Journal
ACS CATALYSIS
Volume 11, Issue 13, Pages 8116-8131Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c01471
Keywords
Cu-based catalyst; oxygen vacancy; hydrogen dissociation; particle size effect; partial hydrogenation of 1,3-BD
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Funding
- Koc University TUPRAS Energy Center (KUTEM)
- Fung Scholarship
- HEC Scholarship
- METU Prof. Dr. Mustafa N. Parlar Education and Research Foundation's 2019 Research Incentive Award
- TARLA
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The study found that the Cu0.5CeMgOx catalyst showed the most stable performance, while the Cu0.3CeMgOx catalyst achieved complete 1,3-BD conversion with complete suppression of total hydrogenation. These findings offer new possibilities for designing noble metal-free, highly selective, and stable copper-based catalysts.
A series of CunCeMgOx catalysts with various copper nanoparticle sizes and surface defect densities were synthesized and tested for partial hydrogenation of 1,3-butadiene (1,3-BD). The data demonstrated a reaction pathway involving the dissociation of molecular hydrogen on the peripheral oxygen vacancies (O-v-Cu+) before reacting with 1,3-BD adsorbed on the corresponding Cu+ atoms. Analysis of the performance data indicated that the turnover frequency of these Cu+ sites is approximately five times higher than those of the surface Cu-0 sites. Among the catalysts considered, Cu0.5CeMgOx with the smallest copper nanoparticle size provided a stable performance for at least 15 h time-on-stream, while the others were easily deactivating because of carbon deposition. Furthermore, unlike the conventional copper-based catalysts, the Cu0.3CeMgOx catalyst achieved a complete suppression of total hydrogenation even at space velocities offering a complete 1,3-BD conversion. The findings offer a broad potential for the rational design of noble metal-free, highly selective, and stable copper-based partial hydrogenation catalysts for reactions that are prone to coke formation.
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