posted on 2020-08-29, 13:39authored byXianzhao Shao, Xinyi Miao, Tianlei Zhang, Wei Wang, Junhong Wang, Xiaohui Ji
Efficient
and reversible hydrogen-storage systems derived from
liquid organic compounds are promising alternatives for sustainable
energy supplies. Here, we report a Pd nanoparticle catalyst supported
on porous carbon co-doped with nitrogen and phosphorous for reversible
formate-based chemical hydrogen storage. The materials showed good
catalytic performance for both formate dehydrogenation and bicarbonate
hydrogenation. The N,P-dual-doped carbon was fabricated by directly
pyrolyzing a mixture of 1,10-phenanthroline and triphenylphosphine.
Initial density functional theory (DFT) studies suggested that N and
P co-dopants played synergistic roles in modulating the electronic
properties of the carbon support. X-ray photoelectron spectroscopy
and CO pulse adsorption experiments revealed that the resulting metal–support
interactions enriched the electron density at the Pd active site.
This promoted the activity of Pd nanoparticles for formate dehydrogenation
with a turnover frequency of 3254 h–1, and a high
formate yield exceeding that of individual N-doped or P-doped catalysts
was also obtained for the hydrogenation of bicarbonate.