Selective chemical looping combustion of acetylene in ethylene-rich streams
The requirement for C<sub>2</sub>H<sub>2</sub> concentrations below 2 parts per million (ppm) in gas streams for C<sub>2</sub>H<sub>4</sub> polymerization necessitates its semihydrogenation to C<sub>2</sub>H<sub>4</sub>. We demonstrate selective chemical looping combustion of C<sub>2</sub>H<sub>2</sub> in C<sub>2</sub>H<sub>4</sub>-rich streams by Bi<sub>2</sub>O<sub>3</sub> as an alternative catalytic pathway to reduce C<sub>2</sub>H<sub>2</sub> concentration below 2 ppm. Bi<sub>2</sub>O<sub>3</sub> combusts C<sub>2</sub>H<sub>2</sub> with a first-order rate constant that is 3000 times greater than the rate constant for C<sub>2</sub>H<sub>4</sub> combustion. In successive redox cycles, the lattice O of Bi<sub>2</sub>O<sub>3</sub> can be fully replenished without discernible changes in local Bi coordination or C<sub>2</sub>H<sub>2</sub> combustion selectivity. Heterolytic activation of C-H bonds across Bi-O sites and the higher acidity of C<sub>2</sub>H<sub>2</sub> results in lower barriers for C<sub>2</sub>H<sub>2</sub> activation than C<sub>2</sub>H<sub>4</sub>, enabling selective catalytic hydrocarbon combustion leveraging differences in molecular deprotonation energies.
Authors
- Matthew Neurock (ORCID: https://orcid.org/0000-0003-1458-7837)
- Javier García‐Barriocanal
- Aditya Bhan (ORCID: https://orcid.org/0000-0002-6069-7626)
- Jorge E. Perez-Aguilar (ORCID: https://orcid.org/0000-0001-8650-3132)
- Jiyun Hong (ORCID: https://orcid.org/0000-0002-3631-0559)
- Adam S. Hoffman (ORCID: https://orcid.org/0000-0002-7682-4108)
- Simon R. Bare (ORCID: https://orcid.org/0000-0002-4932-0342)
- K. Andre Mkhoyan (ORCID: https://orcid.org/0000-0003-3568-5452)
- Rishi Raj
- Matthew Jacob
- Huy Dan Nguyen (ORCID: https://orcid.org/0009-0008-4597-7567)
Institutions
- University of Minnesota (US)
- SLAC National Accelerator Laboratory (US)
- Stanford Synchrotron Radiation Lightsource (US)
Publication Details
- Journal
- Science
- Published
- 2025-02-13
- DOI
- https://doi.org/10.1126/science.ads3181
- Citations
- 12
- Primary Topic
- Catalysis and Oxidation Reactions
- Type
- article
- Field-Weighted Citation Impact
- 4.67