Abstract
Bamboo-like nitrogen-doped carbon nanotubes (N-CNTs) were used to synthesize supported palladium catalysts (0.2–2 wt.%) for hydrogen production via gas phase formic acid decomposition. The beneficial role of nitrogen centers of N-CNTs in the formation of active isolated palladium ions and dispersed palladium nanoparticles was demonstrated. It was shown that although the surface layers of N-CNTs are enriched with graphitic nitrogen, palladium first interacts with accessible pyridinic centers of N-CNTs to form stable isolated palladium ions. The activity of Pd/N-CNTs catalysts is determined by the ionic capacity of N-CNTs and dispersion of metallic nanoparticles stabilized on the nitrogen centers. The maximum activity was observed for the 0.2% Pd/N-CNTs catalyst consisting of isolated palladium ions. A ten-fold increase in the concentration of supported palladium increased the contribution of metallic nanoparticles with a mean size of 1.3 nm and decreased the reaction rate by only a factor of 1.4.
Highlights
Rational use of fossil fuel resources is a necessary condition for the long-term stable development of society
Pd/nitrogen-doped carbon nanotubes (N-CNTs) catalyst consisting of isolated palladium ions
We have demonstrated the low intrinsic activity of washed N-CNTs and CNTs in formic acid (FA) decomposition reactions compared to metal supported catalysts [16]
Summary
Rational use of fossil fuel resources is a necessary condition for the long-term stable development of society. In this context, the development of efficient processes for energy production from renewable sources is a topical problem that can be solved using various fundamental studies, in the field of material science. The FA decomposition reaction proceeds on mono-, bi- and trimetallic catalysts deposited on oxide or carbon supports [3,4]. Activity and selectivity of the catalysts towards hydrogen production are determined by the nature of their active component, its dispersion, and electronic state of metals. The application of nitrogen-doped carbon nanomaterials (N-CNMs) as the catalyst supports makes it possible to perform the tailored synthesis of metal supported catalysts with desired properties [5]
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