Ru-based catalysts exhibit excellent activity for the hydrogenation of N-ethylcarbazole(NEC)that is widely used as liquid organic hydrogen carriers(LOHCs).Previous studies showed that the Ru particle size strongly aff...Ru-based catalysts exhibit excellent activity for the hydrogenation of N-ethylcarbazole(NEC)that is widely used as liquid organic hydrogen carriers(LOHCs).Previous studies showed that the Ru particle size strongly affects the catalytic performance of hydrogenation.However,the size effect on the NEC hydrogenation activity remains unclear.In this work,a series of Ru/Al_(2)O_(3) catalysts with precisely controlled Ru particle sizes were engineered.The correlation between the Ru particle size and resulting catalytic performance,including the distribution of reaction intermediates,was systematically investigated.The turnover frequency(TOF)for NEC hydrogenation exhibited a pronounced volcanic trend with the increase of the Ru particle size from 1.73 to 5.76 nm,reaching a maximum value of 117.75 min^(−1) when the Ru particle size was 3.20 nm.These results indicated that the high-efficient catalyst required a balance between high-coordination terrace sites and low-coordination line-edge sites.The kinetics experiments demonstrated that the NEC followed first-order kinetics with an activation energy of 35.74 kJ/mol.This study offers theoretical guidance for designing high-performance hydrogenation catalysts tailored for NEC.展开更多
基金supported by the National Natural Science Foundation of China(Grants 22525801 and 22378011)National Key Research and Development Program of China(Grant 2022YFA1504401).
文摘Ru-based catalysts exhibit excellent activity for the hydrogenation of N-ethylcarbazole(NEC)that is widely used as liquid organic hydrogen carriers(LOHCs).Previous studies showed that the Ru particle size strongly affects the catalytic performance of hydrogenation.However,the size effect on the NEC hydrogenation activity remains unclear.In this work,a series of Ru/Al_(2)O_(3) catalysts with precisely controlled Ru particle sizes were engineered.The correlation between the Ru particle size and resulting catalytic performance,including the distribution of reaction intermediates,was systematically investigated.The turnover frequency(TOF)for NEC hydrogenation exhibited a pronounced volcanic trend with the increase of the Ru particle size from 1.73 to 5.76 nm,reaching a maximum value of 117.75 min^(−1) when the Ru particle size was 3.20 nm.These results indicated that the high-efficient catalyst required a balance between high-coordination terrace sites and low-coordination line-edge sites.The kinetics experiments demonstrated that the NEC followed first-order kinetics with an activation energy of 35.74 kJ/mol.This study offers theoretical guidance for designing high-performance hydrogenation catalysts tailored for NEC.
