Ultrasound-assisted preparation of PdCo bimetallic nanoparticles loaded on beta zeolite for efficient catalytic hydrogen production from dodecahydro-N-ethylcarbazole.

ABSTRACT

Research and development of high-performance catalysts is a key technology to realize hydrogen energy storage and transportation based on liquid organic hydrogen carriers. Co/beta was prepared using beta zeolite as a carrier via an electrostatic adsorption (ESA)-chemical reduction method, and it was used as the template and reducing agent to prepare bimetallic catalysts via an ultrasonic assisted galvanic replacement process (UGR). The fabricated PdCo/beta were characterized by TEM, XPS, FT-IR, XRD, H2-TPR, and H2-TPD. It was shown that the ultrafine PdCo nanoparticles (NPs) are evenly distributed on the surface of the beta zeolite. There is electron transfer between metal NPs and strong-metal-support-interaction (SMSI), which results in highly efficient catalytic dodecahydro-N-ethylcarbazole (12H-NEC) dehydrogenation performance of PdCo bimetallic catalysts. The dehydrogenation efficiency reached 100 % in 4 h at 180 °C and 95.3 % in 6 h at 160 °C. The TOF of 146.22 min-1 is 7 times that of Pd/beta. The apparent activation energy of the reaction is 66.6 kJ/mol, which is much lower than that of Pd/beta. Under the action of ultrasonic waves, the galvanic replacement reaction is accelerated, and the intermetal and metal-carrier interactions are enhanced, which improves the catalytic reaction performance.