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The role of hydrated anions in hydration lubrication

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Nano Research 2023年第1期16卷 1096-1100页

作者： Zibo Li Qian Liu Qiang Li Mingdong Dong Key Laboratory of Colloid and Interface Chemistry of the Ministry of Education School of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China Interdisciplinary Nanoscience Center(iNANO) Aarhus UniversityAarhus C DK-8000Denmark

hydration lubrication has long been invoked to account for the ultralow sliding friction between charged surfaces in aqueous environments,but still not well understood at molecular-level.Herein,we explored the lubrication effect of hydrated halogen anions on positively charged surface at the atomic scale by using three-dimensional atomic force microscopy and friction force microscopy.Atomically resolved three-dimensional imaging revealed that the anion layer was topped by a few hydration layers.The mechanical properties of the hydration layers were found mainly dependent on the concentration of electrolyte solutions and independent of the species of hydrated anions.Atomic-scale friction experiments showed that the hydration friction coefficient and friction dissipation at low concentrations were orders of magnitude lower than that at high concentrations and in pure water.Superlubricity can be achieved in low concentration electrolyte solution.These results indicated that the changes of electrolyte solution concentrations led to different adsorption state of anions on the positively charged surface which gave rise to the difference of the friction behaviors.The findings in this study reveal the role of hydrated anions in hydration lubrication and provide deep insights into the origins of hydration lubrication.

关键词： hydration lubrication hydration structures anions friction three-dimensional atomic force microscopy(3D-AFM)

hydration lubrication

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Friction 2013年第1期1卷 1-23页

作者： Jacob KLEIN Department of Materials&Interfaces Weizmann Institute of ScienceRehovot76100Israel

The hydration lubrication paradigm,whereby hydration layers are both strongly held by the charges they surround,and so can support large pressures without being squeezed out,and at the same time remain very rapidly relaxing and so have a fluid response to shear,provides a framework for understanding,controlling,and designing very efficient boundary lubrication systems in aqueous and biological media.This review discusses the properties of confined water,which-unlike organic solvents-retains its fluidity down to molecularly thin films.It then describes lubrication by hydrated ions trapped between charged surfaces,and by other hydrated boundary species including charged and zwitterionic polymer brushes,surfactant monolayers,liposomes,and biological macromolecules implicated in synovial joint lubrication.Finally,challenges and prospects for future development of this new boundary lubrication approach are considered.

关键词： hydration lubrication biolubrication boundary lubrication liposomes polymer brushes hydration repulsion hydration layers

A sulfonated modification of PEEK for ultralow friction

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Friction 2023年第6期11卷 881-893页

作者： Shihua YUAN Chenhui ZHANG State Key Laboratory of Tribology Tsinghua UniversityBeijing100084China

Polyether ether ketone(PEEK)is a widely used material for friction pairs due to its excellent mechanical strength,good wear resistance,and chemical inertness.However,some modifications are necessary when PEEK is used as a water-lubricated friction pair.In this study,a novel sulfonation method was developed to design a water-lubricated friction pair with ultralow friction,good wear resistance,and high loading capacity.PEEK powders were sulfonated using ClSO3H and sintered to form bulk plastic.The sulfonated PEEK(SPEEK)plastic exhibited good tribological properties.At a low sliding speed,the friction coefficient was smaller than 0.02 when a 3 wt% NaCl solution was used as the lubricant.The order of magnitude of the wear rate was as low as 10^(-8) mm^(3)/(N·m).The mechanism of friction reduction was mainly hydration lubrication.The negatively charged -SO_(3)^(-) groups on the friction pair can adsorb hydrated Na+cations by electrostatic interactions.These hydrated Na+cations have a high load capacity and low shearing resistance.The ultralow wear mechanism observed in this study is possibly due to ultralow friction properties of the friction pairs prepared through the proposed sulfonation and thermoforming procedures.

关键词： polyether ether ketone(PEEK) sulfonation hydration lubrication friction wear

Unlocking the secrets behind liquid superlubricity:A state-ofthe-art review on phenomena and mechanisms

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Friction 2022年第8期10卷 1137-1165页

作者： Tianyi HAN Shuowen ZHANG Chenhui ZHANG State Key Laboratory of Tribology Tsinghua UniversityBeijing 100084China

Superlubricity,the state of ultralow friction between two sliding surfaces,has become a frontier subject in tribology.Here,a state-of-the-art review of the phenomena and mechanisms of liquid superlubricity are presented based on our ten-year research,to unlock the secrets behind liquid superlubricity,a major approach to achieve superlubricity.An overview of the discovery of liquid superlubricity materials is presented from five different categories,including water and acid-based solutions,hydrated materials,ionic liquids(ILs),two-dimensional(2D)materials as lubricant additives,and oil-based lubricants,to show the hydrodynamic and hydration contributions to liquid superlubricity.The review also discusses four methods to further expand superlubricity by solving the challenge of lubricants that have a high load-carrying capacity with a low shear resistance,including enhancing the hydration contribution by strengthening the hydration strength of lubricants,designing friction surfaces with higher negative surface charge densities,simultaneously combining hydration and hydrodynamic contribution,and using 2D materials(e.g.,graphene and black phosphorus)to separate the contact of asperities.Furthermore,uniform mechanisms of liquid superlubricity have been summarized for different liquid lubricants at the boundary,mixed,and hydrodynamic lubrication regimes.To the best of our knowledge,almost all the immense progresses of the exciting topic,superlubricity,since the first theoretical prediction in the early 1990s,focus on uniform superlubricity mechanisms.This review aims to guide the research direction of liquid superlubricity in the future and to further expand liquid superlubricity,whether in a theoretical research or engineering applications,ultimately enabling a sustainable state of ultra-low friction and ultra-low wear as well as transformative improvements in the efficiency of mechanical systems and human bodies.

关键词： liquid superlubricity hydrodynamic lubrication hydration lubrication surface potential surface forces

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

Designing soft/hard double network hydrogel microsphere/UHMWPE composites to promote water lubrication performance

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Friction 2021年第3期9卷 551-568页

作者： Chaobao WANG Xiuqin BAI Conglin DONG Zhiwei GUO Chengqing YUAN Anne NEVILLE School of Energy and Power Engineering Wuhan University of TechnologyWuhan 430063China Key Laboratory of Marine Power Engineering&Technology(Ministry of Transport) Wuhan University of TechnologyWuhan 430063China Institute of Functional Surfaces School of Mechanical EngineeringUniversity of LeedsLeeds LS29JTUnited Kingdom

Several soft tissues residing in the living body have excellent hydration lubrication properties and can provide effective protection during relative motion.In order to apply this advantage of soft matters in practical applications and try to avoid its disadvantage,such as swelling and weakening in water,a design strategy of a soft/hard double network(DN)hydrogel microsphere modified ultrahigh molecular weight polyethylene(UHMWPE)composite is proposed in this study.A series of microspheres of urea-formaldehyde(UF),polyacrylamide(PAAm)hydrogel,UF/PAAm double network,and their composites were prepared.The mechanical properties,swelling,wettability,friction properties,and the lubrication mechanisms of the composites were investigated.The results show that DN microspheres can have an excellent stability and provide hydration lubrication.The performance of 75 DN-1 composite was superior to others.This finding will provide a novel strategy for the development of water-lubricated materials and have wide application in engineering fields.

关键词： double network microsphere composite friction properties hydration lubrication

Biomimetic injectable hydrogel microspheres with enhanced lubrication and controllable drug release for the treatment of osteoarthritis

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Bioactive Materials 2021年第10期6卷 3596-3607页

作者： Ying Han Jielai Yang Weiwei Zhao Haimang Wang Yulong Sun Yuji Chen Jing Luo Lianfu Deng Xiangyang Xu Wenguo Cui Hongyu Zhang State Key Laboratory of Tribology Department of Mechanical EngineeringTsinghua UniversityBeijing100084China Department of Orthopaedics Shanghai Key Laboratory for Prevention and Treatment of Bone and Joint DiseasesShanghai Institute of Traumatology and OrthopaedicsRuijin HospitalShanghai Jiao Tong University School of MedicineShanghai200025China Beijing Research Institute of Automation for Machinery Industry Co. LtdBeijing100120China

The occurrence of osteoarthritis(OA)is highly associated with the reduced lubrication property of the joint,where a progressive and irreversible damage of the articular cartilage and consecutive inflammatory response dominate the mechanism.In this study,bioinspired by the super-lubrication property of cartilage and catecholamine chemistry of mussel,we successfully developed injectable hydrogel microspheres with enhanced lubrication and controllable drug release for OA treatment.Particularly,the lubricating microspheres(GelMA@DMA-MPC)were fabricated by dip coating a self-adhesive polymer(DMA-MPC,synthesized by free radical copolymerization)on superficial surface of photo-crosslinked methacrylate gelatin hydrogel microspheres(GelMA,prepared via microfluidic technology),and encapsulated with an anti-inflammatory drug of diclofenac sodium(DS)to achieve the dual-functional performance.The tribological test and drug release test showed the enhanced lubrication and sustained drug release of the GelMA@DMA-MPC microspheres.In addition,the functionalized microspheres were intra-articularly injected into the rat knee joint with an OA model,and the biological tests including qRT-PCR,immunofluorescence staining assay,X-ray radiography and histological staining assay all revealed that the biocompatible microspheres provided significant therapeutic effect against the development of OA.In summary,the injectable hydrogel microspheres developed herein greatly improved lubrication and achieved sustained local drug release,therefore representing a facile and promising technique for the treatment of OA.

关键词： Microfluidics Hydrogel microspheres Catecholamine chemistry hydration lubrication Drug delivery

Gelatin-based composite hydrogels with biomimetic lubrication and sustained drug release

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Friction 2022年第2期10卷 232-246页

作者： Kuan ZHANG Jielai YANG Yulong SUN Yi WANG Jing LIANG Jing LUO Wenguo CUI Lianfu DENG Xiangyang XU Bo WANG Hongyu ZHANG State Key Laboratory of Tribology Department of Mechanical EngineeringTsinghua UniversityBeijing 100084China School of Chemical and Biological Engineering Shandong University of Science and TechnologyQingdao 266590China Department of Orthopedics Ruijin HospitalShanghai Jiao Tong University School of MedicineShanghai 200025China Shanghai Key Laboratory for Prevention and Treatment of Bone and Joint Diseases Shanghai Institute of Traumatology and OrthopaedicsRuijin HospitalShanghai Jiao Tong University School of MedicineShanghai 200025China Beijing Research Institute of Automationfor Machinery Industry Co. Ltd.Beijing 100120China

The occurrence of osteoarthritis is closely related to progressive and irreversible destruction of the articular cartilage,which increases the friction significantly and causes further inflammation of the joint.Thus,a scaffold for articular cartilage defects should be developed via lubrication restoration and drug intervention.In this study,we successfully synthesized gelatin-based composite hydrogels,namely GelMA–PAM–PMPC,with the properties of biomimetic lubrication and sustained drug release by photopolymerization of methacrylic anhydride modified gelatin(GelMA),acrylamide(AM),and 2-methacryloyloxyethyl phosphorylcholine(MPC).Tribological test showed that the composite hydrogels remarkably enhanced lubrication due to the hydration lubrication mechanism,where a tenacious hydration shell was formed around the zwitterionic phosphocholine headgroups.In addition,drug release test indicated that the composite hydrogels efficiently encapsulated an anti-inflammatory drug(diclofenac sodium)and achieved sustained release.Furthermore,the in vitro test revealed that the composite hydrogels were biocompatible,and the mRNA expression of both anabolic and catabolic genes of the articular cartilage was suitably regulated.This indicated that the composite hydrogels could effectively protect chondrocytes from inflammatory cytokine-induced degeneration.In summary,the composite hydrogels that provide biomimetic hydration lubrication and sustained local drug release represent a promising scaffold for cartilage defects in the treatment of osteoarthritis.

关键词： hydrogel articular cartilage zwitterionic polymer hydration lubrication drug delivery