Selective Oxidation of Methane to Formaldehyde over a Silica-Supported Cobalt Single-Atom Catalyst
Selective Oxidation of Methane to Formaldehyde over a Silica-Supported Cobalt Single-Atom Catalyst
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二氧化硅负载钴单原子催化剂选择性氧化甲烷生成甲醛
DOI：
10.1021/acs.jpcc.1c08739
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发表时间：
2022
期刊：
影响因子：
--
通讯作者：
Takahashi Keisuke
中科院分区：
文献类型：
--
作者：
Ohyama Junya;Abe Daiki;Hirayama Airi;Iwai Hiroki;Tsuchimura Yuka;Sakamoto Kazuki;Irikura Momoka;Nakamura Yuri;Yoshida Hiroshi;Machida Masato;Nishimura Shun;Yamamoto Tomokazu;Matsumura Syo;Takahashi Keisuke
甲烷催化氧化制甲醛和甲醇因其在能源效率上优于传统的甲烷吸热蒸汽重整多步反应工艺而备受关注。然而，CH4直接氧化过程中部分氧化产物的选择性获得是一个挑战。在本研究中，对不同Co负载的Co/ sio2进行了CH4/O2/H2O气体流动反应的测试。结果表明，低负荷≤0.1 wt %的Co/ sio2在部分氧化反应中表现出较高的选择性，主要生成HCHO，而高负荷的Co/ sio2则进行完全氧化。利用x射线吸收精细结构能谱、x射线光电子能谱、x射线衍射和扫描透射电镜分析表明，低Co负载下生成的单个Co原子有效地选择性氧化ch4生成HCHO，而高Co负载下生成的co3o4纳米粒子促进了完全氧化。
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/SiO2with various Co loadings was tested for the CH4/O2/H2O gas flow reaction. As a result, Co/SiO2with a low loading of ≤0.1 wt % showed high selectivity for the partial oxidation reaction and mainly produced HCHO, while Co/SiO2with 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 CH4to HCHO, while Co3O4nanoparticles generated at high Co loadings promoted the complete oxidation.
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影响因子：
16.6
作者：
Tang Y;Li Y;Fung V;Jiang DE;Huang W;Zhang S;Iwasawa Y;Sakata T;Nguyen L;Zhang X;Frenkel AI;Tao FF
通讯作者：
Tao FF
影响因子：
2.5
作者：
Ravel, B;Newville, M
通讯作者：
Newville, M
掺钛 SBA-15 上氧化钒提高甲醛催化氧化的选择性
影响因子：
3.9
作者：
P. Wallis;E. Schönborn;V. N. Kalevaru;Andreas Martin;S. Wohlrab
通讯作者：
S. Wohlrab
丙烯在铜和钴的混合氧化物上的氧化
DOI：
10.1039/f19797501337
发表时间：
1979
期刊：
Journal of the Chemical Society, Faraday Transactions
影响因子：
--
作者：
H. Baussart;R. Delobel;M. Bras;J. Leroy
通讯作者：
J. Leroy