Potter, ME;
McColl, K;
Cora, F;
Levy, AB;
Raja, R;
(2017)
Theoretical insights into the nature of synergistic enhancement in bimetallic CoTiAlPO-5 catalysts for ammonia activation.
Catalysis Science & Technology
, 7
(16)
pp. 3474-3480.
10.1039/c7cy00965h.
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Abstract
Bimetallic catalytic synergy, the concurrent action of two different metal ions in the same material, has resulted in improved efficiency in many catalytic systems and for a range of chemical processes. Via a computational mechanistic study, we investigate the catalytic benefits of the bimetallic CoTiAlPO-5 material in comparison to the monometallic CoAlPO-5 system, on the activation of NH3. The presence of Ti in a framework site adjacent to Co stabilises the Co(II) oxidation state, and increases the Co(III)/Co(II) reduction potential. We show that this change lowers the activation barrier for the homolytic H extraction from NH3 by Co(III), from 162 kJ mol−1 in the monometallic CoAlPO-5 catalyst to 140 kJ mol−1 in the bimetallic CoTiAlPO-5 (175 and 111 kJ mol−1 respectively when considering both dispersion and free energy corrections). Elucidation of mechanistic details through computational studies can make significant contributions to the rational design of catalytic materials.
| Type: | Article |
|---|---|
| Title: | Theoretical insights into the nature of synergistic enhancement in bimetallic CoTiAlPO-5 catalysts for ammonia activation |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1039/c7cy00965h |
| Publisher version: | http://doi.org/10.1039/c7cy00965h |
| Language: | English |
| Additional information: | This journal is © The Royal Society of Chemistry 2017. This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Science & Technology, Physical Sciences, Chemistry, Physical, Chemistry, DOPED NANOPOROUS ALUMINOPHOSPHATES, AEROBIC OXIDATION, ELECTRONIC-PROPERTIES, MOLECULAR-SIEVES, AB-INITIO, HYDROCARBONS, DENSITY, MECHANISM, DESIGN, OXYGEN |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS 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/1573095 |
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