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Bioinspired surface functionalization of biodegradable mesoporous silica nanoparticles for enhanced lubrication and drug release

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Friction 2023年第7期11卷 1194-1211页

作者： Xiaowei MAO Kexin CHEN Yanlong ZHAO Chunrong Xiong Jing LUO Yuguang WANG Bo WANG Hongyu ZHANG School of Chemical Engineering and Technology Hainan UniversityHaikou 570228China State Key Laboratory of Tribology Department of Mechanical EngineeringTsinghua UniversityBeijing 100084China Peking University School of Nursing&National Engineering Laboratory for Digital and Material Technology of Stomatology Beijing 100191China Beijing Research Institute of Automation for Machinery Industry Co. Ltd.Beijing 100120China Center of Digital Dentistry Peking University School and Hospital of Stomatology&NHC Research Center of Engineering and Technology for Computerized DentistryBeijing 100081China College of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266590China

Osteoarthritis is associated with the significantly increased friction of the joint,which results in progressive and irreversible damage to the articular cartilage.A synergistic therapy integrating lubrication enhancement and drug delivery is recently proposed for the treatment of early-stage osteoarthritis.In the present study,bioinspired by the self-adhesion performance of mussels and super-lubrication property of articular cartilages,a biomimetic self-adhesive dopamine methacrylamide-poly(2-methacryloyloxyethyl phosphorylcholine)(DMA-MPC)copolymer was designed and synthesized via free radical polymerization.The copolymer was successfully modified onto the surface of biodegradable mesoporous silica nanoparticles(bMSNs)by the dip-coating method to prepare the dual-functional nanoparticles(bMSNs@DMA-MPC),which were evaluated using a series of surface characterizations including the transmission electron microscope(TEM),Fourier transform infrared(FTIR)spectrum,thermogravimetric analysis(TGA),X-ray photoelectron spectroscopy(XPS),etc.The tribological test and in vitro drug release test demonstrated that the developed nanoparticles were endowed with improved lubrication performance and achieved the sustained release of an anti-inflammatory drug,i.e.,diclofenac sodium(DS).In addition,the in vitro biodegradation test showed that the nanoparticles were almost completely biodegraded within 10 d.Furthermore,the dual-functional nanoparticles were biocompatible and effectively reduced the expression levels of two inflammation factors such as interleukin-1β(IL-1β)and interleukin-6(IL-6).In summary,the surface functionalized nanoparticles with improved lubrication and local drug release can be applied as a potential intra-articularly injected biolubricant for synergistic treatment of early-stage osteoarthritis.

关键词： surface functionalization phosphorylcholine coating mesoporous silica nanoparticles hydration lubrication osteoarthritis

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surface functionalization OF POLYSTYRENE TO BIND WITH FMRF PEPTIDES FOR NOVEL BIOCOMPATIBILITY

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Chinese Journal of Polymer Science 2010年第6期28卷 895-902页

作者： Yong Chen Hong-sheng Lu Peng Wang Department of Applied Chemistry School of Chemical & Environmental Engineering Shandong University of Science and Technology Qingdao 266510 China Department of Environmental Science and Technology School of Chemical & Environmental Engineering Shandong University of Science and Technology Qingdao 266510 China

A generic method was described to change surface biocompatibihty by introducing reactive functional groups onto surfaces of polymeric substrates and covalently binding them with biomolecules.A block copolymer with protected carboxylic acid functionality,poly（styrene-b-tert-butyl acrylate）（PS-PtBA）,was spin coated from solutions in toluene on a bioinert polystyrene（PS） substrate to form a bilayer structure：a surface layer of the poly（tert-butyl acrylate）（PtBA） blocks that order at the air-polymer interface and a bottom layer of the PS blocks that entangle with the PS substrate.The thickness of the PtBA layer and the area density of tert-butyl ester groups of PtBA increased linearly with the concentration of the spin coating solution until a 2 nm saturated monolayer coverage of PtBA was achieved at the concentration of 0.4%W/W.The protected carboxylic acid groups were generated by exposing the tert-butyl ester groups of PtBA to trifluoroacetic acid （TFA） for bioconjugation with FMRF peptides via amide bonds.The yield of the bioconjugation reaction for the saturated surface was calculated to be 37.1%based on X-ray photoelectron spectroscopy（XPS） measurements.The success of each functionalization step was demonstrated and characterized by XPS and contact angle measurements.This polymer functionalization/modification concept can be virtually applied to any polymeric substrate by choosing appropriate functional block copolymers and biomolecules to attain novel biocompatibility.

关键词： surface functionalization Biocompatibility Bioconjugation reaction

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surface functionalization of SPR chip for specific molecular interaction analysis under flow condition

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Journal of Innovative Optical Health Sciences 2017年第2期10卷 30-39页

作者： Tao Ma Xiaoxia Chen Qing Peng Pengfei Zhang Yonghong He Department of Ophthalmology Shanxi Eye Hospital Taiyuan 030002P.R.China Department of Ophthalmology Xin Hua hospital affiliated to Shanghai Jiao Tong University School of Medicine Shanghai 200092 P.R.China Department of Ophthalmology MinHang Hospital Affiliated to Fudan University Shanghai 201199P.R.China Shenzhen Key Laboratory for Minimal Invasive Medical Technologies Institute of optical imaging and sensing Graduate School at Shenzhen Tsinghua University Shenzhen 518055P.R.China Department of Physics Tsinghua University Beijing 100084P.R.China

surface functionalization of sensor chip for probe immobilization is crucial for the biosensing applications of surface plasmon resonance(SPR)sensors.In this paper,we report a method circulating the dopamine aqueous solution to coat polydopamine film on sensing surface for surface functionalization of SPR chip.The polydopamine film with available thickness can be easily prepared by controlling the circulation time and the biorecognition elements can be immobilized on the polydopamine film for specific molecular interaction analysis.These opera-tions are all performed under flow condition in the fuidic system,and have the advantages of easy implementation,less time consuming,and low cost,because the reagents and devices used in the operations are routinely applied in most laboratories.In this study,the specific absorption between the protein A probe immobilized on the sensing surface and human immunoglobulin G in the buffer is monitored based on this surface functionalization strategy to demonstrated its feasibility for SPR biosensing applications.

关键词： surface plasmon resonance surface functionalization dopamine molecular interac-tion analysis

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surface functionalization of PEO Nanofibers Using a TiO_(2) Suspension as Sheath Fluid in a Modified Coaxial Electrospinning Process

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Chemical Research in Chinese Universities 2021年第3期37卷 571-577页

作者： ZHENG Gaofeng PENG Hao JIANG Jiaxin KANG Guoyi LIU Juan ZHENG Jianyi LIU Yifang Department of Instrumental and Electrical Engineering Xiamen UniversityXiamen361102P.R.China Fujian Innovation Center of Additive Manufacturing Fuzhou350118P.R.China

Convenient and integration fabrication process is a key issue for the application of functional nanofibers.A surface functionalization method was developed based on coaxial electrospinning to produce ultraviolet(UV)protection nanofibers.The titanium dioxide(TiO_(2))nanoparticles suspension was delivered through the shell channel of the coaxial spinneret,by which the aggregation of TiO_(2) nanoparticles was overcome and the distribution uniformity on the surface of polyethylene oxide(PEO)nanofiber was obtained.With the content of TiO_(2) increasing from 0 to 3%(mass fraction),the average diameter of nanofibers increased from(380±30)nm to(480±100)nm.The surface functionalization can be realized during the electrospinning process to gain PEO/TiO_(2) composite nanofibers directly.The uniform distribution of TiO_(2) nanoparticles on the surface of nanofibers enhanced the UV absorption and resistance performance.The maximum UV protection factor(UPF)value of composite nanofibers reaches 2751.This work presented a novel surface-functionalized way for the preparation of composite nanofiber,which has great application potential in the field of micro/nano system integration fabrication.

关键词： Coaxial electrospinning surface functionalization TiO_(2)nanoparticle Composite nanofiber UV protection

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A facile strategy for tuning the density of surface-grafted biomolecules for melt extrusion-based additive manufacturing applications

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Bio-Design and Manufacturing 2024年第3期7卷 277-291页

作者： I.A.O.Beeren G.Dos Santos P.J.Dijkstra C.Mota J.Bauer H.Ferreira Rui L.Reis N.Neves S.Camarero-Espinosa M.B.Baker L.Moroni Department of Complex Tissue Regeneration MERLN Institute for Technology-Inspired Regenerative MedicineMaastricht University6229 ER MaastrichtThe Netherlands 3B’s Research Group I3Bs–Research Institute on BiomaterialsBiodegradables and BiomimeticsHeadquarters of the European Institute of Excellence on Tissue Engineering and Regenerative MedicineUniversity of MinhoAveParkZona Industrial da Gandra4805-017 BarcoGuimarãesPortugal ICVS/3B’s-PT Government Associate Laboratory 4806-909 Braga/GuimarãesPortugal POLYMAT University of the Basque Country UPV/EHU20018 Donostia/San SebastiánSpain IKERBASQUE Basque Foundation for Science48009 BilbaoSpain

Melt extrusion-based additive manufacturing(ME-AM)is a promising technique to fabricate porous scaffolds for tissue engi-neering applications.However,most synthetic semicrystalline polymers do not possess the intrinsic biological activity required to control cell fate.Grafting of biomolecules on polymeric surfaces of AM scaffolds enhances the bioactivity of a construct;however,there are limited strategies available to control the surface density.Here,we report a strategy to tune the surface density of bioactive groups by blending a low molecular weight poly(ε-caprolactone)5k(PCL5k)containing orthogonally reactive azide groups with an unfunctionalized high molecular weight PCL75k at different ratios.Stable porous three-dimensional(3D)scaf-folds were then fabricated using a high weight percentage(75 wt.%)of the low molecular weight PCL 5k.As a proof-of-concept test,we prepared films of three different mass ratios of low and high molecular weight polymers with a thermopress and reacted with an alkynated fluorescent model compound on the surface,yielding a density of 201-561 pmol/cm^(2).Subsequently,a bone morphogenetic protein 2(BMP-2)-derived peptide was grafted onto the films comprising different blend compositions,and the effect of peptide surface density on the osteogenic differentiation of human mesenchymal stromal cells(hMSCs)was assessed.After two weeks of culturing in a basic medium,cells expressed higher levels of BMP receptor II(BMPRII)on films with the conjugated peptide.In addition,we found that alkaline phosphatase activity was only significantly enhanced on films contain-ing the highest peptide density(i.e.,561 pmol/cm^(2)),indicating the importance of the surface density.Taken together,these results emphasize that the density of surface peptides on cell differentiation must be considered at the cell-material interface.Moreover,we have presented a viable strategy for ME-AM community that desires to tune the bulk and surface functionality via blending of(modified)polymers.Furthermore,the use of alkyne-a

关键词： Additive manufacturing Blending surface functionalization surface density Click chemistry Human

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Removal of endocrine disrupting chemicals from water through urethane functionalization of microfiltration membranes via electron beam irradiation

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Frontiers of Environmental Science & Engineering 2024年第4期18卷 61-74页

作者： Zahra Niavarani Daniel Breite Muhammad Yasir Vladimir Sedlarik Andrea Prager Nadja Schönherr Bernd Abel Roger Gläser Agnes Schulze Leibniz Institute of surface Engineering eV.(IOM) Permoserstrasse 1504318 LeipzigGermany Centre of Polymer Systems University InstituteTomas Bata University in ZlinTrida Tomase Bati 567876001 ZlinCzech Republic Institute of Chemical Technology Leipzig UniversityLinnestrasse 304103 LeipzigGermany

Polyethersulphone(PES)membranes modified with urethane functional groups were prepared through an interfacial reaction using electron beam irradiation.The removal of eight endocrine disrupting chemicals(EDCs)was studied using both pristine and functionalized PES membranes.The prepared membranes underwent characterization using several techniques,including attenuated total reflectance-Fourier transform infrared(ATR-FTIR)spectroscopy,scanning electron microscopy,contact angle analysis,and measurements of pure water flux.Furthermore,dynamic adsorption experiments were conducted to evaluate the adsorption mechanism of the prepared membrane toward the eight EDCs.The urethane functionalized membranes were hydrophilic(52°contact angle)and maintained a high permeate flux(26000 L/h m2 bar)throughout the filtration process.Dynamic adsorption results demonstrated that the introduction of urethane functional groups on the membranes significantly enhanced the removal efficiency of 17β-estradiol,estriol,bisphenol A,estrone,ethinylestradiol,and equilin.The adsorption loading of 17β-estradiol on the functionalized PES membrane was 6.7±0.7 mg/m^(2),exhibiting a 5-fold increase compared to the unmodified PES membrane.The membranes were successfully regenerated and reused for three adsorption cycles without experiencing any loss of adsorption capacity.

关键词： surface functionalization Electron beam irradiation Microfiltration Endocrine disrupting chemicals

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Plenty more room on the glass bottom： surface functionalization and nanobiotechnology for cell isolation

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Nano Research 2018年第10期11卷 5107-5129页

作者： Ali Ansari P. I. Imoukhuede Bioengineering Department University of Illinois at Urbana-Champaign Urbana IL 61B01 USA Biomedical Engineering Department Washington University in St. Louis St. Louis MO 63130 USA

surface functionalization is a widely adopted technique for surface modification which allows researchers to customize surfaces to integrate with their research. surface functionalization has been used recently to adapt surfaces to integrate with biological materials specifically to isolate cells or mimic biological tissues through cell patterning. Cell isolation and cell patterning both can be integrated with extant techniques or surfaces to customize the research to whatever needs to be tested. Substrates such as metals, biologically mimicking surfaces, environmental responsive surfaces, and even three-dimensional surfaces such as hydrogels have all been adapted to allow for functionalization for both patterning and isolation. In this review we have described both the advantages and disadvantages of these techniques and the related chemistries to better understand these tools and how best to apply them in the hope that we can further expand upon the research in the field.

关键词： surface functionalization cell isolation cell patterning self-assembled monolayers hyclrogels surface modification

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The role of surface functionalization of silica nanoparticles for bioimaging

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Journal of Innovative Optical Health Sciences 2016年第4期9卷 11-26页

作者： Maria C.Gomes Angela Cunha Tito Trindade João P.C.Tome QOPNA University of Aveiro 3810-193 AveiroPortugal CICECO and Department of Chemistry University of Aveiro 3810-193 AveiroPortugal CESAM and Department of Biology University of Aveiro 3810-193 AveiroPortugal Centro de Quimica Estrutural Instituto Superior Tecnico Universidade de LisboaAv.Rovisco Pais1049-001 LisboaPortugal Department of Organic and Macromolecular Chemistry Ghent University B-9000 Gent Belgium

Among the several types of inorganic nanoparticles available,silica nanoparticles(SNP)have earned their relevance in biological applications namely,as bioimaging agents.In fact,uorescent SNP(FSNP)have been explored in this-eld as protective nanocarriers,overcoming some limitations presented by conventional organic dyes such as high photobleaching rates.A crucial aspect on the use of uorescent SNP relates to their surface properties,since it determines the extent of interaction between nanoparticles and biological systems,namely in terms of colloidal stability in water,cellular recognition and internalization,tracking,biodistribution and speci-city,among others.Therefore,it is imperative to understand the mechanisms underlying the interaction between biosystems and the SNP surfaces,making surface functionalization a relevant step in order to take full advantage of particle properties.The versatility of the surface chemistry on silica platforms,together with the intrinsic hydrophilicity and biocompatibility,make these systems suitable for bioimaging applications,such as those mentioned in this review.

关键词： Fluorescent silica nanoparticles bioimaging surface functionalization nanoparticlecell interactions.

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Double-sided surface functionalization: An effective approach to stabilize and modulate the electronic structure of graphene-like borophene

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InfoMat 2021年第3期3卷 327-336页

作者： Xiao Tang Jinxing Gu Jing Shang Zhongfang Chen Liangzhi Kou School of Mechanical Medical and Process EngineeringQueensland University of TechnologyBrisbaneQueenslandAustralia Department of Chemistry University of Puerto RicoRio Piedras CampusSan JuanPuerto Rico

Graphene-like borophene was theoretically proposed and recently synthesized on Al(111)surface,however,how to conquer its structural instability is still an open question.By means of density functional theory computations,we theoretically predicted that honeycomb borophene can be well stabilized by double-sided surface passivation with monovalent functional groups(X=F,Cl,Br,I,OH,and NH2)due to the electron redistributions.The system undergoes the transition from metallic to semiconducting upon functionalization,while the energy gap depends on the choice of functional groups.Under external strain,the gap values can be manipulated over a broad range.Our further calculations indicated that the functionalized borophene possesses moderate and anisotropic carrier mobility,which is comparable to or even higher than some 2D materials such as MoS2 and phosphorene.Our work provides a feasible strategy to effectively stabilize the graphene-like borophene and tune the electronic properties with great potentials for electronic applications.

关键词： density functional theory calculations graphene-like borophene surface functionalization twodimensional materials

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Enhancement of Ising superconductivity in monolayer NbSe2 via surface fluorination

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Science China Technological Sciences 2024年第7期67卷 2099-2106页

作者： WU JiZheng SHI WuJun WANG Chong DUAN WenHui XU Yong SI Chen School of Materials Science and Engineering Beihang University Center for Transformative Science ShanghaiTech University Shanghai High Repetition Rate XFEL and Extreme Light Facility (SHINE) ShanghaiTech University State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics Tsinghua University Frontier Science Center for Quantum Information

Recently discovered Ising superconductors have garnered considerable interest due to their anomalously large in-plane upper critical fields(Bc2). However, the requisite strong spin-orbital coupling in the Ising pairing mechanism generally renders these superconductors heavy-element dominant with notably low superconducting transition temperatures(Tc). Here, based on the Migdal-Eliashberg theory and the mean-field Bogoliubov-de Gennes Hamiltonian, we demonstrate a significant enhancement of Ising superconductivity in monolayer NbSe2through surface fluorination, as evidenced by concomitant improvements in Tcand Bc2. This enhancement arises from three predominant factors. Firstly, fluorine atoms symmetrically and stably adhere to both sides of the monolayer NbSe2, thereby maintaining the out-of-plane mirror symmetry and locking carrier spins out-of-plane.Secondly, fluorination suppresses the charge density wave in monolayer NbSe2and induces a van Hove singularity in the vicinity of the Fermi level, leading to a marked increase in the number of carriers and, consequently, strengthening the electron-phonon coupling(EPC). Lastly, the appearance of fluorine-related, low-frequency phonon modes further augments the EPC. Our findings suggest a promising avenue to elevate Tcin two-dimensional Ising superconductors without compromising their Ising pairing.

关键词： Ising superconductivity surface functionalization upper critical field NbSe 2 first-principles calculations

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