Intercalation of rare-earth(RE)into Pt offers an option to optimize the electronic structure of Pt-based catalysts by interaction effect,in which the synergistic catalytic sites are of great significance,yet the under...Intercalation of rare-earth(RE)into Pt offers an option to optimize the electronic structure of Pt-based catalysts by interaction effect,in which the synergistic catalytic sites are of great significance,yet the underpinning mechanism remains elusive.Herein,the introduction of silanol nests enables the alloy formation on the SiO_(2)surface.The amination modification is disclosed to induce the electron transfer from RE to Pt and weaken the adsorption of CO on electron-rich Pt species.In situ/operando spectroscopic analyses in conjunction with density functional theory calculations demonstrate the electronic couple of Pt atoms and adjacent Ce atoms concurrently achieves the enhancement of CO oxidation and suppression of H_(2)oxidation.Additionally,CO_(2)is readily desorbed from the Pt_(5)Ce(111)surface to enhance intrinsic activity and longevity.These findings provide an atomic-level insight into the synergistic catalytic sites on regulating the electronic state of the Pt-RE alloy catalysts toward highly selective oxidation reactions.展开更多
The rapid advancement of electronic devices has resulted in increasingly demanding performance requirements for highvoltage LiCoO_(2)(LCO)cathodes.However,LCO exhibits significant irreversible phase transitions and de...The rapid advancement of electronic devices has resulted in increasingly demanding performance requirements for highvoltage LiCoO_(2)(LCO)cathodes.However,LCO exhibits significant irreversible phase transitions and detrimental side reactions under high voltages.Herein,Mg/Zr co-doped and Li_(3)PO_(4)-coated LiCoO_(2)(denoted as MZP-LCO)was synthesized through an element self-diffusion reaction at a high temperature.Mg^(2+)and Zr^(4+)can partially replace Li+in the LCO structure,creating a homogeneous concentration distribution with a 60 nm thickness from the surface to the interior.Mg^(2+)serves as a stabilizing"pillar"to suppress Co-O layer sliding during deep delithiation,enhancing the structural integrity of LCO,while Zr^(4+)expands the Li+deintercalation channels,thereby increasing the capacity.Furthermore,a Li_(3)PO_(4)nano-coating layer forms in situ on the surface of the LCO,improving Li+transport efficiency and successfully inhibiting harmful side reactions at the electrode surface.The half-cell of MZP-LCO exhibits a capacity of 154.7 mAh·g^(-1)after 200 cycles at 0.5C within 3.0-4.6 V,and demonstrates superior rate capability,maintaining a capacity of 156.1 mAh·g^(-1)at 10C.The exceptional electrochemical performance can be attributed to the synergistic effects of the uniform Mg/Zr doping within the LCO and the Li_(3)PO_(4)coating nanolayer on the surface.These findings offer valuable insights for resolving the issues related to LCO cathode performance degradation at high voltages.展开更多
This study reports several modification strategies to optimize and enhance the performance of twodimensional(2D) metal organic frameworks(MOFs)-derived catalysts in peroxydisulfate(PDS) activation.The raw 2D Ni-MOF an...This study reports several modification strategies to optimize and enhance the performance of twodimensional(2D) metal organic frameworks(MOFs)-derived catalysts in peroxydisulfate(PDS) activation.The raw 2D Ni-MOF and 2D Ni-Fe-MOF without modification show poor catalytic activities for PDS activation and high metal ion leaching. The carbonization of 2D MOF can increase the activity of the catalyst but cannot solve the metal leaching problem. The further acid treatment of carbonization products can further improve the catalytic activity and decrease the metal ion leaching. The in-situ growth of2D MOF on graphene oxide(GO) support with subsequent carbonization and acid treatment offers the best performance in PDS activation for organic pollutant removal with low metal ion leaching. Compared with other PDS systems, the Ni-Fe-C-acid/GO system displays much lower catalyst and PDS dosages for p-chloroaniline degradation. This study presents new insights in the modification strategies of 2D MOFbased catalysts in PDS activation.展开更多
The introduction of neurotrophic factors into injured peripheral nerve sites is beneficial to peripheral nerve regeneration.However,neurotrophic facto rs are rapidly degraded in vivo and obstruct axonal regeneration w...The introduction of neurotrophic factors into injured peripheral nerve sites is beneficial to peripheral nerve regeneration.However,neurotrophic facto rs are rapidly degraded in vivo and obstruct axonal regeneration when used at a supraphysiological dose,which limits their clinical benefits.Bioactive mimetic peptides have been developed to be used in place of neurotrophic factors because they have a similar mode of action to the original growth fa ctors and can activate the equivalent receptors but have simplified sequences and structures.In this study,we created polydopamine-modified chitin conduits loaded with brain-derived neurotrophic factor mimetic peptides and vascular endothelial growth fa ctor mimetic peptides(Chi/PDA-Ps).We found that the Chi/PDA-Ps conduits were less cytotoxic in vitro than chitin conduits alone and provided sustained release of functional peptides.In this study,we evaluated the biocompatibility of the Chi/P DA-Ps conduits.Brain-derived neurotrophic factor mimetic peptide and vascular endothelial growth fa ctor mimetic peptide synergistically promoted prolife ration of Schwann cells and secretion of neurotrophic factors by Schwann cells and attachment and migration of endothelial cells in vitro.The Chi/P DA-Ps conduits were used to bridge a 2 mm gap between the nerve stumps in rat models of sciatic nerve injury.We found that the application of Chi/PDA-Ps conduits could improve the motor function of rats and reduce gastrocnemius atrophy.The electrophysiological results and the microstructure of regenerative nerves showed that the nerve conduction function and re myelination was further resto red.These findings suggest that the Chi/PDA-Ps conduits have great potential in peripheral nerve injury repair.展开更多
This study explores a novel approach to biochar modification aimed at increasing persistent free radical(PFR)formation on biochar surfaces,thereby enhancing aniline removal via peroxymonosulfate(PMS)activation.By adju...This study explores a novel approach to biochar modification aimed at increasing persistent free radical(PFR)formation on biochar surfaces,thereby enhancing aniline removal via peroxymonosulfate(PMS)activation.By adjusting pyrolysis temperatures and doping ratios,optimal conditions were established.Spearman’s analysis highlighted the importance of C=C bonds,the ID/IG ratio,and pyridinic N in generating PFRs.The modified biochar derived at 500℃(MB500),in conjunction with the PMS system demonstrated impressive efficiency,achieving 92%aniline removal within 30 min.Detailed adsorption tests and active species detection indicated that aniline degradation occurred through both direct oxidation by PFRs and indirect oxidation by reactive species,particularly superoxide radicals(O_(₂)^(⋅⁻)).Furthermore,the synergistic effects of heteroatom nitrogen and Na_(2)CO_(3)modifications significantly impacted PFR formation and stability.These findings provide valuable insights into the mechanisms of PFR-mediated catalytic oxidation,highlighting the key roles of pyridinic rings,with or without oxygenated groups,in enhancing catalytic performance of biochar.This research advances the understanding of biochar surface chemistry and presents an effective strategy for developing high-performance biochar-based catalysts for environmental remediation,addressing the limitations of unmodified biochar through targeted surface modifications.展开更多
Creating economical and effective catalysts for the oxygen evolution reaction(OER)is essential for enhancing the efficiency of electrochemical water splitting.In this study,we designed a multicomponent heterogeneous i...Creating economical and effective catalysts for the oxygen evolution reaction(OER)is essential for enhancing the efficiency of electrochemical water splitting.In this study,we designed a multicomponent heterogeneous interfacial catalyst,Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH,using a simple two-step method.In situ Raman and X-ray photoelectron spectroscopy(XPS)measurements revealed the dynamic phase change occurring during the OER process.The FeOOH layer on Ni(OH)_(2)/NiCo(OH)_(6)altered the electronic structure,facilitating the emergence of the active NiOOH phase and markedly improving OER kinetics.Significantly,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1 catalyst demonstrated a current density of 10 mA·cm^(-2)at an overpotential of merely 208 mV,accompanied by a Tafel slope of 37.72 mV·dec-1,exhibiting exceptional stability over a duration of 100 h at 10 mA·cm^(-2).Furthermore,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1(+)lIPt/C(-)electrolyzer cell showcased a remarkably low driving voltage of 1.52 V to achieve 10 mA·cm^(-2),while also displaying impressive durability under alkaline conditions for over100 h.This work enhances our understanding of the interfacial structure-activity relationship in composite catalysts,aiding the design of efficient catalysts with rapid kinetics.展开更多
基金financially supported by the National Natural Science Foundation of China(22468034)the Natural Science Foundation of Inner Mongolia(2021MS02008 and 2022MS02011)the Key Research and Development Project of Ordos(YF20240062)。
文摘Intercalation of rare-earth(RE)into Pt offers an option to optimize the electronic structure of Pt-based catalysts by interaction effect,in which the synergistic catalytic sites are of great significance,yet the underpinning mechanism remains elusive.Herein,the introduction of silanol nests enables the alloy formation on the SiO_(2)surface.The amination modification is disclosed to induce the electron transfer from RE to Pt and weaken the adsorption of CO on electron-rich Pt species.In situ/operando spectroscopic analyses in conjunction with density functional theory calculations demonstrate the electronic couple of Pt atoms and adjacent Ce atoms concurrently achieves the enhancement of CO oxidation and suppression of H_(2)oxidation.Additionally,CO_(2)is readily desorbed from the Pt_(5)Ce(111)surface to enhance intrinsic activity and longevity.These findings provide an atomic-level insight into the synergistic catalytic sites on regulating the electronic state of the Pt-RE alloy catalysts toward highly selective oxidation reactions.
基金supported by the National Natural Science Foundation of China(No.22062008)the program of Qingjiang Excellent Young Talents(No.JXUSTQJBJ2020008)supported by Jiangxi University of Science and Technology。
文摘The rapid advancement of electronic devices has resulted in increasingly demanding performance requirements for highvoltage LiCoO_(2)(LCO)cathodes.However,LCO exhibits significant irreversible phase transitions and detrimental side reactions under high voltages.Herein,Mg/Zr co-doped and Li_(3)PO_(4)-coated LiCoO_(2)(denoted as MZP-LCO)was synthesized through an element self-diffusion reaction at a high temperature.Mg^(2+)and Zr^(4+)can partially replace Li+in the LCO structure,creating a homogeneous concentration distribution with a 60 nm thickness from the surface to the interior.Mg^(2+)serves as a stabilizing"pillar"to suppress Co-O layer sliding during deep delithiation,enhancing the structural integrity of LCO,while Zr^(4+)expands the Li+deintercalation channels,thereby increasing the capacity.Furthermore,a Li_(3)PO_(4)nano-coating layer forms in situ on the surface of the LCO,improving Li+transport efficiency and successfully inhibiting harmful side reactions at the electrode surface.The half-cell of MZP-LCO exhibits a capacity of 154.7 mAh·g^(-1)after 200 cycles at 0.5C within 3.0-4.6 V,and demonstrates superior rate capability,maintaining a capacity of 156.1 mAh·g^(-1)at 10C.The exceptional electrochemical performance can be attributed to the synergistic effects of the uniform Mg/Zr doping within the LCO and the Li_(3)PO_(4)coating nanolayer on the surface.These findings offer valuable insights for resolving the issues related to LCO cathode performance degradation at high voltages.
基金supported by the National Key R&D Program of China (No. 2019YFC1905400)。
文摘This study reports several modification strategies to optimize and enhance the performance of twodimensional(2D) metal organic frameworks(MOFs)-derived catalysts in peroxydisulfate(PDS) activation.The raw 2D Ni-MOF and 2D Ni-Fe-MOF without modification show poor catalytic activities for PDS activation and high metal ion leaching. The carbonization of 2D MOF can increase the activity of the catalyst but cannot solve the metal leaching problem. The further acid treatment of carbonization products can further improve the catalytic activity and decrease the metal ion leaching. The in-situ growth of2D MOF on graphene oxide(GO) support with subsequent carbonization and acid treatment offers the best performance in PDS activation for organic pollutant removal with low metal ion leaching. Compared with other PDS systems, the Ni-Fe-C-acid/GO system displays much lower catalyst and PDS dosages for p-chloroaniline degradation. This study presents new insights in the modification strategies of 2D MOFbased catalysts in PDS activation.
基金the National Natural Science Foundation of China,Nos.31771322,31571235the Natural Science Foundation of Beijing,No.7212121+3 种基金Beijing Science Technology New Star Cross Subject of China,No.2018019Shenzhen Science and Technology Plan Project of China,No.JCYJ 20190806162205278the Key Laboratory of Trauma and Neural Regeneration(Peking University),Ministry of Educationa grant from National Center for Trauma Medicine,No.BMU2020XY005-01(all to PXZ)。
文摘The introduction of neurotrophic factors into injured peripheral nerve sites is beneficial to peripheral nerve regeneration.However,neurotrophic facto rs are rapidly degraded in vivo and obstruct axonal regeneration when used at a supraphysiological dose,which limits their clinical benefits.Bioactive mimetic peptides have been developed to be used in place of neurotrophic factors because they have a similar mode of action to the original growth fa ctors and can activate the equivalent receptors but have simplified sequences and structures.In this study,we created polydopamine-modified chitin conduits loaded with brain-derived neurotrophic factor mimetic peptides and vascular endothelial growth fa ctor mimetic peptides(Chi/PDA-Ps).We found that the Chi/PDA-Ps conduits were less cytotoxic in vitro than chitin conduits alone and provided sustained release of functional peptides.In this study,we evaluated the biocompatibility of the Chi/P DA-Ps conduits.Brain-derived neurotrophic factor mimetic peptide and vascular endothelial growth fa ctor mimetic peptide synergistically promoted prolife ration of Schwann cells and secretion of neurotrophic factors by Schwann cells and attachment and migration of endothelial cells in vitro.The Chi/P DA-Ps conduits were used to bridge a 2 mm gap between the nerve stumps in rat models of sciatic nerve injury.We found that the application of Chi/PDA-Ps conduits could improve the motor function of rats and reduce gastrocnemius atrophy.The electrophysiological results and the microstructure of regenerative nerves showed that the nerve conduction function and re myelination was further resto red.These findings suggest that the Chi/PDA-Ps conduits have great potential in peripheral nerve injury repair.
基金fouded by the General Program of Stable Support Plan for Universities in Shenzhen City(Grant No.GXWD20231130102759003)the National Natural Science Foundation of China(Grant No.42177044).
文摘This study explores a novel approach to biochar modification aimed at increasing persistent free radical(PFR)formation on biochar surfaces,thereby enhancing aniline removal via peroxymonosulfate(PMS)activation.By adjusting pyrolysis temperatures and doping ratios,optimal conditions were established.Spearman’s analysis highlighted the importance of C=C bonds,the ID/IG ratio,and pyridinic N in generating PFRs.The modified biochar derived at 500℃(MB500),in conjunction with the PMS system demonstrated impressive efficiency,achieving 92%aniline removal within 30 min.Detailed adsorption tests and active species detection indicated that aniline degradation occurred through both direct oxidation by PFRs and indirect oxidation by reactive species,particularly superoxide radicals(O_(₂)^(⋅⁻)).Furthermore,the synergistic effects of heteroatom nitrogen and Na_(2)CO_(3)modifications significantly impacted PFR formation and stability.These findings provide valuable insights into the mechanisms of PFR-mediated catalytic oxidation,highlighting the key roles of pyridinic rings,with or without oxygenated groups,in enhancing catalytic performance of biochar.This research advances the understanding of biochar surface chemistry and presents an effective strategy for developing high-performance biochar-based catalysts for environmental remediation,addressing the limitations of unmodified biochar through targeted surface modifications.
基金financially supported by the National Natural Science Foundation of China(Nos.52306142,52272202 and W2421027)Yunnan Major Scientific and Technological Projects(No.202202AG050017-02)+2 种基金Yunnan Fundamental Research Projects(No.202101BE070001-017)the Science and Technology Innovation and Entrepreneurship Fund of China Coal Technology&Engineering Group Co.,Ltd.(Nos.2022-MS002 and 2023-TD-MS007)Bintuan Science and Technology Program(No.2022DB009)
文摘Creating economical and effective catalysts for the oxygen evolution reaction(OER)is essential for enhancing the efficiency of electrochemical water splitting.In this study,we designed a multicomponent heterogeneous interfacial catalyst,Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH,using a simple two-step method.In situ Raman and X-ray photoelectron spectroscopy(XPS)measurements revealed the dynamic phase change occurring during the OER process.The FeOOH layer on Ni(OH)_(2)/NiCo(OH)_(6)altered the electronic structure,facilitating the emergence of the active NiOOH phase and markedly improving OER kinetics.Significantly,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1 catalyst demonstrated a current density of 10 mA·cm^(-2)at an overpotential of merely 208 mV,accompanied by a Tafel slope of 37.72 mV·dec-1,exhibiting exceptional stability over a duration of 100 h at 10 mA·cm^(-2).Furthermore,the Ni(OH)_(2)/NiCo(OH)_(6)@FeOOH 2:1(+)lIPt/C(-)electrolyzer cell showcased a remarkably low driving voltage of 1.52 V to achieve 10 mA·cm^(-2),while also displaying impressive durability under alkaline conditions for over100 h.This work enhances our understanding of the interfacial structure-activity relationship in composite catalysts,aiding the design of efficient catalysts with rapid kinetics.
