光催化灭活是公认的控制病原微生物最具前景手段之一。本文以尿素和硫代巴比妥酸为起始原料,通过热聚合反应制备S掺杂g-C_(3)N_(4)(SCN),随后采用光还原法将Ag纳米粒负载于SCN表面获得新颖的可见光响应型Ag/SCN抗菌材料。对所制备纳米...光催化灭活是公认的控制病原微生物最具前景手段之一。本文以尿素和硫代巴比妥酸为起始原料,通过热聚合反应制备S掺杂g-C_(3)N_(4)(SCN),随后采用光还原法将Ag纳米粒负载于SCN表面获得新颖的可见光响应型Ag/SCN抗菌材料。对所制备纳米材料进行XRD、SEM、TEM、XPS及UV-Vis DRS表征,并深入探讨其在可见光下灭活大肠杆菌(E.coli)的性能和机制。结果表明,Ag纳米粒均匀且牢固地负载在SCN表面,纳米材料表现出显著增强的可见光响应能力。当负载量为6%时,Ag/SCN-6呈现出最佳的光催化灭菌活性,60 min内能够将6.2 lg CFU·mL^(-1)的E.coli全部灭活。自由基捕获实验结果表明,超氧自由基(·O-2)是灭活过程中最主要活性物种,它协同光生空穴(h+)和羟基自由基(·OH)主导了光催化抗菌的进程。展开更多
Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with ...Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.展开更多
Superwetting materials have drawn unprecedented attention in the treatment of oily wastewater due to their preferable anti-fouling property and selective oil/water separation.However,it is still a challenge to fabrica...Superwetting materials have drawn unprecedented attention in the treatment of oily wastewater due to their preferable anti-fouling property and selective oil/water separation.However,it is still a challenge to fabricate multifunctional and environmentally friendly materials,which can be stably applied to purify the actual complicated wastewater.Here,a Ag/Ag/α-Fe_(2)O_(3) heterostructure anchored copper mesh was intentionally synthesized using a facile two-step hydrothermal method.The resultant mesh with superhydrophilicity and underwater superoleophobicity was capable of separating various oil/water mixtures with superior separation efficiency and high permeationflux driven by gravity.Benefiting from the joint effects of the smaller band gap of Ag/α-Fe_(2)O_(3) heterojunction,inherent antibacterial capacity of Ag/α-Fe_(2)O_(3) and Ag nanoparticles,favorable conductive substrate,as well as the hierarchical structure with superwettability,such mesh presented remarkably enhanced degradation capability toward organic dyes under visible light irradiation and antibacterial activity against both Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus)compared with the pure Ag/α-Fe_(2)O_(3) coated mesh.Impressively,the mesh exhibited bifunctional water purification performance,in which organic dyes were eliminated simultaneously from water during oil/water separation in onefiltration process.More importantly,this mesh behaved exceptional chemical resistance,mechanical stability and long-term reusability.Therefore,this material with multifunctional integration may hold promising potential for steady water purification in practice.展开更多
This study was aimed to investigate the effects of hydrothermal aging, propene and SO<sub>2</sub> poisoning on the ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) performance of both...This study was aimed to investigate the effects of hydrothermal aging, propene and SO<sub>2</sub> poisoning on the ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) performance of both Cu-SAPO-34 and Cu-ZSM-5. The catalytic activities of fresh, aged and poisoned samples were tested in ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) of NO<sub>x</sub> conditions. The XRD, TG and N<sub>2</sub>-desorption results showed that the structures of the Cu-SAPO-34 and Cu-ZSM-5 remained intact after 750˚C hydrothermally aged, SO<sub>2</sub> and propene poisoned. After hydrothermal aging at 750˚C for 12 h, the NO reduction performance of Cu-ZSM-5 was significantly reduced at lower temperatures, while that of Cu-SAPO-34 was less affected. Moreover, Cu-SAPO-34 catalyst showed high NO conversion with SO<sub>2</sub> or propene compared to Cu-ZSM-5. However, Cu-ZSM-5 showed a larger drop in catalytic activity with SO<sub>2</sub> or propene compared to Cu-SAPO-34 catalyst. The H<sub>2</sub>-TPR results showed that Cu<sup>2 </sup> ions could be reduced to Cu<sup> </sup> and Cu<sup>0</sup> for Cu-ZSM-5, while no significant transformation of copper species was observed for Cu-SAPO-34. Meanwhile, the UV-vis DRS results showed that CuO species were formed in Cu-ZSM-5, while little changes were observed for the Cu-SAPO-34. Cu-SAPO-34 showed high sulfur and hydrocarbon poison resistance compared to Cu-ZSM-5. In summary, Cu-SAPO-34 with small-pore zeolite showed higher hydrothermal stability and better hydrocarbon and sulfur poison resistant than Cu-ZSM-5 with medium-pore.展开更多
文摘光催化灭活是公认的控制病原微生物最具前景手段之一。本文以尿素和硫代巴比妥酸为起始原料,通过热聚合反应制备S掺杂g-C_(3)N_(4)(SCN),随后采用光还原法将Ag纳米粒负载于SCN表面获得新颖的可见光响应型Ag/SCN抗菌材料。对所制备纳米材料进行XRD、SEM、TEM、XPS及UV-Vis DRS表征,并深入探讨其在可见光下灭活大肠杆菌(E.coli)的性能和机制。结果表明,Ag纳米粒均匀且牢固地负载在SCN表面,纳米材料表现出显著增强的可见光响应能力。当负载量为6%时,Ag/SCN-6呈现出最佳的光催化灭菌活性,60 min内能够将6.2 lg CFU·mL^(-1)的E.coli全部灭活。自由基捕获实验结果表明,超氧自由基(·O-2)是灭活过程中最主要活性物种,它协同光生空穴(h+)和羟基自由基(·OH)主导了光催化抗菌的进程。
基金supported by National Natural Science Foundation of China(52208272,41706080 and 51702328)the Basic Scientific Fund for National Public Research Institutes of China(2020S02 and 2019Y03)+3 种基金the Basic Frontier Science Research Program of Chinese Academy of Sciences(ZDBS-LY-DQC025)the Young Elite Scientists Sponsorship Program by CAST(No.YESS20210201)the Strategic Leading Science&Technology Program of the Chinese Academy of Sciences(XDA13040403)the Key Research and Development Program of Shandong Province(Major Scientific and Technological Innovation Project)(2019JZZY020711).
文摘Since the catalytic activity of most nanozymes is still far lower than the corresponding natural enzymes,there is urgent need to discover novel highly efficient enzyme-like materials.In this work,Co_(3)V_(2)O_(8)with hollow hexagonal prismatic pencil structures were prepared as novel artificial enzyme mimics.They were then decorated by photo-depositing Ag nanoparticles(Ag NPs)on the surface to further improve its catalytic activities.The Ag NPs decorated Co_(3)V_(2)O_(8)(ACVPs)showed both excellent oxidase-and peroxidase-like catalytic activities.They can oxidize the colorless 3,3’,5,5’-tetramethylbenzidine rapidly to induce a blue change.The enhanced enzyme mimetic activities can be attributed to the surface plasma resonance(SPR)effect of Ag NPs as well as the synergistic catalytic effect between Ag NPs and Co_(3)V_(2)O_(8),accelerating electron transfer and promoting the catalytic process.ACVPs were applied in constructing a colorimetric sensor,validating the occurrence of the Fenton reaction,and disinfection,presenting favorable catalytic performance.The enzyme-like catalytic mechanism was studied,indicating the chief role of⋅O_(2)-radicals in the catalytic process.This work not only discovers a novel functional material with double enzyme mimetic activity but also provides a new insight into exploiting artificial enzyme mimics with highly efficient catalytic ability.
基金This work was financially supported by the Shandong Provincial Natural Science Foundation(ZR2020QB116)the Excellent Young Talents Foundation in Universities of Anhui Province(gxyq2021223)the Key Research Project of Natural Science in Universities of Anhui Province.(KJ2020A0749).
文摘Superwetting materials have drawn unprecedented attention in the treatment of oily wastewater due to their preferable anti-fouling property and selective oil/water separation.However,it is still a challenge to fabricate multifunctional and environmentally friendly materials,which can be stably applied to purify the actual complicated wastewater.Here,a Ag/Ag/α-Fe_(2)O_(3) heterostructure anchored copper mesh was intentionally synthesized using a facile two-step hydrothermal method.The resultant mesh with superhydrophilicity and underwater superoleophobicity was capable of separating various oil/water mixtures with superior separation efficiency and high permeationflux driven by gravity.Benefiting from the joint effects of the smaller band gap of Ag/α-Fe_(2)O_(3) heterojunction,inherent antibacterial capacity of Ag/α-Fe_(2)O_(3) and Ag nanoparticles,favorable conductive substrate,as well as the hierarchical structure with superwettability,such mesh presented remarkably enhanced degradation capability toward organic dyes under visible light irradiation and antibacterial activity against both Escherichia coli(E.coli)and Staphylococcus aureus(S.aureus)compared with the pure Ag/α-Fe_(2)O_(3) coated mesh.Impressively,the mesh exhibited bifunctional water purification performance,in which organic dyes were eliminated simultaneously from water during oil/water separation in onefiltration process.More importantly,this mesh behaved exceptional chemical resistance,mechanical stability and long-term reusability.Therefore,this material with multifunctional integration may hold promising potential for steady water purification in practice.
文摘This study was aimed to investigate the effects of hydrothermal aging, propene and SO<sub>2</sub> poisoning on the ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) performance of both Cu-SAPO-34 and Cu-ZSM-5. The catalytic activities of fresh, aged and poisoned samples were tested in ammonia-selective catalytic reduction (NH<sub>3</sub>-SCR) of NO<sub>x</sub> conditions. The XRD, TG and N<sub>2</sub>-desorption results showed that the structures of the Cu-SAPO-34 and Cu-ZSM-5 remained intact after 750˚C hydrothermally aged, SO<sub>2</sub> and propene poisoned. After hydrothermal aging at 750˚C for 12 h, the NO reduction performance of Cu-ZSM-5 was significantly reduced at lower temperatures, while that of Cu-SAPO-34 was less affected. Moreover, Cu-SAPO-34 catalyst showed high NO conversion with SO<sub>2</sub> or propene compared to Cu-ZSM-5. However, Cu-ZSM-5 showed a larger drop in catalytic activity with SO<sub>2</sub> or propene compared to Cu-SAPO-34 catalyst. The H<sub>2</sub>-TPR results showed that Cu<sup>2 </sup> ions could be reduced to Cu<sup> </sup> and Cu<sup>0</sup> for Cu-ZSM-5, while no significant transformation of copper species was observed for Cu-SAPO-34. Meanwhile, the UV-vis DRS results showed that CuO species were formed in Cu-ZSM-5, while little changes were observed for the Cu-SAPO-34. Cu-SAPO-34 showed high sulfur and hydrocarbon poison resistance compared to Cu-ZSM-5. In summary, Cu-SAPO-34 with small-pore zeolite showed higher hydrothermal stability and better hydrocarbon and sulfur poison resistant than Cu-ZSM-5 with medium-pore.
