An energy-effective polyaniline coated graphite felt （PANI@GF） composite cathode for the elec- tro-Fenton （E-Fenton） process was synthesized through an electro-polymerization method. The electrocatalytic activity ...An energy-effective polyaniline coated graphite felt （PANI@GF） composite cathode for the elec- tro-Fenton （E-Fenton） process was synthesized through an electro-polymerization method. The electrocatalytic activity of the cathode for the 2e- ORR process was investigated and dimethyl phthalate （DMP） was used as a model substrate to evaluate its performance in the E-Fenton process. The as-prepared PANI@GF composite possessed a three-dimensional porous structure, which is favorable for 02 diffusion, while the large amount of N atoms in the conductive polyaniline （PANI） enhanced 2e- ORR reactivity. The DMP degradation of the E-Fenton system using PANI@GF was significantly enhanced owing to the improvement in ORR performance. The apparent kinetic con- stant for DMP degradation was 0.0753 min-1, five times larger than that of GF. The optimal carboni- zation temperature and polymerization time for the preparation of the PANI@GF composite cath- ode was found to be 900 ℃ and 1 h, respectively. Measurement conditions are a crucial factor for proper evaluation of cathode electrocatalytic performance. Accordingly, the 02 flow rate, Fe^2＋ con- centration, and pH for DMP degradation were optimized at 0.4 L/min, 1.0 mmol/L, and 3.0, respec- tively. These results indicate that the present PANI@GF composite cathode is energy-effective and promising for potential use as an E-Fenton system cathode for the removal of organic pollutants in wastewater.展开更多
Herein,the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework(Fe_(3)N@NG/NC)is investigated as a heterogeneous electro-Fenton(HE-EF)catalyst for the efficie...Herein,the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework(Fe_(3)N@NG/NC)is investigated as a heterogeneous electro-Fenton(HE-EF)catalyst for the efficient removal of organics.The simultaneous carbonization and ammonia etching of iron-based metal organic framework(Fe-MOF)materials yielded well-dispersed N-doped carbon-coated Fe_(3)N nanoparticles with a diameter of~70 nm.The Fe_(3)N and pyridinic N endowed the composite with high HE-EF activity for decomposing the electrogenerated H_(2)O_(2) to•OH.The Fe_(3)N@NG/NC exhibited outstanding HE-EF performance in removing various organic pollutants with low iron leaching.A removal rate of 97-100%could be obtained for rhodamine B(RhB),dimethyl phthalate,methylene blue,and orange Ⅱ in 120 min at a pH of 5.0.When the solution pH was set to 3.0,5.0,7.0,and 9.0,the removal rate of RhB reached 100%,96%,92%,and 81%,respectively,in 60 min at an optimum voltage of 0.0 V(vs.reversible hydrogen electrode(RHE)).Moreover,the concentration of leached iron was expected to be below 0.03 mg/L in a wide pH range of 3.0-9.0.In addition,the RhB removal efficiency remained as high as 90%after six cycles in the reusability experiments.This work highlights the MOF-derived Fe_(3)N composite as an efficient HE-EF catalyst and the corresponding catalytic mechanism,which facilitates its application in wastewater treatment.展开更多
基金supported by the Sino-Greek Science and Technology Cooperation Project (2013DFG62590)the National Natural Science Foundation of China (21575299, 21576300, 21276290)+1 种基金Guangdong Province Nature Science Foundation (2014A030313150)Guangzhou Science and Technology Plan Project (201607010104)~~
文摘An energy-effective polyaniline coated graphite felt （PANI@GF） composite cathode for the elec- tro-Fenton （E-Fenton） process was synthesized through an electro-polymerization method. The electrocatalytic activity of the cathode for the 2e- ORR process was investigated and dimethyl phthalate （DMP） was used as a model substrate to evaluate its performance in the E-Fenton process. The as-prepared PANI@GF composite possessed a three-dimensional porous structure, which is favorable for 02 diffusion, while the large amount of N atoms in the conductive polyaniline （PANI） enhanced 2e- ORR reactivity. The DMP degradation of the E-Fenton system using PANI@GF was significantly enhanced owing to the improvement in ORR performance. The apparent kinetic con- stant for DMP degradation was 0.0753 min-1, five times larger than that of GF. The optimal carboni- zation temperature and polymerization time for the preparation of the PANI@GF composite cath- ode was found to be 900 ℃ and 1 h, respectively. Measurement conditions are a crucial factor for proper evaluation of cathode electrocatalytic performance. Accordingly, the 02 flow rate, Fe^2＋ con- centration, and pH for DMP degradation were optimized at 0.4 L/min, 1.0 mmol/L, and 3.0, respec- tively. These results indicate that the present PANI@GF composite cathode is energy-effective and promising for potential use as an E-Fenton system cathode for the removal of organic pollutants in wastewater.
文摘Herein,the application of a N-doped graphitic-carbon-coated iron nitride composite dispersed in a N-doped carbon framework(Fe_(3)N@NG/NC)is investigated as a heterogeneous electro-Fenton(HE-EF)catalyst for the efficient removal of organics.The simultaneous carbonization and ammonia etching of iron-based metal organic framework(Fe-MOF)materials yielded well-dispersed N-doped carbon-coated Fe_(3)N nanoparticles with a diameter of~70 nm.The Fe_(3)N and pyridinic N endowed the composite with high HE-EF activity for decomposing the electrogenerated H_(2)O_(2) to•OH.The Fe_(3)N@NG/NC exhibited outstanding HE-EF performance in removing various organic pollutants with low iron leaching.A removal rate of 97-100%could be obtained for rhodamine B(RhB),dimethyl phthalate,methylene blue,and orange Ⅱ in 120 min at a pH of 5.0.When the solution pH was set to 3.0,5.0,7.0,and 9.0,the removal rate of RhB reached 100%,96%,92%,and 81%,respectively,in 60 min at an optimum voltage of 0.0 V(vs.reversible hydrogen electrode(RHE)).Moreover,the concentration of leached iron was expected to be below 0.03 mg/L in a wide pH range of 3.0-9.0.In addition,the RhB removal efficiency remained as high as 90%after six cycles in the reusability experiments.This work highlights the MOF-derived Fe_(3)N composite as an efficient HE-EF catalyst and the corresponding catalytic mechanism,which facilitates its application in wastewater treatment.
