The development of novel nanozymes for environmental contamination remediation is a worthwhile research direction.However,most of the reported nanozymes cannot degrade efficiently due to the limitation of the internal...The development of novel nanozymes for environmental contamination remediation is a worthwhile research direction.However,most of the reported nanozymes cannot degrade efficiently due to the limitation of the internal active sites not being able to come into direct contact with contaminants.Therefore,we reported Fe-N-C single-atom nanozymes(SAzymes)with atomically dispersed FeN4 active sites anchored on a three-dimensional hierarchically ordered microporous-mesoporous-macroporous nitrogen doped carbon matrix(3DOM Fe-N-C)for the degradation of a targeted environmental pollutant(rhodamine B(RhB)).The three-dimensional(3D)hierarchically ordered porous structure may accelerate mass transfer and improve the accessibility of active sites.This structure and high metal atom utilization endow Fe-N-C SAzyme with enhanced tri-enzyme-mimic activities,comprising oxidase-mimic,peroxidase-mimic,and catalase-mimic activities.Based on its excellent peroxidase-mimic activity,3DOM Fe-N-C can degrade RhB by hydroxyl radicals(·OH)generated in the presence of hydrogen peroxide.This study provides a new idea for designing porous Fe-N-C SAzymes for environmental contamination remediation.展开更多
A series of β-cyclodextrin-conjugated 4-arm poly(ethylene glycol)-poly(lactide-co-glycolide) (4-arm PEG-PLGA) copolymers were synthesized by a ring-opening polymerization of D,L-lactide and glycolide using 4-a...A series of β-cyclodextrin-conjugated 4-arm poly(ethylene glycol)-poly(lactide-co-glycolide) (4-arm PEG-PLGA) copolymers were synthesized by a ring-opening polymerization of D,L-lactide and glycolide using 4-arm PEG as initiator, and then conjugated with mono(6-ethylenediamine-6-deoxy)- β-cyclodextrin (CDen) or ethylenediamino-bridged bis- β-CD (BCDen). The chemical structures of copolymers were confirmed by IH-NMR and FTIR spectroscopy. The , β-CD-conjugated PEG-PLGA formed stable reverse micelles due to the formation of fl-CD and bovine serum albumin (BSA) inclusion complexation, which could accommodate BSA in the organic solvent with improved encapsulation efficiency. Moreover, we demonstrated a one-step approach to construct macroporous protein-containing films using these reverse micelles. The films with ordered pore arrays were directly prepared from reverse micelles. Interestingly, the protein was totally located in the whole matrix except for the pores.展开更多
The development of an efficient Pt-based electrocatalyst in acidic and alkaline electrolytes is of great significance to the field of electrocatalytic hydrogen evolution.Herein,we report a strategy for in situ growth ...The development of an efficient Pt-based electrocatalyst in acidic and alkaline electrolytes is of great significance to the field of electrocatalytic hydrogen evolution.Herein,we report a strategy for in situ growth of Pt_(3)Ni truncated octahedrons on Ti3C2Tx nanosheets and then obtain an ordered porous catalyst via a template method.Meanwhile,we use the finite element calculation to clarify the relationship between the component structure and performance and find that the performance of the spherical shell microstructure catalyst is higher than that of the disc structure catalyst,which is also verified by experiments.The experimental analysis shows that the ordered porous catalyst is conducive to enhancing electrocatalytic hydrogen evolution activity in acidic and alkaline electrolytes.In an acidic solution,the overpotential is 25 mV(10 mA·cm^(−2)),and the Tafel slope is 22.86 mV·dec−1.In an alkaline solution,the overpotential is 44.1 mV(10 mA·cm^(−2)),and the Tafel slope is 39.06 mV·dec−1.The synergistic coupling between Ti3C2Tx and Pt_(3)Ni nanoparticles improves the stability of the catalyst.The in situ growth strategy and design of microstructure with its correlation with catalytic performance represent critical steps toward the rational synthesis of catalysts with excellent catalytic activity.展开更多
基金We are grateful for the support from the Ministry of Science and Technology of China(Nos.2016YFA0203203 and 2019YFA0709202)the National Natural Science Foundation of China(No.22074137).
文摘The development of novel nanozymes for environmental contamination remediation is a worthwhile research direction.However,most of the reported nanozymes cannot degrade efficiently due to the limitation of the internal active sites not being able to come into direct contact with contaminants.Therefore,we reported Fe-N-C single-atom nanozymes(SAzymes)with atomically dispersed FeN4 active sites anchored on a three-dimensional hierarchically ordered microporous-mesoporous-macroporous nitrogen doped carbon matrix(3DOM Fe-N-C)for the degradation of a targeted environmental pollutant(rhodamine B(RhB)).The three-dimensional(3D)hierarchically ordered porous structure may accelerate mass transfer and improve the accessibility of active sites.This structure and high metal atom utilization endow Fe-N-C SAzyme with enhanced tri-enzyme-mimic activities,comprising oxidase-mimic,peroxidase-mimic,and catalase-mimic activities.Based on its excellent peroxidase-mimic activity,3DOM Fe-N-C can degrade RhB by hydroxyl radicals(·OH)generated in the presence of hydrogen peroxide.This study provides a new idea for designing porous Fe-N-C SAzymes for environmental contamination remediation.
基金financially supported by the National Natural Science Foundation of China(Nos.21374079 and 21244004)Program for New Century Excellent Talents in Universities(No.NCET-11-1063)Program for Prominent Young College Teachers of Tianjin Educational Committee
文摘A series of β-cyclodextrin-conjugated 4-arm poly(ethylene glycol)-poly(lactide-co-glycolide) (4-arm PEG-PLGA) copolymers were synthesized by a ring-opening polymerization of D,L-lactide and glycolide using 4-arm PEG as initiator, and then conjugated with mono(6-ethylenediamine-6-deoxy)- β-cyclodextrin (CDen) or ethylenediamino-bridged bis- β-CD (BCDen). The chemical structures of copolymers were confirmed by IH-NMR and FTIR spectroscopy. The , β-CD-conjugated PEG-PLGA formed stable reverse micelles due to the formation of fl-CD and bovine serum albumin (BSA) inclusion complexation, which could accommodate BSA in the organic solvent with improved encapsulation efficiency. Moreover, we demonstrated a one-step approach to construct macroporous protein-containing films using these reverse micelles. The films with ordered pore arrays were directly prepared from reverse micelles. Interestingly, the protein was totally located in the whole matrix except for the pores.
基金Thanks for the financial support of the National Key R&D Program of China(Nos.2021YFB3200700 and 2016YFC1100502)the National Natural Science Foundation of China(Nos.21875260 and 21671193)+3 种基金Beijing Nature Science Foundation(No.2202069)Zhongguancun Open Laboratory Concept Verification Project(No.202205229)the Foundation of State Key Laboratory of Digital Manufacturing Equipment and Technology(No.DMETKF2022004)the China Science and Technology Cloud for calculation support.
文摘The development of an efficient Pt-based electrocatalyst in acidic and alkaline electrolytes is of great significance to the field of electrocatalytic hydrogen evolution.Herein,we report a strategy for in situ growth of Pt_(3)Ni truncated octahedrons on Ti3C2Tx nanosheets and then obtain an ordered porous catalyst via a template method.Meanwhile,we use the finite element calculation to clarify the relationship between the component structure and performance and find that the performance of the spherical shell microstructure catalyst is higher than that of the disc structure catalyst,which is also verified by experiments.The experimental analysis shows that the ordered porous catalyst is conducive to enhancing electrocatalytic hydrogen evolution activity in acidic and alkaline electrolytes.In an acidic solution,the overpotential is 25 mV(10 mA·cm^(−2)),and the Tafel slope is 22.86 mV·dec−1.In an alkaline solution,the overpotential is 44.1 mV(10 mA·cm^(−2)),and the Tafel slope is 39.06 mV·dec−1.The synergistic coupling between Ti3C2Tx and Pt_(3)Ni nanoparticles improves the stability of the catalyst.The in situ growth strategy and design of microstructure with its correlation with catalytic performance represent critical steps toward the rational synthesis of catalysts with excellent catalytic activity.