Heterogeneous Fenton/photo Fenton type processes using a Fe-exchanged zeolite of Y-type have been applied for the degradation of a model textile synthetic water based on Black B azodye. Research work has been directed...Heterogeneous Fenton/photo Fenton type processes using a Fe-exchanged zeolite of Y-type have been applied for the degradation of a model textile synthetic water based on Black B azodye. Research work has been directed to compare process efficiency and to establish their advantages over corresponding homogenous Fenton type processes. By optimizing the amount of reactants and process conditions, a complete decolorization of the effluent and a reduction greater than 80 per cent in the total organic carbon content is achieved. The influence of solar radiation on the heterogeneous process has been also studied. Homogeneous and heterogeneous Fenton processes yielded similar decolorization and mineralization, but the concentration of Fe ions in the bulk after the treatment was not significant in the latter case. Moreover, the catalyst support can be reused in successive cycles without significant loss of effectiveness. The use of solar radiation as a source of energy for operating the process accelerates the decomposition of azodye, making the process economical and environmentally sustainable.展开更多
Chemodynamic therapy(CDT)as an emerging modality in cancer treatment,its implementation remains a daunting challenge by the lack of smart Fenton catalyst under acidic tumor microenvironments.Herein,we have successfull...Chemodynamic therapy(CDT)as an emerging modality in cancer treatment,its implementation remains a daunting challenge by the lack of smart Fenton catalyst under acidic tumor microenvironments.Herein,we have successfully constructed a Fe_(3)O_(4)@MIL-100 heterojunction by growing Fe-based metal-organic framework(MIL-100)onto the surface of Fe_(3)O_(4) nanoparticles.The as-made heterojunction after encapsu-lating glucose oxidase(termed FMG)is demonstrated as a pH-responsive intelligent Fenton nanosystem with the synergistic effect of starvation therapy(ST).Density functional theory(DFT)calculations reveal that such heterojunction could greatly reduce the energy barrier of the Fenton reaction,which better ex-plains the mechanism of Fenton performance improvement.Moreover,the encapsulated glucose oxidase has successfully activated the ST process,in which its generated H_(2)O_(2) and gluconic acid further improve the CDT efficiency.More O_(2) from the enhanced CDT in turn promotes the enzymatic reaction of glucose oxidase.The Fenton/cascade enzymatic reaction operates in a self-feedback manner as proposed.In vitro and in vivo experiments demonstrate that such intelligent Fenton nanoreactors provide a powerful anti-cancer mechanism for effective tumor ablation with enough safety.This work provides insights into the developments of MOF-based heterojunctions as powerful anticancer treatment nanoreactors.展开更多
Fenton reaction is one of most promising approaches for efficient removal of various robust organic pollutants in wastewater,however it faces several intrinsic challenges such as acidic condition,sludge waste and sens...Fenton reaction is one of most promising approaches for efficient removal of various robust organic pollutants in wastewater,however it faces several intrinsic challenges such as acidic condition,sludge waste and sensitive to sulfide-containing compound.Here we reported a novel FeS1.92 as an efficient and sulfide resistant heterogeneous Fenton catalyst under mild condition.This novel FeS1.92 was facilely prepared through a mechanochemical synthesis of mackinawite(FeS) with sulfur powder(S) by ball milling.The sulfured mackinawite(FeS1.92) exhibits high performance in activating H2 O2 to generate hydroxyle radicals for organic waste remediation.Furthermore,this FeS1.92 based heterogeneous Fenton catalyst is highly sulfide resistant and shows improved performance for degrading sulfide-containing organic pollutants.This study provides an effective mechanochemical approach to fabricate heterogeneous Fenton catalysts for sulfide-containing wastewater treatment.展开更多
In order to overcome the drawback of the low degree of separation from an aqueous solution of MnO_2, Fe_3 O_4-MnO_2 core-shell nanocomposites were used as heterogeneous Fenton-like catalysts for the removal of acid or...In order to overcome the drawback of the low degree of separation from an aqueous solution of MnO_2, Fe_3 O_4-MnO_2 core-shell nanocomposites were used as heterogeneous Fenton-like catalysts for the removal of acid orange 7. On the basis of the catalyst characterization, the catalytic ability of the as-synthesized nanocomposites was examined. The results showed that Fe304-Mn02 core-shell nanocomposites had greater catalytic ability than Fe_3 O_4 or MnO_2 used alone. Meanwhile, the catalyst dosage, H_2 O_2 dosage, temperature, and initial pH had significant effects on the removal of acid orange 7. A high degree of stability and reusability were exhibited by Fe_3 O_4-MnO_2 core-shell nanocomposites. Both HO· and HO_2· were generated in the reaction and HO· was the main radical for the removal of acid orange 7. A mechanism for H_2 O_2 catalytic decomposition using Fe_3 O_4-MnO_2 core-shell nanocomposites to produce HO·is proposed.展开更多
A novel Fe-Pd bifunctional catalyst supported on mesh-type γ-Al<sub>2</sub>O<sub>3</sub>/Al was prepared and applied in the degradation of Rhodamine B (RhB). The monolithic mesh-type Fe-Pd/γ-...A novel Fe-Pd bifunctional catalyst supported on mesh-type γ-Al<sub>2</sub>O<sub>3</sub>/Al was prepared and applied in the degradation of Rhodamine B (RhB). The monolithic mesh-type Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al bifunctional catalyst could be separated from the solution directly and could synthesize H<sub>2</sub>O<sub>2</sub> in situ. The characterization results showed that Fe could improve the dispersion of Pd<sup>0</sup>, and the electronic interactions between Pd and Fe could increase the Pd<sup>0</sup> contents on the catalyst, which increased the productivity of H<sub>2</sub>O<sub>2</sub>. Furthermore, DFT calculations proved that the addition of Fe could inhibit the dissociation of O<sub>2</sub> and promote the nondissociative hydrogenation of O<sub>2</sub> on the surface of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al, which resulted in the increasement of H<sub>2</sub>O<sub>2</sub> selectivity. Finally, the in-situ synthesized H<sub>2</sub>O<sub>2</sub> by Pd was furtherly decomposed in situ by Fe to generate<span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span style="white-space:normal;color:#FFFFFF;font-family:Roboto, " background-color:#d46399;"=""><img src="Edit_e6a13073-7151-40b7-b2c3-a59a59d064fc.png" alt="" /></span></span></span>OH radicals to degrade organic pollutants. Therefore, Fe-Pd/ γ-Al<sub>2</sub>O<sub>3</sub>/Al catalysts exhibited excellent catalytic activity in the in-situ synthesis of H<sub>2</sub>O<sub>2</sub> and the degradation of RhB due to the synergistic effects between Pd and Fe on the catalyst. It provided a new idea for the design of bifunctional electro-Fenton catalysts. Ten cycles of experiments showed that the catalytic activity of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al catalyst could be maintained for a long time.展开更多
文摘Heterogeneous Fenton/photo Fenton type processes using a Fe-exchanged zeolite of Y-type have been applied for the degradation of a model textile synthetic water based on Black B azodye. Research work has been directed to compare process efficiency and to establish their advantages over corresponding homogenous Fenton type processes. By optimizing the amount of reactants and process conditions, a complete decolorization of the effluent and a reduction greater than 80 per cent in the total organic carbon content is achieved. The influence of solar radiation on the heterogeneous process has been also studied. Homogeneous and heterogeneous Fenton processes yielded similar decolorization and mineralization, but the concentration of Fe ions in the bulk after the treatment was not significant in the latter case. Moreover, the catalyst support can be reused in successive cycles without significant loss of effectiveness. The use of solar radiation as a source of energy for operating the process accelerates the decomposition of azodye, making the process economical and environmentally sustainable.
基金supported by the Hainan Provincial Key Research and Development Program(No.ZDYF2021SHFZ246)the National Natural Science Foundation of China(Nos.52003069 and 51872263).
文摘Chemodynamic therapy(CDT)as an emerging modality in cancer treatment,its implementation remains a daunting challenge by the lack of smart Fenton catalyst under acidic tumor microenvironments.Herein,we have successfully constructed a Fe_(3)O_(4)@MIL-100 heterojunction by growing Fe-based metal-organic framework(MIL-100)onto the surface of Fe_(3)O_(4) nanoparticles.The as-made heterojunction after encapsu-lating glucose oxidase(termed FMG)is demonstrated as a pH-responsive intelligent Fenton nanosystem with the synergistic effect of starvation therapy(ST).Density functional theory(DFT)calculations reveal that such heterojunction could greatly reduce the energy barrier of the Fenton reaction,which better ex-plains the mechanism of Fenton performance improvement.Moreover,the encapsulated glucose oxidase has successfully activated the ST process,in which its generated H_(2)O_(2) and gluconic acid further improve the CDT efficiency.More O_(2) from the enhanced CDT in turn promotes the enzymatic reaction of glucose oxidase.The Fenton/cascade enzymatic reaction operates in a self-feedback manner as proposed.In vitro and in vivo experiments demonstrate that such intelligent Fenton nanoreactors provide a powerful anti-cancer mechanism for effective tumor ablation with enough safety.This work provides insights into the developments of MOF-based heterojunctions as powerful anticancer treatment nanoreactors.
基金the National Natural Science Foundation of China (No.21777097)Shanghai Shuguang Grant(No.17SG11)the China Postdoctoral Science Foundation (Nos.2017M621483,2018T110397)。
文摘Fenton reaction is one of most promising approaches for efficient removal of various robust organic pollutants in wastewater,however it faces several intrinsic challenges such as acidic condition,sludge waste and sensitive to sulfide-containing compound.Here we reported a novel FeS1.92 as an efficient and sulfide resistant heterogeneous Fenton catalyst under mild condition.This novel FeS1.92 was facilely prepared through a mechanochemical synthesis of mackinawite(FeS) with sulfur powder(S) by ball milling.The sulfured mackinawite(FeS1.92) exhibits high performance in activating H2 O2 to generate hydroxyle radicals for organic waste remediation.Furthermore,this FeS1.92 based heterogeneous Fenton catalyst is highly sulfide resistant and shows improved performance for degrading sulfide-containing organic pollutants.This study provides an effective mechanochemical approach to fabricate heterogeneous Fenton catalysts for sulfide-containing wastewater treatment.
基金supported by the National Natural Science Foundation of China(Grant No.51508564)
文摘In order to overcome the drawback of the low degree of separation from an aqueous solution of MnO_2, Fe_3 O_4-MnO_2 core-shell nanocomposites were used as heterogeneous Fenton-like catalysts for the removal of acid orange 7. On the basis of the catalyst characterization, the catalytic ability of the as-synthesized nanocomposites was examined. The results showed that Fe304-Mn02 core-shell nanocomposites had greater catalytic ability than Fe_3 O_4 or MnO_2 used alone. Meanwhile, the catalyst dosage, H_2 O_2 dosage, temperature, and initial pH had significant effects on the removal of acid orange 7. A high degree of stability and reusability were exhibited by Fe_3 O_4-MnO_2 core-shell nanocomposites. Both HO· and HO_2· were generated in the reaction and HO· was the main radical for the removal of acid orange 7. A mechanism for H_2 O_2 catalytic decomposition using Fe_3 O_4-MnO_2 core-shell nanocomposites to produce HO·is proposed.
文摘A novel Fe-Pd bifunctional catalyst supported on mesh-type γ-Al<sub>2</sub>O<sub>3</sub>/Al was prepared and applied in the degradation of Rhodamine B (RhB). The monolithic mesh-type Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al bifunctional catalyst could be separated from the solution directly and could synthesize H<sub>2</sub>O<sub>2</sub> in situ. The characterization results showed that Fe could improve the dispersion of Pd<sup>0</sup>, and the electronic interactions between Pd and Fe could increase the Pd<sup>0</sup> contents on the catalyst, which increased the productivity of H<sub>2</sub>O<sub>2</sub>. Furthermore, DFT calculations proved that the addition of Fe could inhibit the dissociation of O<sub>2</sub> and promote the nondissociative hydrogenation of O<sub>2</sub> on the surface of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al, which resulted in the increasement of H<sub>2</sub>O<sub>2</sub> selectivity. Finally, the in-situ synthesized H<sub>2</sub>O<sub>2</sub> by Pd was furtherly decomposed in situ by Fe to generate<span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span lang="EN-US" style="white-space:normal;font-size:10pt;font-family:;" "=""><span style="white-space:normal;color:#FFFFFF;font-family:Roboto, " background-color:#d46399;"=""><img src="Edit_e6a13073-7151-40b7-b2c3-a59a59d064fc.png" alt="" /></span></span></span>OH radicals to degrade organic pollutants. Therefore, Fe-Pd/ γ-Al<sub>2</sub>O<sub>3</sub>/Al catalysts exhibited excellent catalytic activity in the in-situ synthesis of H<sub>2</sub>O<sub>2</sub> and the degradation of RhB due to the synergistic effects between Pd and Fe on the catalyst. It provided a new idea for the design of bifunctional electro-Fenton catalysts. Ten cycles of experiments showed that the catalytic activity of Fe-Pd/γ-Al<sub>2</sub>O<sub>3</sub>/Al catalyst could be maintained for a long time.
