Preparation Of Copper/iron-based Catalysts By Biomass-MOFs Dual Template And Its Applicatio

With the development of society and economy,energy shortage and environmental pollution have become the focus of present research work.The existence of these problems makes researchers eager to develop new catalyst materials to alleviate the crisis.In this work,by using abundant biomass in nature and low cost and easily obtained MOFs as dual-template precursors.And then by controllable calcination,Cu/Fe based functional composite catalytic materials with highly active catalytic sites and stable pore structures were prepared.Their applications in the fields of catalytic reduction,photocatalytic hydrogen production,and photo-fenton were explored and studied.This work provided examples for the rational and effective preparation of carbon-based composite catalysts.1.Firstly,octahedral HKUST-1-P was encapsulated in corncobs,and a series of P-doped Cu/Cu₂O/C catalysts were obtained by regulating temperature calcination.The results of XRD,SEM,FT-IR,XPS,BET and UV-Vis showed the composition,morphology and structure of these composites.The catalyst prepared at 400℃showed excellent catalytic activity and high stability for the removal of 4-NP and ofloxacin.The removal rate of 4-NP and ofloxacin reached>99%within 90 s and 95.7%within 10 min respectively,which remained unchanged after six cycles.2.MOF-2 with hexahedral morphology was grown on corncob by microwave and oven.And then a series of Cu/Cu₂O/C catalysts were obtained by calcination of composite materials at different temperatures.Characterization results of XRD,SEM,BET,XPS and UV-DRS showed composition,morphology,structure and visible-light absorption properties of composites.Through 4-NP reaction,we found that although MOF-2/corncob-microwave-350 could transform 4-NP to>99%within 60 s,the catalyst could not achieve the cyclic stability result of 60 s,indicating that MOF-2/corncob-microwave-350 could not be stably applied to the reduction reaction.Then by UV-Vis DRS characterization,we found that the catalyst materials could be applied to the photocatalytic reaction.Thus,we further expanded the application of photocatalytic hydrogen production.By comparing the hydrogen production of the composites synthesized by the microwave generation method and the oven synthesis method,we found that MOF-2/corncob-oven-400 had the best hydrogen production capacity and the hydrogen production capacity could reach 2728.9μmol/g under visible light after 8 h.MOF-2/corncob-oven-400 was used in four cycles to show stable photocatalytic hydrogen production capacity.3.Fe₂O₃/C catalysts were successfully prepared by MIL-101-Fe/biomass.XRD,SEM,BET and XPS characterization results showed the presence of Fe₂O₃.We found that MIL-101-Fe/absorbent cotton-400 had the best performance for Rh B degradation reaction and we further confirm that hydroxyl radical is the main active substance in this reaction.Then,we proved that MIL-101-Fe/absorbent cotton-400 could be used in CIP,OFX and NOR degradation reaction.And the degradation efficiency of NOR was the best,up to 80.8%.The degradation tests under different p H conditions proved that the photo-fenton reaction can be carried out in a neutral environment.Then MIL-101-Fe/absorbent cotton-400 was used in four cycles of reaction,and showed a relatively stable photocatalytic degradation efficiency.