Thermal treatment of fluorinated porous carbon in ammonia flow to produce a nitrogen-doped support for highly dispersed nickel effectively catalyzing formic acid dehydrogenation

Nitrogen-doped carbon attracts researchers as a catalyst support due to its ability to provide high dispersion of deposited metal, which can show improved properties in various catalytic reactions as compared to the metal on nitrogen-free carbon supports. Here, we developed a procedure for modification of a porous carbon material by fluorination with bromine trifluoride vapor at room temperature followed by heating in gaseous ammonia to produce a nitrogen-doped carbon support for nickel catalyst. The obtained support has a specific surface area of 1030 m(2)/g and a total nitrogen content of 4.8 at.%, with half of it in the form of pyridinic nitrogen, which is necessary for stabilization of nickel atoms. These characteristics of the support allow a simple impregnation method to achieve a content of nickel single-atom sites up to 4.9 wt.%. Increasing the metal content to 7.4 wt.% leads to the formation of nickel particles with an average size of less than 1 nm. The catalysts were tested in the decomposition reaction of gaseous formic acid and showed high (>99 %) and stable selectivity toward hydrogen production.