TY - JOUR
T1 - Commercial Gold Complexes Supported on Functionalised Carbon Materials as Efficient Catalysts for the Direct Oxidation of Ethane to Acetic Acid
AU - Ribeiro, Ana P. C.
AU - Matias, Inês A. S.
AU - Carabineiro, Sónia A. C.
AU - Martins, Luísa M. D. R. S.
N1 - UIDB/00100/2020
UIDP/00100/2020
LA/P/0056/2020
IST-ID/119/2018
SFRH/BD/146426/2019
CEEC-INST/00102/2018
UIDB/50006/2020
UIDP/50006/2020
Base-UIDB/50020/2020
Programmatic-UIDP/50020/2020
PY - 2022/2
Y1 - 2022/2
N2 - The single-pot efficient oxidation of ethane to acetic acid catalysed by Au(I) or Au(III) compounds, chlorotriphenylphosphinegold(I) (1), chlorotrimethylphosphinegold(I) (2), 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidenegold(I) chloride (3), dichloro(2-pyridinecarboxylato)gold(III) (4), homogenous and supported on different carbon materials: activated carbon (AC), multi-walled carbon nanotubes (CNT) and carbon xerogel (CX), oxidised with nitric acid followed by treatment with NaOH (-ox-Na), is reported. The reactions were performed in water/acetonitrile. The materials were selective for the production of acetic acid, with no trace of by-products being detected. The best homogenous catalysts were complexes 2 and 3 which showed the highest ethane conversion and an acetic acid yield of ca. 21%, followed by 4 and 1. The heterogenised materials showed much better activity than the homogenous counterparts, with acetic acid yields up to 41.4% for 4@CNT-ox-Na, and remarkable selectivity (with acetic acid being the only product detected). The heterogenised catalysts with the best results were reused up to five cycles, with no significant loss of activity, and maintaining high selectivity for acetic acid. 4@CNT-ox-Na showed not only the best catalytic activity but also the best stability during the recycling runs.
AB - The single-pot efficient oxidation of ethane to acetic acid catalysed by Au(I) or Au(III) compounds, chlorotriphenylphosphinegold(I) (1), chlorotrimethylphosphinegold(I) (2), 1,3-bis(2,6-diisopropylphenyl)imidazol-2-ylidenegold(I) chloride (3), dichloro(2-pyridinecarboxylato)gold(III) (4), homogenous and supported on different carbon materials: activated carbon (AC), multi-walled carbon nanotubes (CNT) and carbon xerogel (CX), oxidised with nitric acid followed by treatment with NaOH (-ox-Na), is reported. The reactions were performed in water/acetonitrile. The materials were selective for the production of acetic acid, with no trace of by-products being detected. The best homogenous catalysts were complexes 2 and 3 which showed the highest ethane conversion and an acetic acid yield of ca. 21%, followed by 4 and 1. The heterogenised materials showed much better activity than the homogenous counterparts, with acetic acid yields up to 41.4% for 4@CNT-ox-Na, and remarkable selectivity (with acetic acid being the only product detected). The heterogenised catalysts with the best results were reused up to five cycles, with no significant loss of activity, and maintaining high selectivity for acetic acid. 4@CNT-ox-Na showed not only the best catalytic activity but also the best stability during the recycling runs.
KW - Acetic acid
KW - Carbon
KW - Ethane oxidation
KW - Gold
KW - Heterogeneous catalysis
UR - http://www.scopus.com/inward/record.url?scp=85123540078&partnerID=8YFLogxK
U2 - 10.3390/catal12020165
DO - 10.3390/catal12020165
M3 - Article
AN - SCOPUS:85123540078
SN - 2073-4344
VL - 12
JO - Catalysts
JF - Catalysts
IS - 2
M1 - 165
ER -