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Fig. 2.4 Cartilage has two main lubrication modes: (a) Fluid Film Lubrication: Shear stress (fric­tion force per unit surface area) is represented by σ=ηv/D, where η is the lm viscosity, v is the sliding velocity, and D is the lm thickness. Shear stress varies linearly with sliding velocity, and a continuous lubricating lm reduces friction during joint movement. (b) Boundary Lubrication: Frictional dissipation for specic lubricating molecules creates a protective boundary layer that is independent of different substrates, reducing direct contact and minimizing friction between carti­lage surfaces [172]
N. Chowdhury etal.
cartilage surface. Although cartilage experiences signicant compression loading, it exhibits a notable tensile modulus, restricting substantial expansion in the trans­verse direction. This high tensile stiffness resists lateral expansion like a conning chamber’s rigid side wall. Thus, signicant pressure generation by the interstitial uid is required to support the applied compressive stress, even during unconned compression. In Fig.2.4a, the uid lm lubrication regime is shown elaborately where uid lm lubrication is dened as shear stress (friction force per unit surface area) is represented by σ=ηv/D, where η is the lm viscosity, v is the sliding veloc­ity, and D is the lm thickness [20]. The crucial role of collagen in articular cartilage is underscored by its remarkable capacity to effectively withstand tension, even when the tissue is subjected to compressive stress. Collagen in the supercial zone is aligned parallel to the articular surface, this structural arrangement optimizes the interstitial uid’s support on the surface. The Peclet number, a ratio of convective sliding velocity to diffusive interstitial uid ow velocity, is a crucial factor in reducing the coefcient of friction. When there is a moving contact, the interstitial uid experiences pressurization due to migration, and if the migration speed sur­passes the diffusive velocity of interstitial uid, before the contact traction shifts, the pressurized uid has a limited window to escape.
In contrast, during steady state rolling or sliding, when the interstitial uid ows faster through the tissue than the contact region migrates, sufcient time allows the
2 Characterization ofHydrogel Properties intheAdvancement ofBio-Tribology
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uid under pressure to move away from the area experiencing load, resulting in reduced pressure of the interstitial uid. Hence, the notable impact of the pressur­ized uid on cartilage’s frictional and lubrication underscores the complex interac­tion between the uid and solid components of articular cartilage [18, 19].

2.3.2 Boundary Lubrication

Research ndings suggest that under reduced pressures, the presence of uid lms becomes apparent when joint movement brings the opposing cartilage surfaces into direct contact. In these instances, the hydrodynamic lm of synovial uid might not adequately separate the surfaces, particularly when subjected to high-pressure con­ditions or slow sliding speeds. As a result, the cartilage surfaces encounter friction and wear, leading to potential damage and deterioration. Hence, at high pressures, boundary lubrication depends upon the interaction of molecules, such as lubricin, hyaluronic acid, and synovial uid between the joint’s articulating surfaces. In con­ditions where lubrication of uid lm is not feasible due to low uid viscosity, low sliding speeds, and high loads, boundary lubrication or a molecular lm may be observed, and become evident between the articulating surfaces [20, 21]. During periods of rest or low-load conditions, the synovial uid within the joint serves as a lubricant, containing specic lubricating molecules such as lubricin [154]. These molecules adhere to the surfaces of cartilage, establishing a boundary layer that prevents direct contact and reduces friction between the opposing joint surfaces. This mechanism of boundary lubrication effectively minimizes wear and friction during low-intensity movements [16].
Comparable boundary lubricating layers have been observed on tendon surfaces, where specialized binder molecules contribute to low friction over multiple cycles [22, 23]. In cartilage, the formation of boundary-lubricating layers is attributed to the presence of various essential molecules, acting either independently or in syn­ergy. These molecules include lubricin, hyaluronic acid (HA), aggrecans, and phos­pholipids (PLs) as shown in Fig. 2.4b [16]. The presence of these lubricating molecules and the development of lubricating boundary layers, including HA, aggrecans, lubricin, and PLs, effectively reduce friction between cartilage surfaces and shield them from direct contact. This maintains proper joint function and mini­mizes wear during loading conditions [20, 22, 23]. Boundary lubricants play a cru­cial role during the start-up and slow movement phases of joint motion when the hydrodynamic lm may not be fully developed, and the cartilage surfaces are more vulnerable to direct contact [21]. In such instances, the protective layer of boundary lubrication serves as a defense mechanism by signicantly reducing the extent of direct surface interaction, thus mitigating friction and wear.
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2.3.3 Hydrodynamic Lubrication

Articular cartilage, the load-bearing tissue in joints, relies on hydrodynamic lubrica­tion as a crucial mechanism to reduce wear and friction during joint movements. This lubrication process involves the creation of a uid lm between the opposing surfaces of the cartilage, providing favorable conditions of low wear and friction. Various studies have been performed, utilizing experimental and computational approaches, to examine the hydrodynamic lubrication of the articular cartilage. One notable study by Jay, Waller, and Elsaid (2017) focused on examining the role of boundary lubricants, like hyaluronic acid, in reducing friction and wear in specic joints. Their research demonstrated that boundary lubrication is crucial for joint function, protects the articulating surfaces, and reduces friction and wear in the joint [24, 25]. Figures2.5 and 2.6 show the gradual transition from boundary lubrication to hydrodynamic lubrication through mixed and electrohydrodynamic regimes [11,
168]. Similarly, Gleghorn etal. (2008) employed a microuidic device to study the
lubrication properties of cartilage. Their ndings highlighted the crucial role of lubricin, a glycoprotein present in synovial uid, in reducing friction and preventing surface damage [26]. Furthermore, Dowson, Jin, and Wallbridge (2012) conducted experiments to measure the lubrication and friction characteristics of articular carti­lage. Their research provided valuable insights into the composition of synovial uid and the properties of lubricants that contribute to achieving efcient lubrica­tion [27]. These collective studies emphasized the role of boundary lubricants and hydrodynamic lubrication in preserving the health and functionality of articular car­tilage, contributing valuable insights to the eld of joint mechanics [2427].
Fig. 2.5 Stribeck curve explained for a boundary, mixed, and hydrodynamic lubrication regime [168]
2 Characterization ofHydrogel Properties intheAdvancement ofBio-Tribology
Fig. 2.6 (a) boundary lubrication—joints come in direct contact for lack of lubricant. (b) Mixed lubrication has both uid lms including boundary lubrication. (c) Elastohydrodynamic—In the presence of uid lm, deformation happens. (d) Hydrodynamic lubrication full uid lm present [11]
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2.3.4 Squeeze-Film Lubrication

The cartilage layer undergoes deformation, leading to an enlargement of the load­supporting area. Within the lubricant, this deformation plays a role in reducing the speed of the lateral uid. The lubricant uid within the gap is compelled to move from the central high-pressure region into the cartilage, therefore. Tensile hoop stress is prevalent at the surface of the cartilage under the loading condition of com­pressive squeeze lm. In Fig.2.7c, it is shown that interstitial deformation-induced uid exudation and pressurization give rise to the squeeze lm lubrication regime. The radial ow of interstitial uid is induced by the hoop stress within the layer of the cartilage. Although various efforts have been made to address unidirectional ltration, conned-unconned compression, and loading, only Hou etal. consid­ered the biphasic and viscous nature of the uid. The cartilage uid lm exhibits Newtonian behavior, characterized by linear viscosity and incompressibility. Additionally, the cartilage can be described as a linear biphasic material, mainly due to its support from the subchondral bone. The research ndings indicate that for
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Fig. 2.7 (a) Representation of a human joint model. (bd) Depiction of distinct approaches to cartilage lubrication [29]
N. Chowdhury etal.
diarthrodial joints operating under squeeze-lm conditions, the advanced lubrica­tion theory put forth by Walker etal. (1968) is likely to be signicant, alongside other mechanisms such as ultraltration (Maroudas, 1967) or boundary lubrication (Swann and coworkers, 1972, 1985) [28]. These lubrication mechanisms are expected to have substantial effects on joint function and overall health in such cir­cumstances, underscoring their importance in comprehending joint mechanics and maintenance [153].

2.3.5 Synovial Fluid

Synovial uid comprises three essential components—lubricin/(SZP)/PRG4, SAPLs, and HA, which are important effects for tribological characterization [22,
3032]. Synovial uid structure is shown in Fig.2.8 where there is Hyaluronan,
Lubricin, and Aggrecan combined in a uid surface layer [20]. Hyaluronic acid is a primary component of the extracellular matrix, composed of N-acetylglucosamine and repeating sugars glucuronic acid. While it was initially hypothesized that HA has a signicant contribution to lubrication of the cartilage. Bovine synovial uid without HA showed low viscosity which had no impact on the lubrication charac­teristics of the treated uid [33, 34, 155]. This suggests that HA does not form or
2 Characterization ofHydrogel Properties intheAdvancement ofBio-Tribology
Fig. 2.8 Synovial uid structure of articular cartilage [173]
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bind to the surface of the cartilage, which is essential for lubrication. However, it has been observed that HA does contribute to a reduction in friction [35]. Further experiments indicate that HA’s chondroprotective property primarily aids wear mechanisms rather than affecting friction levels [22, 30, 31].
Surface active phospholipids (SAPL) possess hydrophobic properties, leading to the assumption that they protect joints from solid-solid contact. However, research ndings have demonstrated that the removal of SAPL does not impact surface char­acteristics, such as lubrication or friction. Still, there is not enough literature to conrm this, current projections propose that SAPL has minimal impact on synovial uid’s lubricity [30, 36]. Lubricin is encoded by gene prg4 as a group of proteins with a molecular weight of 227–232kDa. Figure2.9 shows the molecular structure of the hypothesized lubricants: (A) SZP, (B) HA, and (C) SAPLs like phosphatidyl­choline [16]. Other related proteins in this group include PRG4 and SZP.According to the hypothesis, SZP, which is a proteoglycan, forms a nanolm, which aids in reducing and smoothing the roughness of the articular cartilage, consequently decreasing friction. Supercial zone protein has also been identied in various ana­tomical locations, such as the meniscus, ligament tendon, and infrapatellar fat pad [36, 37]. Moreover, SZP plays a signicant role in preventing fouling of the articu­lar surface and hyper-proliferation of synovial cells, thus contributing to the overall health and function of the joint [22, 38, 157, 166].
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Fig. 2.9 Molecular structure of the hypothesized lubricants: (a) SZP, (b) HA, and (c) SAPLs like phosphatidylcholine. SZP has a molecular weight of 345kDa, and it originates from the prg4 gene [16]
N. Chowdhury etal.

2.3.6 Hydration Lubrication

Due to its large dipole, the hydration shell surrounding ions in an aqueous medium is rmly bound to the charged ion. The hydration shell demonstrates notable uidity as a result of the quick water molecule exchange with the adjacent unbound water molecules [20]. The hydration shell resists compression under load when ions or charges are present between conning surfaces. It prevents the water of hydration from being squeezed out. However, when subjected to shear forces, the compressed hydration layer behaves uidly [36, 39]. This phenomenon is evident in articular cartilage, where the triphasic model enhances our comprehension of friction proper­ties. The mechanism of hydration lubrication of articular cartilage is shown in Fig.2.10 [42]. Specically, the monovalent ion’s impact within the cartilage’s inter­stitial uid, representing that another uid phase is present, has been investigated to assess its inuence on friction properties [32]. The remarkable lubrication proper­ties of cartilage in aqueous environments stem from its ability to support substantial compressive loads while also displaying a uid-like response to shear forces [39]. Studies have examined the behavior of hydration layers under compression between different surfaces. Despite having a signicantly higher effective viscosity in com­parison to bulk water, the hydration shell remains uid-like and responsive under
2 Characterization ofHydrogel Properties intheAdvancement ofBio-Tribology
Fig. 2.10 Hydration lubrication of cartilage [42]
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shear forces [39]. Lubrication effects have been observed in systems involving trapped hydrated ions, such as between mica surfaces, silica particles and wafers, and macroscopic silicon surfaces. These systems demonstrate remarkably low fric­tion coefcients, even under high-pressure conditions, which further reinforces the concept of hydration lubrication [3941]. Hydration lubrication provides valuable insights into the underlying mechanisms that result in reduced boundary friction seen in cartilage under physiological pressures. Moreover, this concept has been expanded to include other boundary lubrication systems in aqueous solutions, encompassing charged polymers, surfactants, polyzwitterionic brushes, and bilay­ers of PC lipids or liposomes. On their external surfaces, these systems exhibit phosphocholine groups.
2.4 Cartilage Mechanical andSurface Properties
The response of cartilage to physiological forces invivo is inuenced by its mechan­ical characteristics in both tension and compression [43]. The lubrication of the articular cartilage becomes complex due to the tissue’s relatively high compliance and permeability [44]. Calculated permeability (k) was found to be 1.2×10–15m4/Ns and aligns with values reported in the literature [7, 13]. Moreover, the measured elastic modulus (E) was 2.24MPa. The rehydration rate is controlled by the sliding velocity, and the unloading of cartilage tissue during each cycle varies [32]. The tissue’s permeability and the diffusive drag coefcient of uid motion within the porous solid matrix are inversely related. As a result, the load-deformation response of the tissue that was measured is inuenced by the tissue’s non-linearly permeable nature [45]. Osmotic pressure within cartilage impacts uid pressurization and fric­tional properties [46]. The matrix’s osmotic swelling pressure regulates water trans­port in cartilage. The concentration of ions in the adjacent uid medium inuences water rate efux and inux through cartilage [43]. Chemical properties, like proteo­glycan and collagen content, signicantly contribute to cartilage’s tribological prop­erties [43, 47]. The non-linear permeability function strongly affects the stress-relaxation behavior of the tissue and compressive creep, mainly governing phenomena related to viscosity and elasticity [45].
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2.4.1 The Friction ofArticular Cartilage
Ranging from 0.005 to 0.02, hyaline cartilage exhibits a remarkably low coefcient of friction, of any material [16]. Due to cartilage’s biphasic nature, researchers sug­gested that the articular surface’s friction force is related to the load supported by the solid phase [18]. They used a pin-on-plate test conguration to study friction properties, nding initial coefcients of friction (μ0) ranging from 0.0147 to 0.006 and friction coefcients (μq) at uid depressurization ranging from 0.2817 to 0.011 for cartilage lubricated with phosphate-buffered saline (PBS) [44]. Cartilage exhib­its boundary mode lubrication in areas of low speed and high strain, while mixed­mode lubrication follows the Stribeck curve in regions of higher speed and lower strain. At 1–2.5 mm/s, mixed-mode lubrication is prevalent, transitioning from mostly boundary lubrication at lower speeds [44]. The water content inuences the cartilage’s friction properties, with the friction coefcient decreasing as the surface concentration of proteoglycan relates to the water content of the hydrophilic layer [48, 49]. Interstitial uid pressure also affects friction, with higher pressure result­ing in lower friction coefcients [49, 50, 156]. Moreover, frictional properties depend on the nanoscale structure of the surface layer and water content [51]. As loading times increase, uid is displaced from the contact zone, transferring the load to the cartilage’s solid phase, and resulting in higher frictional force during startup. The friction coefcient decreases with increasing load, which implies that the frictional force does not increase in direct proportion to the applied load due to interstitial uid support and benecial friction properties of boundary lubricant molecules in cartilage. A common assumption in the literature is a linear relation­ship between frictional force and applied force, the possibility of a non-linear rela­tion and its effects should be considered [52].
2.4.2 Wear ofCartilage
From a mechanical perspective, wear refers to material removal from contact sur­faces through mechanical action. Cartilage tissue can experience various forms of wear, such as abrasive, adhesive, or fatigue wear [19]. Besides mechanical wear, cartilage, being a biological tissue, is also susceptible to biochemical degradation. The repair process involves collagen and proteoglycan secretion by chondrocytes. However, the avascular nature of cartilage, slow waste removal, and limited nutrient supply lead to reduced metabolic activity and prolonged healing times [53]. Cartilage wear can be aggravated by factors like abnormal biomechanical loading, trauma, altered mechano-chemical transduction by chondrocyte senescence, chon­drocytes, pathological changes, proteolytic enzymes, metabolic disorders in the collagen-proteoglycan matrix, and loss of lubrication mechanisms [54, 55]. These factors can either act individually or in combination, leading to increased wear rates beyond natural or normal repair [54, 55]. The wear of articular cartilage can also be
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Fig. 2.11 (a) The alterations in the articular structure that occur during the progression of osteo­arthritis (OA). (b) Cellular responses observed in cartilage affected by osteoarthritis [56]
inuenced by the specic loading conditions it is exposed to and to its location within the joint. It is experienced repeatedly. The wear mechanism of cartilage is shown in Fig.2.11a, b where alterations in the articular structure that occur during the progression of osteoarthritis and cellular responses observed in cartilage affected by osteoarthritis are depicted. Synovial uid offers protective qualities against car­tilage wear [32]. Surface friction, uid contents, and tissue properties (strength and stiffness) signicantly inuence articular cartilage‘s wear resistance, and synovial lubrication plays a distinct protective role [43, 54].
2.5 Development ofHydrogels forPotential
Replacement Materials
As articular cartilage cannot regenerate completely after injury or defects due to aging, many synthetic materials have been composed to use as biological cartilage replacements. Some potential materials are polymers like silicon, hydrogel, and so on. Recently, a hydrogel is the most potential synthetic bio-replacement material as
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