Chen, Jingkun;
Su, Yuetan;
Meng, Qingjie;
Qian, Hehe;
Shi, Le;
Darr, Jawwad A;
Wu, Zhongbiao;
(2023)
Palladium Encapsulated by an Oxygen-Saturated TiO2 Overlayer for Low-Temperature SO2-Tolerant Catalysis during CO Oxidation.
Angewandte Chemie International Edition
, Article e202310191. 10.1002/anie.202310191.
(In press).
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Abstract
The development of oxidation catalysts that are resistant to sulfur poisoning is crucial for extending the lifespan of catalysts in real-working conditions. Herein, we describe the design and synthesis of oxide-metal interaction (OMI) catalyst under oxidative atmospheres. By using organic coated TiO2, an oxide/metal inverse catalyst with non-classical oxygen-saturated TiO2 overlayers were obtained at relatively low temperature. These catalysts were found to incorporate ultra-small Pd metal and support particles with exceptional reactivity and stability for CO oxidation (under 21 vol% O2 and 10 vol% H2O). In particular, the core (Pd)–shell (TiO2) structured OMI catalyst exhibited excellent resistance to SO2 poisoning, yielding robust CO oxidation performance at 120 °C for 240 h (at 100 ppm SO2 and 10 vol% H2O). The stability of this new OMI catalyst was explained through density functional theory (DFT) calculations that interfacial oxygen atoms at Pd–O–Ti sites (of oxygen-saturated overlayers) serve as non-metal active sites for low-temperature CO oxidation, and change the SO2 adsorption from metal(d)-to-SO2(π*) back-bonding to much weaker σ(Ti–S) bonding.
| Type: | Article |
|---|---|
| Title: | Palladium Encapsulated by an Oxygen-Saturated TiO2 Overlayer for Low-Temperature SO2-Tolerant Catalysis during CO Oxidation |
| Location: | Germany |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1002/anie.202310191 |
| Publisher version: | https://doi.org/10.1002/anie.202310191 |
| 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: | Metal-support interaction; sulfur tolerance; CO oxidation; Stability, non-metal active site |
| 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-pp.ucl.ac.uk/id/eprint/10179690 |
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