Abstract
N-Ethylcarbazole (NEC), as a promising liquid organic hydrogen carrier (LOHC), can store and release hydrogen through a reversible catalytic hydrogenation and dehydrogenation reaction. In this paper, RuPd bimetallic nanocatalyst supported on MgAl-layered double hydroxide (RuPd/LDH) was prepared by ultrasonic-assisted reduction method, and its catalytic performance in NEC hydrogenation was also studied. Under the action of ultrasound, hydroxyl groups (-OH) on the surface of LDH support dissociated into highly reductive hydrogen radicals for the reduction of Ru3+ and Pd2+ to Ru0 and Pd0. For the 4Ru1Pd/LDH-(300-1) catalyst prepared under ultrasonic conditions of 25 kHz, 300 W, and 1 h, the average size of the metal nanoparticles was only 1.23 nm, which indicated that Ru, Pd, and RuPd NPs were highly dispersed on the support. The strong electronic effects between Ru and Pd improved its catalytic performance in NEC hydrogenation. With m(Ru+Pd)/m(NEC) = 0.2wt%, pressure of 6 MPa, and temperature of 120 °C, the selectivity of dodecahydro-N-ethylcarbazole (12H-NEC) was 98.07%, and the capacity and percentage of hydrogen storage were 5.75wt% and 99.3%, respectively. After the catalyst was recycled 8 times, the percentage of hydrogen storage still reached 98.9%, showing higher stability. The preparation method is simple and environmentally friendly, providing an idea for the preparation of ultrafine bimetallic catalysts with high catalytic activity and stability.
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This work was supported by the National Key R&D Program (2018YFE0108800) and the Science Foundation of Heilongjiang Academy of Sciences (YZ2022SH01&WS2021SH01).
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All authors contributed to the study conception and design. Material preparation, data collection, and analysis were performed by Xiaoran Liu, Jiaming Shi, Xuefeng Bai, and Wei Wu. The first draft of the manuscript was written by Xiaoran Liu, and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
Conceptualization: Wei Wu, Xuefeng Bai and Xiaoran Liu. Methodology: Xiaoran Liu. Formal analysis and investigation: Xiaoran Liu and Jiaming Shi. Writing—original draft preparation: Xiaoran Liu. Writing—review and editing: Wei Wu and Xuefeng Bai. Funding acquisition: Wei Wu and Xuefeng Bai. Resources: Wei Wu and Xuefeng Bai. Supervision: Wei Wu and Xuefeng Bai.
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Liu, X., Shi, J., Bai, X. et al. Ultrasonic-assisted synthesis of highly stable RuPd bimetallic catalysts supported on MgAl-layered double hydroxide for N-ethylcarbazole hydrogenation. Environ Sci Pollut Res 29, 48558–48572 (2022). https://doi.org/10.1007/s11356-022-19203-0
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DOI: https://doi.org/10.1007/s11356-022-19203-0