced CO₂ Hydrogenation to Methanol

Experimental Investigation of Sorption-Enhanced CO₂ Hydrogenation to Methanol

Applications of Al₂O₃‐Based Nano‐Catalysts in Thermocatalytic CO₂ Transformations: Impacts of Surface Acidity and Basicity

CO_xFixation to Elementary Building Blocks: Anaerobic Syngas Fermentation vs. Chemical Catalysis