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.

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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
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article

Selective chemical looping combustion of acetylene in ethylene-rich streams

Matthew Neurock, Javier García‐Barriocanal, Aditya Bhan, Jorge E. Perez-Aguilar et al.
12 citations
Science
Catalysis and Oxidation Reactions
4.67
article

Selective chemical looping combustion of acetylene in ethylene-rich streams

Matthew Neurock, Javier García‐Barriocanal, Aditya Bhan, Jorge E. Perez-Aguilar, Jiyun Hong, Adam S. Hoffman, Simon R. Bare, K. Andre Mkhoyan, Rishi Raj, Matthew Jacob, Huy Dan Nguyen
article en
12 citations

Abstract

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.

ScienceVol. 387(6735)
University of Minnesota (US), SLAC National Accelerator Laboratory (US), Stanford Synchrotron Radiation Lightsource (US)
Openalex Percentile: Top 5%
Catalysis and Oxidation Reactions
4.67
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