Search

This study investigated the ammonia decomposition mechanism over Ru/CeO2. Isotopic tests using ND3 revealed that the rate-determining step involves adsorbed nitrogen atoms on Ru. Moreover, an inverse kinetic isotope effect where ND3 decomposition was faster than NH3 was clearly observed. The origin of the inverse effect was explained by the lower D coverage on the catalyst surface compared to H coverage for mitigating the inhibition of ND3 activation. [ABSTRACT FROM AUTHOR]

Microwave‐driven catalytic processes have attracted the attention of many researchers and industries as these processes are powerful strategies for use in industrial electrification. However, undetectable hot spots inside the catalyst bed can be misleading in terms of the deceptive effects of microwaves on acceleration of catalytic reactions because of the lack of physicochemical knowledge about these processes. In this paper, the hot spots temperatures were estimated based on catalytic ammonia (NH3) synthesis/decomposition equilibrium. The reaction temperature estimated from the chemical equilibrium was more than 100 °C higher than the catalyst bed surface temperature measured with an infrared thermometer under microwave irradiation. Assuming a formation of very steep local high temperature fields, rigorous kinetic analysis led to an estimate that the active site fraction which reaches the high temperature was only about 10 % of total sites. Compared with a resistivity heating furnace, the energy input was reduced by more than 85 % under microwave irradiation. The temperature estimated by the chemical equilibrium was almost corresponding to the temperature estimated by an oscillation of extended X‐ray absorption fine structure recorded under microwave irradiation. This paper presents a proposal for a method to estimate hot spots based on thermodynamic equilibrium, yielding a quantitative evaluation of energy consumption reduction caused by microwaves. [ABSTRACT FROM AUTHOR]

This study investigated the ammonia decomposition mechanism over Ru/CeO 2 . Isotopic tests using ND 3 revealed that the rate-determining step involves adsorbed nitrogen atoms on Ru. Moreover, an inverse kinetic isotope effect where ND 3 decomposition was faster than NH 3 was clearly observed. The origin of the inverse effect was explained by the lower D coverage on the catalyst surface compared to H coverage for mitigating the inhibition of ND 3 activation.