This study comprehensively investigates the degradation performance and mechanism of environmental persistent pollutants(EPs)by combining experimental and theoretical calculations with dielectric barrier discharge(DBD...This study comprehensively investigates the degradation performance and mechanism of environmental persistent pollutants(EPs)by combining experimental and theoretical calculations with dielectric barrier discharge(DBD)plasma synergized with persulfate.The findings demonstrated that DBD plasma could generate reactive radicals,including·OH,^(1)O_(2) and·O_(2)^(-),which primarily activate persulfate through OH and·O_(2)^(-)to produce the potent oxidizing radical SO_4^(-).This process facilitated enhanced degradation and mineralization of MeP wastewater.The performance of DBD/persulfute(PS)in degrading MeP was evaluated by kinetics,energy efficiency,and co-factor calculations,combined with degradation under different influencing factors.The actives in the system were analyzed by free radical scavenging assays and UV spectrophotometric testing to determine their effects.The findings indicated that persulfate was effectively activated by DBD plasma and that·O_(2)^(-)played a significant role.The presence of persulfate elevated the levels of H_(2)O_(2) and O_(3) in the solution.The intermediates formed during the degradation of MeP were detected using LC-MS and then analyzed alongside density-functional theory(DFT)chemical predictions to anticipate the reactive sites and deduce the potential degradation pathways of methylparaben(MeP).Toxicity evaluation software confirmed that the PS/DBD system reduces acute and developmental toxicity in the water column.The study showed that DBD plasma-activated persulfate was successful in addre ssing newly identified contaminants.展开更多
Hard carbons(HCs)are commercial anode materials for sodium-ion batteries(SIBs),yet their electrochemical performance remains limited by intrinsic structural deficiencies and insufficient Na+storage kinetics.Herein,we ...Hard carbons(HCs)are commercial anode materials for sodium-ion batteries(SIBs),yet their electrochemical performance remains limited by intrinsic structural deficiencies and insufficient Na+storage kinetics.Herein,we report oxygen manipulation in hard carbon,enabled by plasma and laser beam,for improved Na^(+)storage.Starting with commercial HC electrodes,oxygen atoms were first implanted into carbon layers via atmospheric plasma treatment under controlled oxygen partial pressure.Subsequent laser irradiation induced localized thermal shocks that selectively remove oxygen atoms from edge sites,triggering transient carbon lattice rearrangement to simultaneously generate intrinsic defects and optimally sized closed nanopores(1.2-2.0 nm).This dual-stage regulation yielded HC anodes with exceptional Na^(+)storage properties,achieving a high reversible capacity of 335 mAh·g^(-1)at 30 mA·g^(-1)(with 36% enhancement compared with pristine HC)and enhanced Na+diffusion.Through in situ Raman and correlated ex situ spectroscopy analyses(electron paramagnetic resonance(EPR)and X-ray photoelectron spectroscopy(XPS)),we systematically decode the multiscale Na^(+)storage mechanism involving defect adsorption,interlayer intercalation,and nanopore filling.The proposed methodology bridges atomic-scale structural engineering with macroscopic electrode performance optimization,offering a scalable green manufacturing pathway for next-generation SIBs.展开更多
The design and fabrication of advanced soft actuators with programmable actuation are highly desirable in constructing intelligent soft robots.In this work,a programmable light-driven liquid crystalline network(LCN)-b...The design and fabrication of advanced soft actuators with programmable actuation are highly desirable in constructing intelligent soft robots.In this work,a programmable light-driven liquid crystalline network(LCN)-based soft actuator was judiciously designed and prepared by constructing structural anisotropy across the thickness of the film.A three-dimensional(3D)deformable LCN actuator was realized by polymerization-induced phase separation of small-molarweight monomers and polymer networks.The resultant anisotropic LCN displays anisotropic microscale nanoporous architecture across the thickness in addition to uniform alignment at the molecular scale.The actuation behaviors of LCN film are tunable by adjusting the size and distribution of nanopores in LCN bulk via changing polymerization conditions and monomer components.More importantly,the nanoporous LCN film can be harnessed as a promising template to achieve diverse light responsiveness by changing the photothermal dyes via a feasible washing and refilling process,demonstrating a reprogrammable light-driven soft actuator.展开更多
基金supported by the National Natural Science Foundation of China(50867003)。
文摘This study comprehensively investigates the degradation performance and mechanism of environmental persistent pollutants(EPs)by combining experimental and theoretical calculations with dielectric barrier discharge(DBD)plasma synergized with persulfate.The findings demonstrated that DBD plasma could generate reactive radicals,including·OH,^(1)O_(2) and·O_(2)^(-),which primarily activate persulfate through OH and·O_(2)^(-)to produce the potent oxidizing radical SO_4^(-).This process facilitated enhanced degradation and mineralization of MeP wastewater.The performance of DBD/persulfute(PS)in degrading MeP was evaluated by kinetics,energy efficiency,and co-factor calculations,combined with degradation under different influencing factors.The actives in the system were analyzed by free radical scavenging assays and UV spectrophotometric testing to determine their effects.The findings indicated that persulfate was effectively activated by DBD plasma and that·O_(2)^(-)played a significant role.The presence of persulfate elevated the levels of H_(2)O_(2) and O_(3) in the solution.The intermediates formed during the degradation of MeP were detected using LC-MS and then analyzed alongside density-functional theory(DFT)chemical predictions to anticipate the reactive sites and deduce the potential degradation pathways of methylparaben(MeP).Toxicity evaluation software confirmed that the PS/DBD system reduces acute and developmental toxicity in the water column.The study showed that DBD plasma-activated persulfate was successful in addre ssing newly identified contaminants.
基金financially supported by the National Key Research and Development Program of China(No.2023YFB4203702)the National Natural Science Foundation of China(Nos.22179145,22005341,and 22309206)+4 种基金Shandong Provincial Natural Science Foundation(No.ZR2020QB128)Taishan Scholars Program of Shandong Province(No.tsqn20221117)Shandong Provincial Excellent Young Scientists Fund Program(Overseas)(No.2024HWYQ-047)Qingdao Natural Science Foundation(Nos.24-8-4-zrjj-jch and 23-2-1-24-zyyd-jch)Science and Technology Park Incubation Program Project of Qingdao City(No.25-1-1-yqpy-33-qy).
文摘Hard carbons(HCs)are commercial anode materials for sodium-ion batteries(SIBs),yet their electrochemical performance remains limited by intrinsic structural deficiencies and insufficient Na+storage kinetics.Herein,we report oxygen manipulation in hard carbon,enabled by plasma and laser beam,for improved Na^(+)storage.Starting with commercial HC electrodes,oxygen atoms were first implanted into carbon layers via atmospheric plasma treatment under controlled oxygen partial pressure.Subsequent laser irradiation induced localized thermal shocks that selectively remove oxygen atoms from edge sites,triggering transient carbon lattice rearrangement to simultaneously generate intrinsic defects and optimally sized closed nanopores(1.2-2.0 nm).This dual-stage regulation yielded HC anodes with exceptional Na^(+)storage properties,achieving a high reversible capacity of 335 mAh·g^(-1)at 30 mA·g^(-1)(with 36% enhancement compared with pristine HC)and enhanced Na+diffusion.Through in situ Raman and correlated ex situ spectroscopy analyses(electron paramagnetic resonance(EPR)and X-ray photoelectron spectroscopy(XPS)),we systematically decode the multiscale Na^(+)storage mechanism involving defect adsorption,interlayer intercalation,and nanopore filling.The proposed methodology bridges atomic-scale structural engineering with macroscopic electrode performance optimization,offering a scalable green manufacturing pathway for next-generation SIBs.
基金supported by the National Natural Science Foundation of China(Grant No.52202081)Natural Science Foundation of Jiangxi Province(Grant No.20232BAB204030).
文摘The design and fabrication of advanced soft actuators with programmable actuation are highly desirable in constructing intelligent soft robots.In this work,a programmable light-driven liquid crystalline network(LCN)-based soft actuator was judiciously designed and prepared by constructing structural anisotropy across the thickness of the film.A three-dimensional(3D)deformable LCN actuator was realized by polymerization-induced phase separation of small-molarweight monomers and polymer networks.The resultant anisotropic LCN displays anisotropic microscale nanoporous architecture across the thickness in addition to uniform alignment at the molecular scale.The actuation behaviors of LCN film are tunable by adjusting the size and distribution of nanopores in LCN bulk via changing polymerization conditions and monomer components.More importantly,the nanoporous LCN film can be harnessed as a promising template to achieve diverse light responsiveness by changing the photothermal dyes via a feasible washing and refilling process,demonstrating a reprogrammable light-driven soft actuator.
