期刊
DIAMOND AND RELATED MATERIALS
卷 134, 期 -, 页码 -出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.diamond.2023.109771
关键词
Carbon nanotubes; Nitrogen -doped; Palladium; Single atom; Formic acid
Palladium catalysts supported on nitrogen-containing carbon nanotubes showed high activity in the gas-phase formic acid decomposition for hydrogen production. The way of carbon tube doping by nitrogen greatly influenced the catalyst activity. Single-atom Pd2+ species on bamboo-like nitrogen-containing carbon nanotubes played a key role in the catalyst activity. Treating oxidized multiwalled carbon nanotubes with ammonia increased the activity of Pd nanoparticles by forming surface amine groups.
Palladium catalysts supported on different nitrogen-containing carbon nanotubes(N-CNTs) were successfully used in the continuous gas-phase formic acid decomposition for hydrogen pro-duction. A strong influence of a way of carbon tubes doping by nitrogen on the activity of catalysts comprising metallic nanoparticles of ca. 1 nm in size and single-atom Pd2+ species was found. A key role of the single-atom species, demonstrating excellent stability in various chemically aggressive media, in the catalyst activity was discovered when bamboo-like N-CNTs synthesized by catalytic chemical vapor deposition were used as a sup-port. A substantial increase in the activity of Pd nanoparticles was achieved by the use of N-CNTs prepared by the post-treatment of oxidized multiwalled carbon nanotubes by ammonia resulting in the formation of the domi-nating surface amine groups. The combination of the electron-rich palladium nanoparticles and surface amine groups leads to an increase in the TOF value by a factor of 7 at 70 degrees C. The catalyst operates stable at >99 % selectivity to hydrogen with the mass specific performance 200 l H2/gPd . h.
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