The advent of three-dimensional(3D)printed porous Mg alloys is considered a significant milestone in the development of metal-based degradable implants.However,the poor corrosion resistance of additively manufactured ...The advent of three-dimensional(3D)printed porous Mg alloys is considered a significant milestone in the development of metal-based degradable implants.However,the poor corrosion resistance of additively manufactured Mg alloys,along with the occurrences of inflammation and bacterial infections following implantation,pose critical challenges.In this study,two drug-loaded coatings were prepared within a porous Mg alloy using in situ incorporation and post-deposition of layered double hydroxides(LDHs)to enhance corrosion resistance,antibacterial properties,and biological compatibility combined with plasma electrolytic oxidation(PEO).The results revealed that in situ incorporation of LDH capsules effectively reduced the porosity of the PEO layer and improved the long-term corrosion resistance of the coating.The postdeposited LDH layer effectively sealed the PEO layer,demonstrating highly stable corrosion resistance during 7 d electrochemical impedance spectroscopy(EIS)test,with the impedance modulus at 10^(-2) Hz stabilizing at 5×10^(5)Ω·cm^(2).After soaking,the surface morphology of the in situ drug-loaded PEO coating exhibited more cracks and defects,whereas the PEO-LDH coating maintained a relatively dense morphology.Among the tested samples,the PEO-LDH coating showed the best performance in terms of corrosion resistance,cell proliferation and differentiation capabilities,and antibacterial efficacy(>99%).Its strong compatibility with the porous structure of 3D-printed Mg alloy highlights the potential of this coating system for biomedical applications.The design strategy proposed in this study offers valuable insights for future development of drug-loaded coatings for 3D-printed porous materials.展开更多
Solid-solid interface contact and slow ion transport restrict solid-state polymer electrolytes practical application.The differences in interface structure design significantly influence the interfacial Li^(+)transpor...Solid-solid interface contact and slow ion transport restrict solid-state polymer electrolytes practical application.The differences in interface structure design significantly influence the interfacial Li^(+)transport and diffusion as well as the Li atom nucleation,resulting in substantial variations in the macroscopic performance of polymer electrolytes-based solid-state Li metal batteries.Here,ceramic-polymer composite electrolytes(CPCEs)composed of polyvinylidene fluoride-hexafluoropropylene(PVDF-HFP)polymer and Li_(6.75)La_(3)Zr_(1.75)Ta_(0.25)O_(12)(LLZTO)filler has been chosen as the demo to demonstrate that the interfacial electrochemistry between CPCEs and Li anode is not only affected by the physical interface contact but also associated with the internal/interfacial Li^(+)transport mechanism.This work shows that“point to point”Li^(+)diffusion,slow uneven interfacial Li^(+)transport in CPCEs with poor ionic conductivity and rough surface lead to uneven Li atom nucleation,leading to Li dendrites growth.While,the CPCEs with high ionic conductivity and smooth surface facilitate uniform and rapid ion transport,promoting uniform Li nucleation and transverse diffusion.This work highlights the importance of the interface structure design of polymer electrolytes for Li metal interface stability in polymer electrolytes-based quasi-solid-state batteries and provides valuable insights into the interfacial electrochemistry of solidstate batteries.展开更多
We introduce a dual distribution of relaxation(DRT)based approach for analyzing electrochemical impedance spectroscopy(EIS)data in perovskite solar cells(PSCs),combining regression and classification with Bayesian mod...We introduce a dual distribution of relaxation(DRT)based approach for analyzing electrochemical impedance spectroscopy(EIS)data in perovskite solar cells(PSCs),combining regression and classification with Bayesian model selection and Havriliak-Negami(HN)modeling to resolve spectra into discrete,Lorentzian-like peaks.This time-domain decomposition offers a powerful alternative for identifying underlying physical processes,such as charge transfer,trap-assisted recombination,and ionic migration by directly extracting characteristic relaxation times(τ).In contrast to traditional equivalent circuit fitting or conventional DRT methods,which often yield broad and overlapping Gaussian-like peaks,our method enables sharper resolution of individual electrochemical signatures.Furthermore,we validated the framework using simulated EIS spectra for two distinct system types,determining the optimal number of peaks(Q)through statistical model selection.Applied to experimental PSC data under varying bias conditions,the approach helps to identify the voltage-dependent relaxation processes,including fast charge transfer(τ~10^(-6)s),intermediate trap-mediated recombination(τ~10^(-2)s),and slow ionic motion(τ~1 s).Lower-Q models fail to capture low-frequency features such as polarization and charge accumulation,while optimal Q yields accurate,physically meaningful representations of device behavior.This data-driven methodology highlights time-domain DRT as a rigorous and insightful tool for dissecting the complex kinetics that govern PSC performance.展开更多
基金Natural Foundation of Science and Technology Department of Sichuan Province(2024NSFSC0949)Sichuan Science and Technology Program(2023ZYD0115)+1 种基金LiaoNing Revitalization Talents Program(XLYC2403026)Shenyang Young and Middle-aged Science and Technology Innovation Talent Support Program(RC231178).
文摘The advent of three-dimensional(3D)printed porous Mg alloys is considered a significant milestone in the development of metal-based degradable implants.However,the poor corrosion resistance of additively manufactured Mg alloys,along with the occurrences of inflammation and bacterial infections following implantation,pose critical challenges.In this study,two drug-loaded coatings were prepared within a porous Mg alloy using in situ incorporation and post-deposition of layered double hydroxides(LDHs)to enhance corrosion resistance,antibacterial properties,and biological compatibility combined with plasma electrolytic oxidation(PEO).The results revealed that in situ incorporation of LDH capsules effectively reduced the porosity of the PEO layer and improved the long-term corrosion resistance of the coating.The postdeposited LDH layer effectively sealed the PEO layer,demonstrating highly stable corrosion resistance during 7 d electrochemical impedance spectroscopy(EIS)test,with the impedance modulus at 10^(-2) Hz stabilizing at 5×10^(5)Ω·cm^(2).After soaking,the surface morphology of the in situ drug-loaded PEO coating exhibited more cracks and defects,whereas the PEO-LDH coating maintained a relatively dense morphology.Among the tested samples,the PEO-LDH coating showed the best performance in terms of corrosion resistance,cell proliferation and differentiation capabilities,and antibacterial efficacy(>99%).Its strong compatibility with the porous structure of 3D-printed Mg alloy highlights the potential of this coating system for biomedical applications.The design strategy proposed in this study offers valuable insights for future development of drug-loaded coatings for 3D-printed porous materials.
基金supported by the National Key Research and Development Project Intergovernmental International Science and Technology Innovation Cooperation(2022YFE0109400)National Key Research and Development Program of China(2023YFB2405800)Leading Edge Technology of Jiangsu Province(BK20232022,BK20220009)。
文摘Solid-solid interface contact and slow ion transport restrict solid-state polymer electrolytes practical application.The differences in interface structure design significantly influence the interfacial Li^(+)transport and diffusion as well as the Li atom nucleation,resulting in substantial variations in the macroscopic performance of polymer electrolytes-based solid-state Li metal batteries.Here,ceramic-polymer composite electrolytes(CPCEs)composed of polyvinylidene fluoride-hexafluoropropylene(PVDF-HFP)polymer and Li_(6.75)La_(3)Zr_(1.75)Ta_(0.25)O_(12)(LLZTO)filler has been chosen as the demo to demonstrate that the interfacial electrochemistry between CPCEs and Li anode is not only affected by the physical interface contact but also associated with the internal/interfacial Li^(+)transport mechanism.This work shows that“point to point”Li^(+)diffusion,slow uneven interfacial Li^(+)transport in CPCEs with poor ionic conductivity and rough surface lead to uneven Li atom nucleation,leading to Li dendrites growth.While,the CPCEs with high ionic conductivity and smooth surface facilitate uniform and rapid ion transport,promoting uniform Li nucleation and transverse diffusion.This work highlights the importance of the interface structure design of polymer electrolytes for Li metal interface stability in polymer electrolytes-based quasi-solid-state batteries and provides valuable insights into the interfacial electrochemistry of solidstate batteries.
基金the ORSP of Pandit Deendayal Energy University and DST SERB(IPA/2021/96)for the financial supportthe Deanship of Research and Graduate Studies at King Khalid University for funding this work through the Large Research Project under grant number RGP 2/345/45。
文摘We introduce a dual distribution of relaxation(DRT)based approach for analyzing electrochemical impedance spectroscopy(EIS)data in perovskite solar cells(PSCs),combining regression and classification with Bayesian model selection and Havriliak-Negami(HN)modeling to resolve spectra into discrete,Lorentzian-like peaks.This time-domain decomposition offers a powerful alternative for identifying underlying physical processes,such as charge transfer,trap-assisted recombination,and ionic migration by directly extracting characteristic relaxation times(τ).In contrast to traditional equivalent circuit fitting or conventional DRT methods,which often yield broad and overlapping Gaussian-like peaks,our method enables sharper resolution of individual electrochemical signatures.Furthermore,we validated the framework using simulated EIS spectra for two distinct system types,determining the optimal number of peaks(Q)through statistical model selection.Applied to experimental PSC data under varying bias conditions,the approach helps to identify the voltage-dependent relaxation processes,including fast charge transfer(τ~10^(-6)s),intermediate trap-mediated recombination(τ~10^(-2)s),and slow ionic motion(τ~1 s).Lower-Q models fail to capture low-frequency features such as polarization and charge accumulation,while optimal Q yields accurate,physically meaningful representations of device behavior.This data-driven methodology highlights time-domain DRT as a rigorous and insightful tool for dissecting the complex kinetics that govern PSC performance.
