Journal
ACS CATALYSIS
Volume 12, Issue 1, Pages 587-599Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c05078
Keywords
ammonia synthesis; carbon embedded bimetallic nanoparticles; iron and cobalt phthalocyanines; Co-Fe catalyst; alkali promoter; N-2 activation
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Funding
- King Abdullah University of Science and Technology
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Introducing cobalt into iron catalysts significantly enhances the efficiency of ammonia synthesis, especially exhibiting excellent activity at low temperatures. The study reveals a tuning effect on the surface of the catalyst by introducing cobalt, weakening NHx retarding species and making the iron sites more favorable for N-2 activation.
Ammonia is one of the most commonly produced chemicals in the industry. As a result, similar to 1-2% of the world's electrical energy is used, and it produces similar to 1.5-2% of global CO2 emissions. Therefore, developing efficient catalysts at milder conditions is highly desirable. Here, efficient iron/cobalt catalysts for ammonia synthesis are prepared with different Fe/Co ratios from phthalocyanine precursors, resulting in Fe-Co bimetallic nanoparticles embedded in a porous carbon-nitrogen matrix. The incorporation of Co to the Fe catalyst up to 20% wt of Co leads to similar to 40% enhancement in the activity compared to the monometallic Fe-based catalyst. Interestingly, catalysts exhibit excellent activity even at low temperatures (350 degrees C). Ea for the most efficient 6K-FePc80CoPc20 catalyst is found to be 29 kJ.mol(-1), suggesting facile activation of N-2 at low temperatures. An in-depth kinetic study revealed that introducing Co in the Fe catalysts drastically tuned the surface of the catalyst by weakening the various NHx retarding species. Density functional theory calculations confirm the thermodynamic feasibility for introducing 25% of Co at surface Fe sites. This indicates that the presence of Co on the surface draws negative charges from neighboring Fe sites, making the exposed Fe sites neutral and more favorable for N-2 activation on the bimetallic K2O/Co-Fe catalyst and displaying a more thermodynamically feasible energy profile as compared to the pristine K2O/Fe catalyst.
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