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
Nanozymes with intrinsic enzyme-like properties and excellent stability are promising alternatives tonatural enzymes.Yet,their low density of active sites and unclear crystal structure have been the majorobstacles tha...Nanozymes with intrinsic enzyme-like properties and excellent stability are promising alternatives tonatural enzymes.Yet,their low density of active sites and unclear crystal structure have been the majorobstacles that impede their progress.Single-atom nanozymes(SAzymes)have emerged as a uniquesystem to mitigate these issues,due to maximal atomic utilization,well-defined electronic and geometricstructures,and outstanding catalytic activity distinct from their nanosized counterparts.Furthermore,thehomogeneously dispersed active sites and well-defined coordination structures provide rare pathways toshed light on the catalytic mechanisms.In this review,we summarize the latest progress in the rationaldesign and engineering of SAzymes and their applications in biomedicine and biosensing.We then con-clude the review with highlights of the remaining challenges and perspectives of this emergingtechnology.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supported,in part,by the National Science Foundation(CBET-1848841,CHE-1900235,CHE-2003685).
文摘Nanozymes with intrinsic enzyme-like properties and excellent stability are promising alternatives tonatural enzymes.Yet,their low density of active sites and unclear crystal structure have been the majorobstacles that impede their progress.Single-atom nanozymes(SAzymes)have emerged as a uniquesystem to mitigate these issues,due to maximal atomic utilization,well-defined electronic and geometricstructures,and outstanding catalytic activity distinct from their nanosized counterparts.Furthermore,thehomogeneously dispersed active sites and well-defined coordination structures provide rare pathways toshed light on the catalytic mechanisms.In this review,we summarize the latest progress in the rationaldesign and engineering of SAzymes and their applications in biomedicine and biosensing.We then con-clude the review with highlights of the remaining challenges and perspectives of this emergingtechnology.