Ordered mesoporous carbon supported iron catalysts （Fe/OMC） were prepared by the incipient wetness impregnation method and investigated in Fenton-like degradation of 4-chlorophenol （4CP） in this work. XRD and TEM ...Ordered mesoporous carbon supported iron catalysts （Fe/OMC） were prepared by the incipient wetness impregnation method and investigated in Fenton-like degradation of 4-chlorophenol （4CP） in this work. XRD and TEM characterization showed that the iron oxides were well dispersed on the OMC support and grew bigger with the increasing calcination temperature. The catalyst prepared with a lower calcination temperature showed higher decomposition efficiency towards 4CP and H202, but more metals were leached. The effect of different operational parameters such as initial pH, H202 dosage, and reaction temperature on the catalytic activity was evaluated. The results showed that 96.1% of 4CP and 47.4% of TOC was removed after 270 min at 30℃, initial pH of 3 and 6.6 mmol/L H202.88% of 4CP removal efficiency was retained after three successive runs, indicating Fe/OMC a stable catalyst for Fenton reaction. 4CP was degraded predominately by the attack of hydroxyl radical formed on the catalyst surface and in the bulk solution due to iron leaching. Based on the degradation intermediates detected by high performance liquid chromatography, possible oxidation pathways were proposed during the 4CP degradation.展开更多
以F127为模板剂,Ni Cl2为镍源,尿素为氮源,间苯二酚甲醛原位聚合树脂为碳源,分别采用均相法和两相法制备Ni-NOMC-1,Ni-N-OMC-2纳米复合材料。X射线衍射(XRD)、激光拉曼以及透射电子显微镜(TEM)等测试结果表明,复合材料具有有序介孔结构...以F127为模板剂,Ni Cl2为镍源,尿素为氮源,间苯二酚甲醛原位聚合树脂为碳源,分别采用均相法和两相法制备Ni-NOMC-1,Ni-N-OMC-2纳米复合材料。X射线衍射(XRD)、激光拉曼以及透射电子显微镜(TEM)等测试结果表明,复合材料具有有序介孔结构,Ni以金属微粒形式嵌于碳骨架中,提高了有序介孔碳的石墨化程度。X射线光电子能谱测试(XPS)表明尿素热解后以4种形式存在:sp3杂化与C结合的N原子,吡啶N原子,sp2杂化与C结合的N原子以及quaternary-N原子。Ni-N的共改性改变了碳载体的理化性质,有利于Pt纳米粒子的负载与分散。均相法制备的Ni-N-OMC-1复合材料微波负载Pt后,氧还原极限电流密度为5.32 m A·cm-2,氢氧化电化学活性面积高达138.53 m2·g-1,电化学催化活性优于商业20%Pt/C材料(4.49 m A·cm-2,96.98 m2·g-1)。展开更多
In spite of silicon has a superior theoretical capacity, the large volume expansion of Si anodes during Li^+ insertion/extraction is the bottle neck that results in fast capacity fading and poor cycling performance. I...In spite of silicon has a superior theoretical capacity, the large volume expansion of Si anodes during Li^+ insertion/extraction is the bottle neck that results in fast capacity fading and poor cycling performance. In this paper, we report a silicon, single-walled carbon nanotube, and ordered mesoporous carbon nanocomposite synthesized by an evaporation-induced self-assembly process, in which silicon nanoparticles and single-walled carbon nanotubes were added into the phenolic resol with F-127 for co-condensation. The ordered mesoporous carbon matrix and single-walled carbon nanotubes network could effectively accommodate the volume change of silicon nanoparticles, and the ordered mesoporous structure could also provide efficient channels for the fast transport of Li-ions. As a consequence, this hybrid material exhibits a reversible capacity of 861 mAh g^(-1) after 150 cycles at a current density of 400 mAg^(-1). It achieves significant improvement in the electrochemical performance when compared with the raw materials and Si nanoparticle anodes.展开更多
基金financial supported by the National Natural Science Foundation of China(No.20607023,21177130)the Major Science and Technology Program for Water Pollution Control and Treatment(No.2012ZX072020061)
文摘Ordered mesoporous carbon supported iron catalysts （Fe/OMC） were prepared by the incipient wetness impregnation method and investigated in Fenton-like degradation of 4-chlorophenol （4CP） in this work. XRD and TEM characterization showed that the iron oxides were well dispersed on the OMC support and grew bigger with the increasing calcination temperature. The catalyst prepared with a lower calcination temperature showed higher decomposition efficiency towards 4CP and H202, but more metals were leached. The effect of different operational parameters such as initial pH, H202 dosage, and reaction temperature on the catalytic activity was evaluated. The results showed that 96.1% of 4CP and 47.4% of TOC was removed after 270 min at 30℃, initial pH of 3 and 6.6 mmol/L H202.88% of 4CP removal efficiency was retained after three successive runs, indicating Fe/OMC a stable catalyst for Fenton reaction. 4CP was degraded predominately by the attack of hydroxyl radical formed on the catalyst surface and in the bulk solution due to iron leaching. Based on the degradation intermediates detected by high performance liquid chromatography, possible oxidation pathways were proposed during the 4CP degradation.
文摘以F127为模板剂,Ni Cl2为镍源,尿素为氮源,间苯二酚甲醛原位聚合树脂为碳源,分别采用均相法和两相法制备Ni-NOMC-1,Ni-N-OMC-2纳米复合材料。X射线衍射(XRD)、激光拉曼以及透射电子显微镜(TEM)等测试结果表明,复合材料具有有序介孔结构,Ni以金属微粒形式嵌于碳骨架中,提高了有序介孔碳的石墨化程度。X射线光电子能谱测试(XPS)表明尿素热解后以4种形式存在:sp3杂化与C结合的N原子,吡啶N原子,sp2杂化与C结合的N原子以及quaternary-N原子。Ni-N的共改性改变了碳载体的理化性质,有利于Pt纳米粒子的负载与分散。均相法制备的Ni-N-OMC-1复合材料微波负载Pt后,氧还原极限电流密度为5.32 m A·cm-2,氢氧化电化学活性面积高达138.53 m2·g-1,电化学催化活性优于商业20%Pt/C材料(4.49 m A·cm-2,96.98 m2·g-1)。
基金supported by the National Natural Science Foundation of China(NO.91434203,21276257,91534109)"Strategic Priority Research Program" of the Chinese Academy of Sciences(Grant No.XDA09010103)External Cooperation Program of BIC of the Chinese Academy of Sciences(Grant No.GJHZ201306)
文摘In spite of silicon has a superior theoretical capacity, the large volume expansion of Si anodes during Li^+ insertion/extraction is the bottle neck that results in fast capacity fading and poor cycling performance. In this paper, we report a silicon, single-walled carbon nanotube, and ordered mesoporous carbon nanocomposite synthesized by an evaporation-induced self-assembly process, in which silicon nanoparticles and single-walled carbon nanotubes were added into the phenolic resol with F-127 for co-condensation. The ordered mesoporous carbon matrix and single-walled carbon nanotubes network could effectively accommodate the volume change of silicon nanoparticles, and the ordered mesoporous structure could also provide efficient channels for the fast transport of Li-ions. As a consequence, this hybrid material exhibits a reversible capacity of 861 mAh g^(-1) after 150 cycles at a current density of 400 mAg^(-1). It achieves significant improvement in the electrochemical performance when compared with the raw materials and Si nanoparticle anodes.
