Selective chemical looping combustion of acetylene in ethylene-rich streams

• 成果类型: Article
• 署名作者: Jacob, Matthew; Nguyen, Huy; Raj, Rishi; Garcia-Barriocanal, Javier; Hong, Jiyun; Perez-Aguilar, Jorge E.; Hoffman, Adam S.; Mkhoyan, K. Andre; Bare, Simon R.; Neurock, Matthew; Bhan, Aditya
• 署名单位: University of Minnesota System; University of Minnesota Twin Cities; University of Minnesota System; University of Minnesota Twin Cities; Stanford University; United States Department of Energy (DOE); SLAC National Accelerator Laboratory
• 刊物名称: SCIENCE
• ISSN/ISSBN: 0036-11968
• DOI: 10.1126/science.ads3181
• 发表日期: 2025-02-14
• 页码: 744-749
• 关键词: catalytic dehydrogenation dh; initio molecular-dynamics; total-energy calculations; palladium catalysts; bismuth oxide; part 2; hydrogenation; oxygen; shc; ag

摘要

The requirement for C2H2 concentrations below 2 parts per million (ppm) in gas streams for C2H4 polymerization necessitates its semihydrogenation to C2H4. We demonstrate selective chemical looping combustion of C2H2 in C2H4-rich streams by Bi2O3 as an alternative catalytic pathway to reduce C2H2 concentration below 2 ppm. Bi2O3 combusts C2H2 with a first-order rate constant that is 3000 times greater than the rate constant for C2H4 combustion. In successive redox cycles, the lattice O of Bi2O3 can be fully replenished without discernible changes in local Bi coordination or C2H2 combustion selectivity. Heterolytic activation of C-H bonds across Bi-O sites and the higher acidity of C2H2 results in lower barriers for C2H2 activation than C2H4, enabling selective catalytic hydrocarbon combustion leveraging differences in molecular deprotonation energies.