Xie, J;
Jin, R;
Li, A;
Bi, Y;
Ruan, Q;
Deng, Y;
Zhang, Y;
... Tang, J; + view all
(2018)
Highly selective oxidation of methane to methanol at ambient conditions by titanium dioxide-supported iron species.
Nature Catalysis
, 1
(11)
pp. 889-896.
10.1038/s41929-018-0170-x.
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Abstract
Methane activation under moderate conditions and with good selectivity for value-added chemicals still remains a huge challenge. Here, we present a highly selective catalyst for the transformation of methane to methanol composed of highly dispersed iron species on titanium dioxide. The catalyst operates under moderate light irradiation (close to one Sun) and at ambient conditions. The optimized sample shows a 15% conversion rate for methane with an alcohol selectivity of over 97% (methanol selectivity over 90%) and a yield of 18 moles of alcohol per mole of iron active site in just 3 hours. X-ray photoelectron spectroscopy measurements with and without xenon lamp irradiation, light-intensity-modulated spectroscopies, photoelectrochemical measurements, X-ray absorption near-edge structure and extended X-ray absorption fine structure spectra, as well as isotopic analysis confirm the function of the major iron-containing species—namely, FeOOH and Fe2O3, which enhance charge transfer and separation, decrease the overpotential of the reduction reaction and improve selectivity towards methanol over carbon dioxide production.
| Type: | Article |
|---|---|
| Title: | Highly selective oxidation of methane to methanol at ambient conditions by titanium dioxide-supported iron species |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1038/s41929-018-0170-x |
| Publisher version: | https://doi.org/10.1038/s41929-018-0170-x |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Heterogeneous catalysis, Natural gas, Photocatalysis |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Engineering Science > Dept of Chemical Engineering UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10066222 |
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