Huifa Zhang1, James H Clark2, Tong Geng1, Huixian Zhang3, Fahai Cao1. 1. Engineering Research Centre of Large Scale Reactor Engineering and Technology of ministry of Education, East China University of Science and Technology, Shanghai, 200237, P. R. China. 2. Green Chemistry Centre of Excellence, University of York, York, YO105DD, UK. 3. SINOPEC North China E&P Company, Zhengzhou, 450006, P. R. China.
Abstract
A newly designed N and P co-doped carbon material has been developed to catalyze the conversion of 5-hydroxymethylfurfural (HMF) to 2,5-furandialdehyde (DFF) with unprecedented yield and selectivity and demonstrating a synergistic effect between the heteroatoms. The desired catalyst was first synthesized via a pyrolysis method using urea as the nitrogen and carbon source followed by calcination with phytic acid solution as the phosphorus source. The mass ratio of phytic acid to C3 N4 and calcination temperature were varied to investigate their effects on catalyst synthesis and microstructure as well as subsequent catalytic activity in simple reaction systems under oxygen. The effect of reaction conditions on the final HMF conversion and DFF selectivity were also investigated systematically. The P-C-N-5-800 catalyst obtained with the optimized annealing temperature of 800 °C and mass ratio of phytic acid/C3 N4 of 5 enabled a 99.5 % DFF yield at 120 °C for 9 h under 10 bar oxygen pressure, being the highest among any reported metal-free heterogeneous catalyst to date. The excellent performance of P-C-N-5-800 could be ascribed to the synergy between N and P heteroatoms as well as the high content of graphitic-N and the P-C species within the carbon structure. Reusability studies show that the P-C-N-5-800 catalyst was stable and reusable without deactivation. These results strongly suggest that P-C-N-5-800 is a promising catalyst for large-scale production of DFF in a green manner.
A newly designed N and Pco-doped class="Chemical">carbon material has been develoclass="Chemical">ped to catalyze the conversion of class="Chemical">pan class="Chemical">5-hydroxymethylfurfural (HMF) to 2,5-furandialdehyde (DFF) with unprecedented yield and selectivity and demonstrating a synergistic effect between the heteroatoms. The desired catalyst was first synthesized via a pyrolysis method using urea as the nitrogen and carbon source followed by calcination with phytic acid solution as the phosphorus source. The mass ratio of phytic acid to C3 N4 and calcination temperature were varied to investigate their effects on catalyst synthesis and microstructure as well as subsequent catalytic activity in simple reaction systems under oxygen. The effect of reaction conditions on the final HMF conversion and DFF selectivity were also investigated systematically. The P-C-N-5-800 catalyst obtained with the optimized annealing temperature of 800 °C and mass ratio of phytic acid/C3 N4 of 5 enabled a 99.5 % DFF yield at 120 °C for 9 h under 10 bar oxygen pressure, being the highest among any reported metal-free heterogeneous catalyst to date. The excellent performance of P-C-N-5-800 could be ascribed to the synergy between N and P heteroatoms as well as the high content of graphitic-N and the P-C species within the carbon structure. Reusability studies show that the P-C-N-5-800 catalyst was stable and reusable without deactivation. These results strongly suggest that P-C-N-5-800 is a promising catalyst for large-scale production of DFF in a green manner.
Authors: Jessica Michalke; Kirill Faust; Thomas Bögl; Stephan Bartling; Nils Rockstroh; Christoph Topf Journal: Int J Mol Sci Date: 2022-08-05 Impact factor: 6.208