Critical evaluation of parameters affecting Cu nanoparticles formation and their activity in dimethyl adipate hydrogenolysis

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22310%2F22%3A43922238" target="_blank" >RIV/60461373:22310/22:43922238 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/60461373:22320/22:43922238 RIV/60461373:22350/22:43922238

Výsledek na webu

<a href="https://www.sciencedirect.com/science/article/pii/S092058612100420X?via%3Dihub" target="_blank" >https://www.sciencedirect.com/science/article/pii/S092058612100420X?via%3Dihub</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.cattod.2021.09.017" target="_blank" >10.1016/j.cattod.2021.09.017</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Critical evaluation of parameters affecting Cu nanoparticles formation and their activity in dimethyl adipate hydrogenolysis

Popis výsledku v původním jazyce

Supported copper catalysts are promising alternative to replace CuCr catalysts in ester hydrogenolysis and decrease the environmental footprint of the process. However, the effect of the support properties on the Cu nanoparticles formation and, consequently, on the final hydrogenolysis performance has not been investigated in detail. Therefore, we have selected 10 supports with different textural-structural properties and impregnated them by incipient wetness impregnation to achieve 8 wt% Cu loading. Although the silica-based supports provided much larger surface area to deposit Cu compared to ZnO, MgO, or TiO2, the final Cu dispersion was similar for these catalysts due to the insufficient electrostatic attraction. A significant improvement was observed when using ZrO2 as a support, while the best Cu dispersion was achieved using alumina-based supports. The reduced catalysts were tested in dimethyl adipate (DMA) hydrogenolysis to obtain hexane-1,6-diol (HDOL). Due to the good Cu dispersion ensured by ZrO2 and alumina supports, they outperformed the rest of the catalysts reaching the highest DMA conversion of 36 and 22–25%, respectively. Moreover, Cu-ZrO2 reached the highest hydrogenolysis activity (TOFH) due to a good copper-zirconia interaction. The maximum HDOL selectivity of about 8% was obtained over alumina-based catalysts. The increasing number of acid-base sites was found to be responsible for decreasing HDOL selectivity. Over these sites, a large amount of transesterification by-products (&lt;80%) and other side products were formed. Although the larger support surface area may ensure a better Cu dispersion, the acid-base sites or electrostatic attraction during impregnation play a key role by affecting the Cu nanoparticle formation and, consequently, the final catalyst performance. © 2021 Elsevier B.V.

Název v anglickém jazyce

Critical evaluation of parameters affecting Cu nanoparticles formation and their activity in dimethyl adipate hydrogenolysis

Popis výsledku anglicky

Supported copper catalysts are promising alternative to replace CuCr catalysts in ester hydrogenolysis and decrease the environmental footprint of the process. However, the effect of the support properties on the Cu nanoparticles formation and, consequently, on the final hydrogenolysis performance has not been investigated in detail. Therefore, we have selected 10 supports with different textural-structural properties and impregnated them by incipient wetness impregnation to achieve 8 wt% Cu loading. Although the silica-based supports provided much larger surface area to deposit Cu compared to ZnO, MgO, or TiO2, the final Cu dispersion was similar for these catalysts due to the insufficient electrostatic attraction. A significant improvement was observed when using ZrO2 as a support, while the best Cu dispersion was achieved using alumina-based supports. The reduced catalysts were tested in dimethyl adipate (DMA) hydrogenolysis to obtain hexane-1,6-diol (HDOL). Due to the good Cu dispersion ensured by ZrO2 and alumina supports, they outperformed the rest of the catalysts reaching the highest DMA conversion of 36 and 22–25%, respectively. Moreover, Cu-ZrO2 reached the highest hydrogenolysis activity (TOFH) due to a good copper-zirconia interaction. The maximum HDOL selectivity of about 8% was obtained over alumina-based catalysts. The increasing number of acid-base sites was found to be responsible for decreasing HDOL selectivity. Over these sites, a large amount of transesterification by-products (&lt;80%) and other side products were formed. Although the larger support surface area may ensure a better Cu dispersion, the acid-base sites or electrostatic attraction during impregnation play a key role by affecting the Cu nanoparticle formation and, consequently, the final catalyst performance. © 2021 Elsevier B.V.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

20704 - Energy and fuels

Projekt

<a href="/cs/project/GA20-28093S" target="_blank" >GA20-28093S: Nosičové hydrogenolýzní katalyzátory na bázi mědi</a><br>

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2022

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Catalysis Today

ISSN

0920-5861

e-ISSN

1873-4308

Svazek periodika

387

Číslo periodika v rámci svazku

1 March 2022

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

11

Strana od-do

61-71

Kód UT WoS článku

000753605400001

EID výsledku v databázi Scopus

2-s2.0-85116285877