TY - JOUR
T1 - Selective Oxidation of Methane to Formaldehyde over a Silica-Supported Cobalt Single-Atom Catalyst
AU - Ohyama, Junya
AU - Abe, Daiki
AU - Hirayama, Airi
AU - Iwai, Hiroki
AU - Tsuchimura, Yuka
AU - Sakamoto, Kazuki
AU - Irikura, Momoka
AU - Nakamura, Yuri
AU - Yoshida, Hiroshi
AU - Machida, Masato
AU - Nishimura, Shun
AU - Yamamoto, Tomokazu
AU - Matsumura, Syo
AU - Takahashi, Keisuke
N1 - Funding Information:
This work was funded in part by the Japan Science and Technology Agency (JST) CREST (JPMJCR17P2), the Japan Society for the Promotion of Science (JSPS) KAKENHI through a Grant-in-Aid for Scientific Research (B) (20H02524), and Advanced Characterization Platform of the Nanotechnology Platform Japan (JPMXP09 A20KU0371) sponsored by the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. The XAFS experiment was conducted on BL11 at the Saga Light Source (proposal no. 2005041R).
Publisher Copyright:
© Authors 2022
PY - 2022/2/3
Y1 - 2022/2/3
N2 - Catalytic oxidation of methane to formaldehyde and methanol has attracted attention because of its advantage in energy efficiency over the conventional multistep reaction process involving endothermic steam reforming of CH4; however, it is challenging to selectively obtain the partial oxidation products in the direct oxidation of CH4. In the present study, Co/SiO2 with various Co loadings was tested for the CH4/O2/H2O gas flow reaction. As a result, Co/SiO2 with a low loading of ≤0.1 wt % showed high selectivity for the partial oxidation reaction and mainly produced HCHO, while Co/SiO2 with high Co loadings proceeded to complete oxidation. Structural analysis using X-ray absorption fine-structure spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, and scanning transmission electron microscopy suggested that single Co atoms generated at low Co loadings were effective in the selective oxidation of CH4 to HCHO, while Co3O4 nanoparticles generated at high Co loadings promoted the complete oxidation.
AB - Catalytic oxidation of methane to formaldehyde and methanol has attracted attention because of its advantage in energy efficiency over the conventional multistep reaction process involving endothermic steam reforming of CH4; however, it is challenging to selectively obtain the partial oxidation products in the direct oxidation of CH4. In the present study, Co/SiO2 with various Co loadings was tested for the CH4/O2/H2O gas flow reaction. As a result, Co/SiO2 with a low loading of ≤0.1 wt % showed high selectivity for the partial oxidation reaction and mainly produced HCHO, while Co/SiO2 with high Co loadings proceeded to complete oxidation. Structural analysis using X-ray absorption fine-structure spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, and scanning transmission electron microscopy suggested that single Co atoms generated at low Co loadings were effective in the selective oxidation of CH4 to HCHO, while Co3O4 nanoparticles generated at high Co loadings promoted the complete oxidation.
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U2 - 10.1021/acs.jpcc.1c08739
DO - 10.1021/acs.jpcc.1c08739
M3 - Article
AN - SCOPUS:85124136266
SN - 1932-7447
VL - 126
SP - 1785
EP - 1792
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 4
ER -
