Significantly improved dehydrogenation of dodecyl-N-ethylcarbazole over supported PdFe bimetallic nanocatalysts via polydopamine surface modification of Al2O3

Abstract

N-ethylcarbazole (NEC) has great application prospects in hydrogen storage due to its ability to dehydrogenate at lower energy and high hydrogen storage performance. Developing supported metal catalysts with high catalytic activity and stability is key to achieving large-scale application of LOHC hydrogen storage technology. In this paper, bimetallic FePd/Al2O3@PDA-GR catalysts used for the dehydrogenation process of 12H-NEC were prepared by stepwise reduction methods, including chemical reduction and galvanic replacement, using PDA-coated Al2O3 as the support. The characterization results showed that adding PDA could anchor the metal particles, improve the dispersion of metal particles on the support surface, and reduce the agglomeration phenomenon. The nanoparticles of bimetallic catalysts prepared by the galvanic replacement were small, with the particle size distribution of 0.86 nm-2.78 nm, and an average size of 1.52 nm. The large number of exposed active sites enabled the catalysts to reduce the dosage of Pd while still possessing excellent catalytic performance. And part of Pd was coated on Fe NPs in the Fe5Pd1/Al2O3@PDA-GR catalysts prepared by galvanic replacement, which improved the atom utilization of Pd. And there is an obvious electronic interaction between Fe and Pd. In the dehydrogenation process of 12H-NEC to NEC, The prepared FePd/Al2O3@PDA-GR catalyst exhibited excellent catalytic performance and had a significantly greater dehydrogenation efficiency than found in the literature, 95% for 1 h and 100% for 3 h at 180 °C. The temperature drop to 160 °C did not affect the dehydrogenation efficiency, which remained at 98.1% for 3 h. The prepared catalyst had good stability, and the dehydrogenation efficiency was 93.1% after five successive cycles.