J 2023

Copper Phosphinate Complexes as Molecular Precursors for Ethanol Dehydrogenation Catalysts

POKORNÝ, Tomáš, Iaroslav DOROSHENKO, Petr MACHÁČ, Lucie ŠIMONÍKOVÁ, Miroslava BITTOVÁ et. al.

Basic information

Original name

Copper Phosphinate Complexes as Molecular Precursors for Ethanol Dehydrogenation Catalysts

Authors

POKORNÝ, Tomáš (203 Czech Republic, belonging to the institution), Iaroslav DOROSHENKO (203 Czech Republic, belonging to the institution), Petr MACHÁČ (203 Czech Republic, belonging to the institution), Lucie ŠIMONÍKOVÁ (203 Czech Republic, belonging to the institution), Miroslava BITTOVÁ (203 Czech Republic, belonging to the institution), Zdeněk MORAVEC (203 Czech Republic, belonging to the institution), Katerina KARASKOVA (203 Czech Republic), David ŠKODA (203 Czech Republic), Jiří PINKAS (203 Czech Republic, belonging to the institution) and Aleš STÝSKALÍK (203 Czech Republic, guarantor, belonging to the institution)

Edition

Inorganic Chemistry, WASHINGTON, American Chemical Society, 2023, 0020-1669

Other information

Language

English

Type of outcome

Článek v odborném periodiku

Field of Study

10402 Inorganic and nuclear chemistry

Country of publisher

United States of America

Confidentiality degree

není předmětem státního či obchodního tajemství

References:

Impact factor

Impact factor: 4.600 in 2022

RIV identification code

RIV/00216224:14310/23:00132907

Organization unit

Faculty of Science

UT WoS

001123849200001

Keywords in English

CONTINUOUS SYMMETRY MEASURES; CRYSTAL-STRUCTURES; MAGNETIC-PROPERTIES

Tags

International impact, Reviewed
Změněno: 11/4/2024 10:29, Mgr. Marie Šípková, DiS.

Abstract

V originále

Nowadays, the production of acetaldehyde heavily relies on the petroleum industry. Developing new catalysts for the ethanol dehydrogenation process that could sustainably substitute current acetaldehyde production methods is highly desired. Among the ethanol dehydrogenation catalysts, copper-based materials have been intensively studied. Unfortunately, the Cu-based catalysts suffer from sintering and coking, which lead to rapid deactivation with time-on-stream. Phosphorus doping has been demonstrated to diminish coking in methanol dehydrogenation, fluid catalytic cracking, and ethanol-to-olefin reactions. This work reports a pioneering application of the well-characterized copper phosphinate complexes as molecular precursors for copper-based ethanol dehydrogenation catalysts enriched with phosphate groups (Cu-phosphate/SiO2). Three new catalysts (CuP-1, CuP-2, and CuP-3), prepared by the deposition of complexes {Cu(SAAP)}(n) (1), [Cu-6(BSAAP)(6)] (2), and [Cu-3(NAAP)(3)] (3) on the surface of commercial SiO2, calcination at 500 degrees C, and reduction in the stream of the forming gas 5% H-2/N-2 at 400 degrees C, exhibited unusual properties. First, the catalysts showed a rapid increase in catalytic activity. After reaching the maximum conversion, the catalyst started to deactivate. The unusual behavior could be explained by the presence of the phosphate phase, which made Cu2+ reduction more difficult. The phosphorus content gradually decreased during time-on-stream, copper was reduced, and the activity increased. The deactivation of the catalyst could be related to the copper diffusion processes. The most active CuP-1 catalyst reaches a maximum of 73% ethanol conversion and over 98% acetaldehyde selectivity at 325 degrees C and WHSV = 2.37 h(-1).

Links

EF18_046/0015974, research and development project
Name: Modernizace České infrastruktury pro integrativní strukturní biologii
EH22_008/0004572, research and development project
Name: Kvantové materiály pro aplikace v udržitelných technologiích
GJ20-03636Y, research and development project
Name: Nové katalyzátory pro přípravu 1,3-butadienu z ethanolu
Investor: Czech Science Foundation
LM2018127, research and development project
Name: Česká infrastruktura pro integrativní strukturní biologii (Acronym: CIISB)
Investor: Ministry of Education, Youth and Sports of the CR
LM2023042, research and development project
Name: Česká infrastruktura pro integrativní strukturní biologii
Investor: Ministry of Education, Youth and Sports of the CR, CIISB - Czech Infrastructure for Integrative Structural Biology
MUNI/A/1209/2022, interní kód MU
Name: Molekuly, komplexy, makrocykly a xerogely
Investor: Masaryk University, Molecules, complexes, macrocycles, and xerogels
MUNI/A/1298/2022, interní kód MU
Name: Základní a aplikovaný výzkum a vývoj metod chemické a fyzikálně chemické analýzy pro studium přírody a pokročilé technologie
Investor: Masaryk University, Basic and applied research and development of chemical and physicochemical analytical methods for the study of nature and advanced technology
MUNI/J/0007/2021, interní kód MU
Name: Tailored Catalysts for Carbon Dioxide Utilization
Investor: Masaryk University, MASH JUNIOR - MUNI Award In Science and Humanities JUNIOR
90110, large research infrastructures
Name: CzechNanoLab
90242, large research infrastructures
Name: CIISB III