Zhang, Jiajun;
Feng, Kai;
Li, Zhengwen;
Yang, Bin;
Yan, Binhang;
Luo, Kai Hong;
(2023)
Defect-Driven Efficient Selective CO2 Hydrogenation with Mo-Based Clusters.
JACS Au
10.1021/jacsau.3c00206.
(In press).
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Abstract
Synthetic fuels produced from CO2 show promise in combating climate change. The reverse water gas shift (RWGS) reaction is the key to opening the CO2 molecule, and CO serves as a versatile intermediate for creating various hydrocarbons. Mo-based catalysts are of great interest for RWGS reactions featured for their stability and strong metal–oxygen interactions. Our study identified Mo defects as the intrinsic origin of the high activity of cluster Mo2C for CO2-selective hydrogenation. Specifically, we found that defected Mo2C clusters supported on nitrogen-doped graphene exhibited exceptional catalytic performance, attaining a reaction rate of 6.3 gCO/gcat/h at 400 °C with over 99% CO selectivity and good stability. Such a catalyst outperformed other Mo-based catalysts and noble metal-based catalysts in terms of facile dissociation of CO2, highly selective hydrogenation, and nonbarrier liberation of CO. Our study revealed that as a potential descriptor, the atomic magnetism linearly correlates to the liberation capacity of CO, and Mo defects facilitated product desorption by reducing the magnetization of the adsorption site. On the other hand, the defects were effective in neutralizing the negative charges of surface hydrogen, which is crucial for selective hydrogenation. Finally, we have successfully demonstrated that the combination of a carbon support and the carbonization process synergistically serves as a feasible strategy for creating rich Mo defects, and biochar can be a low-cost alternative option for large-scale applications.
| Type: | Article |
|---|---|
| Title: | Defect-Driven Efficient Selective CO2 Hydrogenation with Mo-Based Clusters |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/jacsau.3c00206 |
| Publisher version: | https://doi.org/10.1021/jacsau.3c00206 |
| Language: | English |
| Additional information: | This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. |
| Keywords: | Mo2C nanoparticle, synthesized fuels, RWGS reaction, atomic magnetism, selective hydrogenation |
| 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 Mechanical Engineering |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10177377 |
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