Title | Highly efficient K-Fe/C catalysts derived from metal-organic frameworks towards ammonia synthesis |
Authors | Yan, Pengqi Guo, Wenhan Liang, Zibin Meng, Wei Yin, Zhen Li, Siwei Li, Mengzhu Zhang, Mengtao Yan, Jie Xiao, Dequan Zou, Ruqiang Ma, Ding |
Affiliation | Peking Univ, Beijing Natl Lab Mol Sci, Coll Chem & Mol Engn, Beijing 100871, Peoples R China Peking Univ, Coll Engn, Beijing 100871, Peoples R China Peking Univ, BIC ESAT, Beijing 100871, Peoples R China Peking Univ, Beijing Key Lab Theory & Technol Adv Battery Mat, Dept Mat Sci & Engn, Coll Engn, Beijing 10087, Peoples R China Tianjin Polytech Univ, State Key Lab Separat Membranes & Membrane Proc, Sch Chem & Chem Engn, Tianjin 300387, Peoples R China Univ New Haven, Dept Chem & Chem Engn, West Haven, CT 06516 USA |
Keywords | metal-organic frameworks pyrolysis ammonia synthesis iron nanoparticles K promotion |
Issue Date | 2019 |
Publisher | NANO RESEARCH |
Abstract | Fe-based catalysts have been discovered as the best elementary metal-based heterogeneous catalysts for the ammonia synthesis in industrial application during the last century. Herein, a novel and scalable strategy is developed to prepare the K-promoted Fe/C catalyst with extremely high Fe loading (> 50 wt.%) through pyrolysis of the Fe-based metal-organic framework (MOF) xerogel. The obtained K-Fe/C catalysts exhibited superior activity and stability towards ammonia synthesis. The weight-specific reaction rate of Fe/C with K2O as promoter can achieve 12.4 mmol center dot g(-1)center dot h(-1) at 350 degrees C and 30.4 mmol center dot g(-1)center dot h(-1) at 400 degrees C, approximately four and two times higher than that of the commercial fused-iron catalyst (3.4 mmol center dot g(-1)center dot h(-1) at 350 degrees C and 16.7 mmol center dot g(-1)center dot h(-1) at 400 degrees C) under the same condition, respectively. The excellent performance of K-Fe/C can be ascribed to the inherited structure derived from the metal-organic frame precursors and the promotion of potassium, which can modify the binding energy of reactant molecules on the Fe surface, transfer electrons to iron for effective activation of nitrogen, prevent agglomeration of Fe nanoparticle (NPs) and restrain side reaction of carbon matrix to methane. |
URI | http://hdl.handle.net/20.500.11897/545425 |
ISSN | 1998-0124 |
DOI | 10.1007/s12274-019-2349-0 |
Indexed | SCI(E) EI |
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