Catalytic direct oxidation of methane to methanol by redox of copper mordenite

Catalytic direct oxidation of methane to methanol by redox of copper mordenite
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铜丝光沸石氧化还原催化甲烷直接氧化制甲醇

DOI:
10.1039/d1cy00125f
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发表时间:
2021
影响因子:
5
通讯作者:
Takahashi Keisuke
Takahashi Keisuke
中科院分区:
化学2区
文献类型:
--
作者:
Ohyama Junya;Hirayama Airi;Tsuchimura Yuka;Kondou Nahoko;Yoshida Hiroshi;Machida Masato;Nishimura Shun;Kato Kazuo;Miyazato Itsuki;Takahashi Keisuke

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随着对高能效化学工艺的需求不断增加,对工业上实现甲烷直接转化为甲醇的期望也在不断增长。在这项研究中,催化生产CH 3OH通过直接氧化CH 4与O2进行使用Cu沸石催化剂在CH 4/O2/H2O流动反应。在所研究的各种Cu沸石中,Cu-MOR催化剂表现出相对高的CH 3OH产量,在24 h内的转化数为7.4 molCH 3OH molCu−1(CH 4转化率:0.011%)。用原位X射线吸收光谱和红外光谱研究了催化剂上Cu的活性物种和催化循环。结果表明,Cu(I)/Cu(II)物种的氧化还原是Cu-MOR催化循环的关键.此外,H2O吸附,包括动态Cu物种被发现是催化活性。
Expectations for industrial implementation of direct conversion of CH4 to CH3OH are growing with the increasing demand for energy-efficient chemical processes. In this study, catalytic production of CH3OH by direct oxidation of CH4 with O2 was performed using Cu zeolite catalysts in a CH4/O2/H2O flow reaction. Among the various Cu zeolites investigated, the Cu-MOR catalyst exhibited relatively high CH3OH production with a turnover number of 7.4 molCH3OH molCu−1 over 24 h (CH4 conversion: 0.011%). The catalytically active Cu species and catalytic cycle were investigated by in situ simultaneous X-ray absorption and infrared spectroscopy. The results suggest that the key to the catalytic cycle over Cu-MOR is the redox of Cu(I)/Cu(II) species. Furthermore, H2O-adsorption-included dynamic Cu species are revealed to be catalytically active.
甲烷的酶促氧化。
DOI: 10.1021/acs.biochem.5b00198
发表时间: 2015-04-14
期刊: Biochemistry
影响因子: 2.9
作者:
Sirajuddin S;Rosenzweig AC
通讯作者: Rosenzweig AC