Agglomeration Suppression of a Fe-Supported Catalyst and its Utilization for Low-Temperature Ammonia Synthesis in an Electric Field

摘要

Fe-supported heterogeneous catalysts are used for various reactions, including ammonia synthesis, Fischer–Tropsch synthesis, and exhaust gas cleaning. For the practical use of Fe-supported catalysts, suppression of Fe particle agglomeration is the most important issue to be resolved. As described herein, we found that Al doping in an oxide support suppresses agglomeration of the supported Fe particle. Experimental and computational studies revealed two tradeoff Al doping effects: the Fe particle size decreased and remained without agglomeration by virtue of the anchoring effect of doped Al. Also, some Fe atoms anchored by Al cannot function as an active site because of bonding with oxygen atoms. Using an appropriate amount of Al doping is effective for increasing the number of active Fe sites and catalytic activity. This optimized catalyst showed high practical activity and stability for low-temperature ammonia synthesis in an electric field. The optimized catalyst of 12.5 wt % Fe/Ce_(0.4)Al_(0.1)Zr_(0.5)O_(2-δ) showed the highest ammonia synthesis rate (2.3 mmol g~(–1) h~(–1)) achieved to date under mild conditions (464 K, 0.9 MPa) in an electric field among the Fe catalysts reported.