Pd Nanoparticles Supported on N- and P-Co-doped Carbon as Catalysts for Reversible Formate-Based Chemical Hydrogen Storage

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Abstract
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 DFT studies suggested that N and P co-dopants played synergetic 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 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.
Funding Information
  • Education Department of Shaanxi Province (20JS013, 20JS014)
  • National Natural Science Foundation of China (21503125)
  • Shaanxi Provincial Science and Technology Department (2020JM-602)

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