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Germanium (Ge)-based glass ionomer cements have demonstrated the ability to balance strength with extended setting times, a unique set of characteristics for aluminum-free glass ionomer cements. However, the mechanical properties of current Ge-based glass ionomer cements significantly deteriorate over time, which jeopardizes their clinical potential. This work explores the effect of incrementally decreasing the Si:Ge ratio in the glass phase of zinc-silicate glass ionomer cements to identify potential mechanisms responsible for the time-induced mechanical instability of Ge-based glass ionomer cements. The influence of Ge was evaluated on the basis of changes in mechanical properties and molecular architecture of the cements over a 180-day period. It was observed that the compressive strength and modulus of the cements were sustained when Si:Ge ratios were ≥1:1, but when Si:Ge ratios are <1:1 these properties decreased significantly over time. These mechanical changes were independent of structural changes in the glass ionomer cement matrices, as the level of metal-carboxylate crosslinks remained constant over time across the various Si:Ge ratios explored. However, it was noted the temporal decline of mechanical properties was proportional to the increased release of degradation byproducts, in particular Ge that was released from the cements in substantially greater quantities than other glass constituents. Unexpectedly, the slowest setting cement (Si:Ge 1:1) was also the strongest; behavior that is uncommon in Si-based glass ionomer cements, supports the potential of Ge-containing glass ionomer cements as injectable bone cements in applications such as percutaneous vertebroplasty., (© The Author(s) 2016.)

Objective: To elucidate the mechanism(s) responsible for the profound impact germanium has on the setting reaction of zinc silicate glass ionomer cements (GICs)., Methods: Five <45μm glass powder compositions (0.48-xSiO2, xGeO2, 0.36 ZnO, 0.16 CaO; where x=0.12, 0.24, 0.36, 0.48mol. fraction) were synthesized. Glass degradation was assessed under simulated setting conditions using acetic acid from 0.5 to 60min, monitoring the concentrations of ions released using ICP-OES. Subsequently, GICs were prepared by mixing fresh glass powders with polyacrylic acid (PAA, Mw=12,500g/mol, 50wt% aq. solution) at a 1:0.75 ratio. Cement structure and properties were evaluated using ATR-FTIR and rheology (for 60min), as well as 24h biaxial flexural strength., Results: Reduced Si:Ge ratios yielded faster degrading glasses, yet contrary to expectation, the corresponding ATR-FTIR spectra indicated slower crosslinking within the GIC matrix. Rheology testing found the initial viscosity cement pastes reduced with decreased Si:Ge, and Ge containing cements all set significantly slower than the Si based GIC. Interestingly, biaxial flexural strength remained consistent regardless of setting behavior., Significance: This counter-intuitive combination of behaviors is attributed to the presence of a chemical complex species specific to Ge-containing glasses that delays, but does not hinder, the formation of the GIC matrix. These findings embody chemical complex species as a mechanism to decouple glass reactivity from cement setting rate, a mechanism with the potential to enhance the utility of GICs in both dental and orthopaedic applications., (Copyright © 2016 Academy of Dental Materials. Published by Elsevier Ltd. All rights reserved.)

Chemotherapeutic-loaded bone cement may be an effective method of drug delivery for the management of cancer-related vertebral fractures that require cement injection for pain relief. Recent advancements in the development of aluminum-free glass ionomer cements (GICs) have rendered this class of biomaterials clinically viable for such applications. To expand the therapeutic benefits of these materials, this study examined, for the first time, their drug delivery potential. Through incrementally loading the GIC with methotrexate (MTX) by up to 10-wt%, composition-property relationships were established, correlating MTX loading with working time and setting time, as well as compressive strength, drug release, and cytotoxic effect over 31 days. The most significant finding of this study was that MTX was readily released from the GIC, while maintaining cytotoxic activity. Release correlated linearly with initial loading and appeared to be diffusion mediated, delivering a total of 1-2% of the incorporated drug. MTX loading in this range exerted minimal effects to handling and strength, indicating the clinical utility of the material was not compromised by MTX loading. The MTX-GIC systems examined herein are promising materials for combined structural delivery applications., (© The Author(s) 2015.)

Aluminum-free glass ionomer cements (GICs) are under development for orthopedic applications, but are limited by their insufficient handling properties. Here, the addition of calcium polyphosphate (CPP) was investigated as an additive to an experimental zinc-silicate glass ionomer cement. A 50% maximum increase in working time was observed with CPP addition, though this was not clinically significant due to the short working times of the starting zinc-silicate GIC. Surprisingly, CPP also improved the mechanical properties, especially the tensile strength which increased by ∼33% after 30 days in TRIS buffer solution upon CPP addition up to 37.5 wt%. This strengthening may have been due to the formation of ionic crosslinks between the polyphosphate chains and polyacrylic acid. Thus, CPP is a potential additive to future GIC compositions as it has been shown to improve handling and mechanical properties. In addition, CPP may stimulate new bone growth and provide the ability for drug delivery, which are desirable modifications for an orthopedic cement., (© The Author(s) 2015 Reprints and permissions: sagepub.co.uk/journalsPermissions.nav.)

Adjusting powder-liquid ratio (P/L) and polyacrylic acid concentration (AC) has been documented as a means of tailoring the handling and mechanical properties of glass ionomer cements (GICs). This work implemented a novel approach in which the interactive effects of these two factors on three key GIC properties (working time, setting time, and compressive strength) were investigated using a central composite design of experiments. Using nonlinear regression analysis, formulation-property relationships were derived for each property, which enabled prediction of an optimal formulation (P/L and AC) through application of the desirability approach. A novel aluminum free GIC was investigated, as this material may present the first clinically viable GIC for use in injectable spinal applications, such as vertebroplasty. Ultimately, this study presents the first series of predictive regression models that explain the formulation-dependence of a GIC, and the first statistical method for optimizing both P/L and AC depending on user-defined inputs., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

Non-classical ionomer glasses like those based on zinc-boron-germanium glasses are of special interest in a variety of medical applications owning to their unique combination of properties and potential therapeutic efficacy. These features may be of particular benefit with respect to the utilization of glass ionomer cements for minimally invasive dental applications such as the atruamatic restorative treatment, but also for expanded clinical applications in orthopedics and oral-maxillofacial surgery. A unique system of zinc-boron-germanium-based glasses (10 compositions in total) has been designed using a Design of Mixtures methodology. In the first instance, ionomer glasses were examined via differential thermal analysis, X-ray diffraction, and (11)B MAS NMR spectroscopy to establish fundamental composition - structure-property relationships for the unique system. Secondly, cements were synthesized based on each glass and handling characteristics (working time, Wt, and setting time, St) and compression strength were quantified to facilitate the development of both experimental and mathematical composition-structure-property relationships for the new ionomer cements. The novel glass ionomer cements were found to provide Wt, St, and compression strength in the range of 48-132 s, 206-602 s, and 16-36 MPa, respectively, depending on the ZnO/GeO2 mol fraction of the glass phase. A lower ZnO mol fraction in the glass phase provides higher glass transition temperature, higher N4 rate, and in combination with careful modulation of GeO2 mol fraction in the glass phase provides a unique approach to extending the Wt and St of glass ionomer cement without compromising (in fact enhancing) compression strength. The data presented in this work provide valuable information for the formulation of alternative glass ionomer cements for applications within and beyond the dental clinic, especially where conventional approaches to modulating working time and strength exhibit co-dependencies (i.e. the enhancement of one property comes at the expense of the other) and therefore limit development strategies., (© The Author(s) 2014 Reprints and permissions: sagepub.co.uk/journalsPermissions.nav.)

This short communication determines the strength of two glass polyalkenoate cements that differ from each other through the composition of their glass phase. Sample sets of n=5, 10, 20 and 30 were formulated and tested in biaxial flexure. The derived mean for each sample set was compared against the Weibull characteristic strength. The mean and corresponding characteristic strength show a maximum percentage difference 10.1%, and the 95% confidence intervals calculated from the mean data encompass the corresponding characteristic strength down to a sample set of n=5. This suggests that, for brittle materials such as glass polyalkenoate cements, it is acceptable to test only five samples of each material in biaxial flexure and the resultant 95% confidence intervals will encompass the corresponding Weibull characteristic strength of the material., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

Vertebroplasty (VP) and balloon kyphoplasty (BKP) are now widely used for treating patients in whom the pain due to vertebral compression fractures is severe and has proved to be refractory to conservative treatment. These procedures involve percutaneous delivery of a bolus of an injectable bone cement either directly to the fractured vertebral body, VB (VP) or to a void created in it by an inflatable bone tamp (BKP). Thus, the cement is a vital component of both procedures. In the vast majority of VPs and BKPs, a poly(methyl methacrylate) (PMMA) bone cement is used. This material has many shortcomings, notably lack of bioactivity and very limited resorbability. Thus, there is room for alternative cements. We report here on two variants of a novel, bioactive, Al-free, Zn-based glass polyalkenoate cement (Zn-GPC), and how their properties compare to those of an injectable PMMA bone cement (SIMPL) that is widely used in VP and BKP. The properties determined were injectability, radiopacity, uniaxial compressive strength, and biaxial flexural modulus. In addition, we compared the compression fatigue lives of a validated synthetic osteoporotic VB model (a polyurethane foam cube with an 8 mm-diameter through-thickness cylindrical hole), at 0-2300 N and 3 Hz, when the hole was filled with each of the three cements. A critical review of the results suggests that the performance of each of the Zn-GPCs is comparable to that of SIMPL; thus, the former cements merit further study with a view to being alternatives to an injectable PMMA cement for use in VP and BKP.

The suitability of zinc-based glass polyalkenoate cements (GPCs) for use in orthopaedics can be improved by the substitution of strontium into the glass phase which should impart improved radiopacity and bone forming properties to the cements without retarding strength. The purpose of this research was to produce novel GPCs based on calcium-strontium-zinc-silicate glasses and to evaluate their mechanical properties and biocompatibility with the ultimate objective of developing a new range of cements for skeletal applications. Three glass compositions, based on incremental substitutions of strontium for calcium, were synthesized; BT100 (0.16CaO, 0.36ZnO, 0.48SiO2), BT101 (0.04SrO, 0.12CaO, 0.36ZnO, 0.48SiO2) and BT102 (0.08SrO 0.08CaO, 0.36ZnO, 0.48SiO2). Each glass was then mixed with varying concentrations and molecular weights of polyacrylic acids in order to determine the working times, setting times, compressive strengths and biaxial flexural strengths of the novel cements. The maximum working time and setting time achieved was 29 and 110 s respectively; which, at present is inadequate for current clinical procedures. However, the optimum compressive and biaxial flexural strengths were up to 75 and 34 MPa respectively indicating that these formulations have potential in load bearing applications. Importantly, the substitution of Ca with Sr in the glasses did not have a deleterious effect on strengths or working times. Finally, the bioactivity of the best performing cements was determined in vitro using simulated body fluid. It was found that all cements facilitate the formation of an amorphous calcium phosphate at their surface which increases in density and coverage with time, indicating that these cement will bond directly to bone in vivo.

Glass polyalkenoate cements (GPCs) have been used in dentistry for over 40 years. These novel bioactive materials are the result of a reaction between a finely ground glass (base) and a polymer (acid), usually poly(acrylic acid) (PAA), in the presence of water. This article reviews the types of PAA used as reagents (including how they vary by molar mass, molecular weight, concentration, polydispersity and content) and the way that they control the properties of the conventional GPCs (CGPCs) formulated from them. The article also considers the effect of PAA on the clinical performance of CGPCs, including biocompatibility, rheological and mechanical properties, adhesion, ion release, acid erosion and clinical durability. The review has critically evaluated the literature and clarified the role that the polyacid component of CGPCs plays in setting and maturation. This review will lead to an improved understanding of the chemistry and properties of the PAA phase which will lead to further innovation in the glass-based cements field. [ABSTRACT FROM AUTHOR]