Hollow structure microspheres with composite polymeric-Laponite shells were prepared by electrostatic self-assembly of Laponite on the polymeric hollow microspheres in this work.The multilayer hydrophilic core/hydroph...Hollow structure microspheres with composite polymeric-Laponite shells were prepared by electrostatic self-assembly of Laponite on the polymeric hollow microspheres in this work.The multilayer hydrophilic core/hydrophobic shell polymer latex particles containing carboxyl groups inside were first synthesized via seeded emulsion polymerization,followed by alkali treatment,generating polymeric hollow microspheres.Then,polyethyleneimine（PEI） and Laponite were alternately electrostatic adsorbed on the prepared polymeric hollow microspheres to form polymeric-Laponite composite hollow microspheres.It was indicated that the morphology of alkali-treated microspheres could be tuned through simply altering the dosage of alkali used in the post-treatment process.Along with the increasing of the coating layers,the zeta potential of microspheres absorbed PEI or Laponite approximately tended to be constant respectively,and the thickness of Laponite layer around the hollow microspheres increased clearly,getting more uniform and homogenous.Furthermore,the corresponding polymeric-Laponite hollow microspheres showed high pressure resistance ability compared to the polymeric hollow microspheres.展开更多
Drug-eluting magnesium(Mg)alloy stents have a slower degradation rate and lower restenosis rate compared with uncoated stents,demonstrating good clinical efficacy.However,the release of anti-hyperplasia drugs from coa...Drug-eluting magnesium(Mg)alloy stents have a slower degradation rate and lower restenosis rate compared with uncoated stents,demonstrating good clinical efficacy.However,the release of anti-hyperplasia drugs from coatings delays endothelial tissue repair,thus leading to late stent thrombosis.To address these issues,a dual self-healed coating with various biological properties was fabricated on magnesium fluoride/polydopamine(MgF_(2)/PDA)-treated Mg alloys by spraying-assisted layer-by-layer(LBL)self-assembly of chitosan(CS),gallic acid(GA),and 3-aminobenzeneboronic acid-modified hyaluronic acid(HA-ABBA).The LBL coating,approximately 1.50μm thick,exhibited a uniform morphology with good adhesion strength(~1065 mN).The annual corrosion rate(Pi)of LBL samples was~1400 times slower than that of the Mg substrate,due to the physical barrier function provided by MgF_(2)/PDA layers and the dual self-healed ability of LBL layers.The rapid self-healing ability(with a healing period of~4 h under dynamic/static conditions)resulted from the synergistic interplay between the recombination of diverse chemical bonds within the LBL coating and the coordination of LBL-released GA with Mg2+,as corroborated by computer simulations.Compared with the drug-eluting coatings,the LBL sample demonstrated substantial advantages in anti-oxidation,anti-denaturation of fibrinogen,anti-platelet adhesion,anti-inflammation,anti-hyperplasia,and promoted-endothelialization.These benefits effectively address the limitations associated with drug-eluting coatings.展开更多
Zinc Cr(Ⅲ)passivation layer(Zn-PL)could effectively protect NdFeB materials from corrosion.However,long-term exposure of Zn-PL to ambient atmosphere would reduce its wettability spontaneously,which hinders or deterio...Zinc Cr(Ⅲ)passivation layer(Zn-PL)could effectively protect NdFeB materials from corrosion.However,long-term exposure of Zn-PL to ambient atmosphere would reduce its wettability spontaneously,which hinders or deteriorates the adhesion of post-deposited materials.To solve this issue,a multilayer developed by layer-by-layer assembly approach was designed,and alumina sol and silica sol were prepared.A poly acrylic acid(PAA)layer was firstly deposited on Zn-PL to remove the preabsorbed organic carbon and form poly(zinc acrylate).Then,Al_(2)O_(3)and SiO_(2)sol-gel layers were sequentially assembled on PAA-coated Zn-PL.As a result,the hydrophobic Zn-PL turns into super-hydrophilic by coating organic-inorganic multilayers,which is attributed to the surface enrichment of hydrophilic hydroxyl groups and increases surface roughness.Furthermore,the super-hydrophilic surface displays excellent adhesion property without the negative effect on its other properties,which highlights a good prospect for a wide application of NdFeB or other potential materials.展开更多
We report layer-by-layer （LbL） assembly of TiO2 and H4SiW12O40 （SiW12） multilayer film on silicon wafers and glass slides for photocatalytic degradation of methyl orange （MO）. The photocatalytic efficiency of th...We report layer-by-layer （LbL） assembly of TiO2 and H4SiW12O40 （SiW12） multilayer film on silicon wafers and glass slides for photocatalytic degradation of methyl orange （MO）. The photocatalytic efficiency of the obtained multilayer film increases along with the decrease of pH and salt concentration of the incubation solution. The results show that MO can be almost re- moved in pH 2.0 solution without salt addition in the first 60 min incubation when MO concentration is lower than 15 mg/L. Different salts show an apparent inhibitory effect on photocatalytic degradation of MO with the order of ZnC12〉KCI〉 NaC1〉LiCI. The TiO2/SiW12 multilayer film maintains photocatalytic activity even after five degradation cycles. The reaction of MO photodegradation accords with an apparent first-order dynamics.展开更多
Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in ef...Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient electrolyzers.Here,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)fashion.In particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 h.Furthermore,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V battery.This study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.展开更多
基金supported by Heilongjiang Provincial Natural Science Foundation for Youth, China (No. QC2014C052)Fund of Key Laboratory of Advanced materials of Ministry of Education (No. 2016AML06)the training project for innovation and entrepreneurship of the Harbin University of Science and Technology, China (2016)
文摘Hollow structure microspheres with composite polymeric-Laponite shells were prepared by electrostatic self-assembly of Laponite on the polymeric hollow microspheres in this work.The multilayer hydrophilic core/hydrophobic shell polymer latex particles containing carboxyl groups inside were first synthesized via seeded emulsion polymerization,followed by alkali treatment,generating polymeric hollow microspheres.Then,polyethyleneimine（PEI） and Laponite were alternately electrostatic adsorbed on the prepared polymeric hollow microspheres to form polymeric-Laponite composite hollow microspheres.It was indicated that the morphology of alkali-treated microspheres could be tuned through simply altering the dosage of alkali used in the post-treatment process.Along with the increasing of the coating layers,the zeta potential of microspheres absorbed PEI or Laponite approximately tended to be constant respectively,and the thickness of Laponite layer around the hollow microspheres increased clearly,getting more uniform and homogenous.Furthermore,the corresponding polymeric-Laponite hollow microspheres showed high pressure resistance ability compared to the polymeric hollow microspheres.
基金supported by the National Key Research and Development Program of China(No.2021YFC2400703)the Key Scientific and Technological Research Projects in Henan Province(Nos.232102311155 and 232102230106)Zhengzhou University Major Project Cultivation Special Project(No.125-32214076).
文摘Drug-eluting magnesium(Mg)alloy stents have a slower degradation rate and lower restenosis rate compared with uncoated stents,demonstrating good clinical efficacy.However,the release of anti-hyperplasia drugs from coatings delays endothelial tissue repair,thus leading to late stent thrombosis.To address these issues,a dual self-healed coating with various biological properties was fabricated on magnesium fluoride/polydopamine(MgF_(2)/PDA)-treated Mg alloys by spraying-assisted layer-by-layer(LBL)self-assembly of chitosan(CS),gallic acid(GA),and 3-aminobenzeneboronic acid-modified hyaluronic acid(HA-ABBA).The LBL coating,approximately 1.50μm thick,exhibited a uniform morphology with good adhesion strength(~1065 mN).The annual corrosion rate(Pi)of LBL samples was~1400 times slower than that of the Mg substrate,due to the physical barrier function provided by MgF_(2)/PDA layers and the dual self-healed ability of LBL layers.The rapid self-healing ability(with a healing period of~4 h under dynamic/static conditions)resulted from the synergistic interplay between the recombination of diverse chemical bonds within the LBL coating and the coordination of LBL-released GA with Mg2+,as corroborated by computer simulations.Compared with the drug-eluting coatings,the LBL sample demonstrated substantial advantages in anti-oxidation,anti-denaturation of fibrinogen,anti-platelet adhesion,anti-inflammation,anti-hyperplasia,and promoted-endothelialization.These benefits effectively address the limitations associated with drug-eluting coatings.
基金financially supported by the National Natural Science Foundation of China(No.51371020)。
文摘Zinc Cr(Ⅲ)passivation layer(Zn-PL)could effectively protect NdFeB materials from corrosion.However,long-term exposure of Zn-PL to ambient atmosphere would reduce its wettability spontaneously,which hinders or deteriorates the adhesion of post-deposited materials.To solve this issue,a multilayer developed by layer-by-layer assembly approach was designed,and alumina sol and silica sol were prepared.A poly acrylic acid(PAA)layer was firstly deposited on Zn-PL to remove the preabsorbed organic carbon and form poly(zinc acrylate).Then,Al_(2)O_(3)and SiO_(2)sol-gel layers were sequentially assembled on PAA-coated Zn-PL.As a result,the hydrophobic Zn-PL turns into super-hydrophilic by coating organic-inorganic multilayers,which is attributed to the surface enrichment of hydrophilic hydroxyl groups and increases surface roughness.Furthermore,the super-hydrophilic surface displays excellent adhesion property without the negative effect on its other properties,which highlights a good prospect for a wide application of NdFeB or other potential materials.
基金financially supported by the National Natural Science Foundation of China (21033005)the National Basic Research Program of China (973 Program, 2009CB930103)Natural Science Foundation of Shandong Province (2009ZRB01876)
文摘We report layer-by-layer （LbL） assembly of TiO2 and H4SiW12O40 （SiW12） multilayer film on silicon wafers and glass slides for photocatalytic degradation of methyl orange （MO）. The photocatalytic efficiency of the obtained multilayer film increases along with the decrease of pH and salt concentration of the incubation solution. The results show that MO can be almost re- moved in pH 2.0 solution without salt addition in the first 60 min incubation when MO concentration is lower than 15 mg/L. Different salts show an apparent inhibitory effect on photocatalytic degradation of MO with the order of ZnC12〉KCI〉 NaC1〉LiCI. The TiO2/SiW12 multilayer film maintains photocatalytic activity even after five degradation cycles. The reaction of MO photodegradation accords with an apparent first-order dynamics.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.52273076,52111540268,and 12004195)the 111 Project(No.B18030)in China+1 种基金The authors also acknowledge the financial support by Haihe Laboratory of Sustainable Chemical Transformations(No.YYJC202101)Open Research Fund Program of the State Key Laboratory of Low Dimensional Quantum Physics(No.KF202113).
文摘Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient electrolyzers.Here,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)fashion.In particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 h.Furthermore,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V battery.This study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.
