Owing to the unique coordination environment and high atom utilization efficiency,single atom catalysts have been considered as an ideal artificial enzyme to mimic natural enzymes.Herein,single-atom Fe nanozyme anchor...Owing to the unique coordination environment and high atom utilization efficiency,single atom catalysts have been considered as an ideal artificial enzyme to mimic natural enzymes.Herein,single-atom Fe nanozyme anchored on N-doped Ti_(3)C_(2)Tx(Fe SA/N-Ti_(3)C_(2)Tx)with asymmetrically coordinated Fe-N_(1)C_(2)configuration is synthesized by vacancy capture and heteroatom doping strategy,which exhibits excellent peroxidase-like activity.Based on the results of peroxidase catalytic kinetics and X-ray adsorption fine spectroscopy,the Fe-N_(1)C_(2)active sites in Fe SA/N-Ti_(3)C_(2)Tx are responsible for the excellent performance.Furthermore,the developed Fe SA/N-Ti_(3)C_(2)Tx can be employed to quantitative detection of melatonin(MT),which shows a wide linear detection range(0.01-100μM)and an excellent detection limit(7.3 nM)in buffer,0.01-100μM and 7.8 nM in serum samples.Our work proves that MXene-based single atoms can be promising nanozyme in the field of bioassays.展开更多
Single atom catalysts(SACs)have attracted great attention,yet the quest for highly-efficient catalysts is driven by the current obstacles of ambiguous structure-performance relationship.Here,we report a nature keratin...Single atom catalysts(SACs)have attracted great attention,yet the quest for highly-efficient catalysts is driven by the current obstacles of ambiguous structure-performance relationship.Here,we report a nature keratin-based Fe-S_(1)N_(3)SACs with ultrathin two-dimensional(2D)porous carbon nanosheets structure,by controlling the active center through the precise coordination of sulfur and nitrogen.Compared with natural silk-based Fe-N_(4) catalyst,the Fe-S_(1)N_(3)SACs exhibit excellent Fenton-like oxidation degradation ability.X-ray absorption fine structure(XAFS)and electron paramagnetic resonance(EPR)results confirm that S doping is conducive to electron transfer,to accurately generate·OH with high oxidative degradation capacity at the active site.Therefore,the optimized Fe-S_(1)N_(3)catalyst showed higher oxidation degradation activity for organic pollutant substrates(methylene blue(MB),Rhodamine B(RhB)and phenol),significantly superior to Fe-N_(4) samples.This work is devoted to the treatment and application of natural fibers,which provides a novel method for the synthesis of SACs and the regulation of atomic coordination environment.展开更多
基金supported by Beijing Natural Science Foundation(No.2212018)the National Natural Science Foundation of China(No.21801015).
文摘Owing to the unique coordination environment and high atom utilization efficiency,single atom catalysts have been considered as an ideal artificial enzyme to mimic natural enzymes.Herein,single-atom Fe nanozyme anchored on N-doped Ti_(3)C_(2)Tx(Fe SA/N-Ti_(3)C_(2)Tx)with asymmetrically coordinated Fe-N_(1)C_(2)configuration is synthesized by vacancy capture and heteroatom doping strategy,which exhibits excellent peroxidase-like activity.Based on the results of peroxidase catalytic kinetics and X-ray adsorption fine spectroscopy,the Fe-N_(1)C_(2)active sites in Fe SA/N-Ti_(3)C_(2)Tx are responsible for the excellent performance.Furthermore,the developed Fe SA/N-Ti_(3)C_(2)Tx can be employed to quantitative detection of melatonin(MT),which shows a wide linear detection range(0.01-100μM)and an excellent detection limit(7.3 nM)in buffer,0.01-100μM and 7.8 nM in serum samples.Our work proves that MXene-based single atoms can be promising nanozyme in the field of bioassays.
基金This work was supported by the Beijing Natural Science Foundation(No.2212018)the National Natural Science Foundation of China(No.22105116)+2 种基金Natural Science Foundation of Hebei Province(No.B2021208001)Key Research and Development Program of Shijiazhuang(No.221070361A)the Beijing Institute of Technology Research Fund Program for Young Scholars。
文摘Single atom catalysts(SACs)have attracted great attention,yet the quest for highly-efficient catalysts is driven by the current obstacles of ambiguous structure-performance relationship.Here,we report a nature keratin-based Fe-S_(1)N_(3)SACs with ultrathin two-dimensional(2D)porous carbon nanosheets structure,by controlling the active center through the precise coordination of sulfur and nitrogen.Compared with natural silk-based Fe-N_(4) catalyst,the Fe-S_(1)N_(3)SACs exhibit excellent Fenton-like oxidation degradation ability.X-ray absorption fine structure(XAFS)and electron paramagnetic resonance(EPR)results confirm that S doping is conducive to electron transfer,to accurately generate·OH with high oxidative degradation capacity at the active site.Therefore,the optimized Fe-S_(1)N_(3)catalyst showed higher oxidation degradation activity for organic pollutant substrates(methylene blue(MB),Rhodamine B(RhB)and phenol),significantly superior to Fe-N_(4) samples.This work is devoted to the treatment and application of natural fibers,which provides a novel method for the synthesis of SACs and the regulation of atomic coordination environment.
