Nitrogen-doped carbon(N-C)materials have demonstrated exceptional performances in activating peroxymonosulfate(PMS)for environmental remediation.However,accommodating higher nitrogen contents remains challenging in N-...Nitrogen-doped carbon(N-C)materials have demonstrated exceptional performances in activating peroxymonosulfate(PMS)for environmental remediation.However,accommodating higher nitrogen contents remains challenging in N-C due to the thermodynamic instability of C-N skeleton.In this study,we proposed an innovative epitaxial growth approach to synthesize two-dimensional N-C nanosheets.Leveraging the abundant amino groups supplied by the polymer dots as growing sites,we successfully attained a high nitrogen level and spontaneously introduced abundant structural defects in the carbon framework.The resulting N-C nanosheets exhibited outstanding catalytic activity for the activation of PMS toward selective oxidation of diethyl 1,4-dihydro-2,6-dimethyl-3,5-pyridinedicarboxylate(1,4-DHP)into diethyl2,6-dimethylpyridine-3,5-dicarboxylate,which serves as a valuable intermediate in the synthesis of various pharmaceutical compounds.Comprehensive experimental and characterization investigations verified that the nitrogen sites and defects are the primary active sites for PMS activation and selective oxidation of 1,4-DHP.This work offered an efficient approach for the fabrication of high-nitrogen-loading carbon materials for catalytic oxidation reactions.展开更多
基金the financial support from Australian Research Council under DECRA Scheme(No.DE210100253)merit SXR beamline from Australian Nuclear Science and Technology Organization(ANSTO,No.AS231/SXR/19680)。
文摘Nitrogen-doped carbon(N-C)materials have demonstrated exceptional performances in activating peroxymonosulfate(PMS)for environmental remediation.However,accommodating higher nitrogen contents remains challenging in N-C due to the thermodynamic instability of C-N skeleton.In this study,we proposed an innovative epitaxial growth approach to synthesize two-dimensional N-C nanosheets.Leveraging the abundant amino groups supplied by the polymer dots as growing sites,we successfully attained a high nitrogen level and spontaneously introduced abundant structural defects in the carbon framework.The resulting N-C nanosheets exhibited outstanding catalytic activity for the activation of PMS toward selective oxidation of diethyl 1,4-dihydro-2,6-dimethyl-3,5-pyridinedicarboxylate(1,4-DHP)into diethyl2,6-dimethylpyridine-3,5-dicarboxylate,which serves as a valuable intermediate in the synthesis of various pharmaceutical compounds.Comprehensive experimental and characterization investigations verified that the nitrogen sites and defects are the primary active sites for PMS activation and selective oxidation of 1,4-DHP.This work offered an efficient approach for the fabrication of high-nitrogen-loading carbon materials for catalytic oxidation reactions.
