title: Supercritical CO2 mediated incorporation of Pd onto templated carbons: a route to optimizing the Pd particle size and hydrogen uptake density.
abstract: Palladium nanoparticles are deposited onto zeolite template carbon (ZTC) via supercritical CO2 (scCO2) mediated hydrogenation of a CO2-phillic transition metal precursor. The supercritical fluid (SCF) mediated metal incorporation approach enabled the decoration of ZTC with 0.2-2.0 wt % of well-dispersed Pd nanoparticles of size 2-5 nm. The resulting Pd-doped ZTCs exhibit enhanced hydrogen uptake and storage density. The ZTC (with surface area of 2046 m(2)/g) had a hydrogen storage capacity (at 77 K and 20 bar) of 4.9 wt %, while the Pd-ZTCs had uptake of 4.7-5.3 wt % despite a surface area in the range 1390-1858 m(2)/g. The Pd-ZTCs thus exhibit enhanced hydrogen storage density (14.3-18.3 μmol H2/m(2)), which is much higher than that of Pd-free ZTC (12.0 μmol H2/m(2)). The hydrogen isosteric heat of adsorption (Qst) was found to be higher for the Pd-doped carbons (6.7 kJ/mol) compared to the parent ZTC (5.3 kJ/mol). The deposition of small amounts of Pd (up to 2 wt %) along with well-dispersed Pd nanoparticles of size of 2-5 nm is essential for the enhancement of hydrogen uptake and illustrates the importance of optimizing the balance between metal loading/particle size and surface area to achieve the best metal/porous carbon composite for enhanced hydrogen uptake.
authors.affiliation: University of Nottingham, University Park, Nottingham NG7 2RD, UK.
authors.forename: Eric
authors.initials: E
authors.lastname: Masika
authors.forename: Richard A
authors.initials: RA
authors.lastname: Bourne
authors.forename: Thomas W
authors.initials: TW
authors.lastname: Chamberlain
authors.forename: Robert
authors.initials: R
authors.lastname: Mokaya