Li, Zhengwen;
Zhang, Jiajun;
Tian, Jiaming;
Feng, Kai;
Chen, Yuxin;
Li, Xiao;
Zhang, Zhihe;
... Yan, Binhang; + view all
(2024)
Decoupling Active Sites Enables Low-Temperature Semihydrogenation of Acetylene.
ACS Catalysis
, 14
(3)
pp. 1514-1524.
10.1021/acscatal.3c05508.
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Abstract
Achieving high ethylene selectivity while preserving high reactivity for semihydrogenation of acetylene over Pd-based catalysts is still challenging. Here, we propose a structure of encapsulated Pd nanoparticles to enhance catalytic performance via a low-dose doping-segregation strategy using Pd-doped SrTiO3 as a precursor. The encapsulated Pd nanoclusters are revealed to be protected by a thin TiOx shell to prevent contact with acetylene/ethylene. However, hydrogen can still be efficiently activated on the encapsulated Pd sites and react with the adsorbed acetylene on surface Ti3+ sites via hydrogen spillover. By taking advantage of weaker ethylene adsorption on partially reduced oxide TiOx, this catalyst shows an enhanced performance of 98% conversion and 92% selectivity with a specific activity of 5552 molC2H2·molPd–1·h–1 at 100 °C, significantly surpassing most Pd-based catalysts. This strategy decouples active sites for the activation of different reactants, providing a thought for the development of highly active and selective hydrogenation catalysts.
| Type: | Article |
|---|---|
| Title: | Decoupling Active Sites Enables Low-Temperature Semihydrogenation of Acetylene |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acscatal.3c05508 |
| Publisher version: | http://dx.doi.org/10.1021/acscatal.3c05508 |
| 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: | Semihydrogenation of acetylene; doping-segregation; decoupled active sites; hydrogen spillover; Pd-based catalyst |
| 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.ucl.ac.uk/id/eprint/10187159 |
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