Guan, Xuze;
Han, Rong;
Asakura, Hiroyuki;
Wang, Zhipeng;
Xu, Siyuan;
Wang, Bolun;
Kang, Liqun;
... Wang, Feng Ryan; + view all
(2022)
Designing Reactive Bridging O2– at the Atomic Cu–O–Fe Site for Selective NH3 Oxidation.
ACS Catalysis
, 12
pp. 15207-15217.
10.1021/acscatal.2c04863.
(In press).
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Abstract
Surface oxidation chemistry involves the formation and breaking of metal–oxygen (M–O) bonds. Ideally, the M–O bonding strength determines the rate of oxygen absorption and dissociation. Here, we design reactive bridging O2– species within the atomic Cu–O–Fe site to accelerate such oxidation chemistry. Using in situ X-ray absorption spectroscopy at the O K-edge and density functional theory calculations, it is found that such bridging O2– has a lower antibonding orbital energy and thus weaker Cu–O/Fe–O strength. In selective NH3 oxidation, the weak Cu–O/Fe–O bond enables fast Cu redox for NH3 conversion and direct NO adsorption via Cu–O–NO to promote N–N coupling toward N2. As a result, 99% N2 selectivity at 100% conversion is achieved at 573 K, exceeding most of the reported results. This result suggests the importance to design, determine, and utilize the unique features of bridging O2– in catalysis.
| Type: | Article |
|---|---|
| Title: | Designing Reactive Bridging O2– at the Atomic Cu–O–Fe Site for Selective NH3 Oxidation |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1021/acscatal.2c04863 |
| Publisher version: | https://doi.org/10.1021/acscatal.2c04863 |
| Language: | English |
| Additional information: | This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0). |
| Keywords: | Reactive O2− oxidation chemistry heterogeneous catalysis NH3 emission control, single-atom 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 Chemical Engineering |
| URI: | https://discovery-pp.ucl.ac.uk/id/eprint/10161517 |
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