TY - JOUR

T1 - Ethanol dehydrogenation to acetaldehyde over Co@N-doped carbon

AU - Chernov, Aleksey N.

AU - Astrakova, Tatiana V.

AU - Koltunov, Konstantin Yu

AU - Sobolev, Vladimir I.

N1 - Funding Information: Funding: This work was supported by the Ministry of Science and Higher Education of the Russian Federation within the governmental order for Boreskov Institute of Catalysis (project AAAA-A21-121011390008-4). Publisher Copyright: © 2021 by the authors. Licensee MDPI, Basel, Switzerland.

PY - 2021/11

Y1 - 2021/11

N2 - Cobalt and nitrogen co-doped carbon materials (Co@CN) have recently attracted significant attention as highly efficient noble-metal-free catalysts exhibiting a large application range. In a similar research interest, and taking into account the ever-increasing importance of bioethanol as a renewable raw material, here, we report the results on ethanol dehydrogenation to acetaldehyde over Co@NC catalysts. The catalyst samples were synthesized by a variety of affordable techniques, ensuring generation of various types of Co species incorporated in carbon, such as subnanosized cobalt sites and nano-sized particles of metallic cobalt and cobalt oxides. The catalytic activity was tested under both oxidative and non-oxidative gas-phase conditions at 200–450 °C using a fixed-bed flow reactor. The non-oxidative conditions proved to be much more preferable for the target reaction, competing, however, with ethanol dehydration to ethylene. Under specified reaction conditions, ethanol conversion achieved a level of 66% with 84% selectivity to acetaldehyde at 400 °C. The presence of molecular oxygen in the feed led mainly to deep oxidation of ethanol to COx, giving acetaldehyde in a comparatively low yield. The potential contribution of carbon itself and supported cobalt forms to the observed reaction pathways is discussed.

AB - Cobalt and nitrogen co-doped carbon materials (Co@CN) have recently attracted significant attention as highly efficient noble-metal-free catalysts exhibiting a large application range. In a similar research interest, and taking into account the ever-increasing importance of bioethanol as a renewable raw material, here, we report the results on ethanol dehydrogenation to acetaldehyde over Co@NC catalysts. The catalyst samples were synthesized by a variety of affordable techniques, ensuring generation of various types of Co species incorporated in carbon, such as subnanosized cobalt sites and nano-sized particles of metallic cobalt and cobalt oxides. The catalytic activity was tested under both oxidative and non-oxidative gas-phase conditions at 200–450 °C using a fixed-bed flow reactor. The non-oxidative conditions proved to be much more preferable for the target reaction, competing, however, with ethanol dehydration to ethylene. Under specified reaction conditions, ethanol conversion achieved a level of 66% with 84% selectivity to acetaldehyde at 400 °C. The presence of molecular oxygen in the feed led mainly to deep oxidation of ethanol to COx, giving acetaldehyde in a comparatively low yield. The potential contribution of carbon itself and supported cobalt forms to the observed reaction pathways is discussed.

KW - Acetaldehyde

KW - Cobalt-nitrogen-carbon catalyst

KW - Dehy-drogenation

KW - Ethanol conversion

KW - Heterogeneous catalysis

UR - http://www.scopus.com/inward/record.url?scp=85119333002&partnerID=8YFLogxK

U2 - 10.3390/catal11111411

DO - 10.3390/catal11111411

M3 - Article

AN - SCOPUS:85119333002

VL - 11

JO - Catalysts

JF - Catalysts

SN - 2073-4344

IS - 11

M1 - 1411

ER -