TY - JOUR
T1 - Intramolecular cyclization of alkynoic acid catalyzed by Na-salt-modified Au nanoparticles supported on metal oxides
AU - Huang, Qi An
AU - Ikeda, Takaaki
AU - Haruguchi, Kazuki
AU - Kawai, Seiya
AU - Yamamoto, Eiji
AU - Murayama, Haruno
AU - Ishida, Tamao
AU - Honma, Tetsuo
AU - Tokunaga, Makoto
N1 - Funding Information:
This work was financially supported by the ALCA program (No. 11102798 ) and JSPS KAKENHI (Grant Number 19H02755). XAFS experiments were performed at the BL14B2 of SPring-8 following the approval of the Japan Synchrotron Radiation Research Institute ( JASRI ; proposal Nos. 2018B1787 , 2019A1800 , 2020A1638 , and 2020A1769 ). STEM observations were performed at the Ultramicroscopy Research Center, Kyushu University . XPS measurements were supported by the Nanotechnology Platform Program (Molecule and Material Synthesis) of the Ministry of Education, Culture, Sports, Science and Technology ( MEXT ), Japan (Grant No. JPMXP09 S20KU0055 ).
Funding Information:
This work was financially supported by the ALCA program (No. 11102798) and JSPS KAKENHI (Grant Number 19H02755). XAFS experiments were performed at the BL14B2 of SPring-8 following the approval of the Japan Synchrotron Radiation Research Institute (JASRI; proposal Nos. 2018B1787, 2019A1800, 2020A1638, and 2020A1769). STEM observations were performed at the Ultramicroscopy Research Center, Kyushu University. XPS measurements were supported by the Nanotechnology Platform Program (Molecule and Material Synthesis) of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan (Grant No. JPMXP09 S20KU0055).
Publisher Copyright:
© 2022 Elsevier B.V.
PY - 2022/8/5
Y1 - 2022/8/5
N2 - Zirconia-supported sodium-salt-modified Au(0) nanoparticles (NPs) (Na-Au/ZrO2) catalyst was prepared, and it was stable and recyclable in the intramolecular cyclization of alkynoic acids. In particular, the effect of sodium species in Na-Au/ZrO2, which has been overlooked in previous studies, was studied, and they were found to play an essential role in the reaction. In addition, the relationship between the kinetics and size of Au NPs revealed that the active sites of the catalyst are located on the surface of the supported Au NPs. Moreover, detailed kinetic studies revealed that the cyclization was a zero-order reaction with respect to substrate concentration, and the rate-determining step of the reaction is presumed to be protodeauration. The maximum turnover number (TON) of the reaction of 5-hexynoic acid in a continuous flow reactor exceeded 9000, which is the highest TON obtained in the presence of a heterogeneous Au catalyst.
AB - Zirconia-supported sodium-salt-modified Au(0) nanoparticles (NPs) (Na-Au/ZrO2) catalyst was prepared, and it was stable and recyclable in the intramolecular cyclization of alkynoic acids. In particular, the effect of sodium species in Na-Au/ZrO2, which has been overlooked in previous studies, was studied, and they were found to play an essential role in the reaction. In addition, the relationship between the kinetics and size of Au NPs revealed that the active sites of the catalyst are located on the surface of the supported Au NPs. Moreover, detailed kinetic studies revealed that the cyclization was a zero-order reaction with respect to substrate concentration, and the rate-determining step of the reaction is presumed to be protodeauration. The maximum turnover number (TON) of the reaction of 5-hexynoic acid in a continuous flow reactor exceeded 9000, which is the highest TON obtained in the presence of a heterogeneous Au catalyst.
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U2 - 10.1016/j.apcata.2022.118765
DO - 10.1016/j.apcata.2022.118765
M3 - Article
AN - SCOPUS:85133629981
SN - 0926-860X
VL - 643
JO - Applied Catalysis A: General
JF - Applied Catalysis A: General
M1 - 118765
ER -