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In this work, the influence of the liquid phase composition on the physicochemical properties of double hybrid-type bone substitutes was investigated. The solid phase of obtained biomicroconcretes was composed of highly reactive α-tricalcium phosphate powder (α-TCP) and hybrid hydroxyapatite/chitosan granules (HA/CTS). Various combinations of disodium phosphate (Na 2 HPO 4 ) solution and citrus pectin gel were used as liquid phases. The novelty of this study is the development of double-hybrid materials with a dual setting system. The double hybrid phenomenon is due to the interactions between polycationic polymer (chitosan in hybrid granules) and polyanionic polymer (citrus pectin). The chemical and phase composition (FTIR, XRD), setting times (Gillmore needles), injectability, mechanical strength, microstructure (SEM) and chemical stability in vitro were studied. The setting times of obtained materials ranged from 4.5 to 30.5 min for initial and from 7.5 to 55.5 min for final setting times. The compressive strength varied from 5.75 to 13.24 MPa. By incorporating citrus pectin into the liquid phase of the materials, not only did it enhance their physicochemical properties, but it also resulted in the development of fully injectable materials featuring a dual setting system. It has been shown that the properties of materials can be controlled by using the appropriate ratio of citrus pectin in the liquid phase.

Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Materials based on highly reactive α-tricalcium phosphate (α-TCP) powder were developed and evaluated. Furthermore, the impact of different polymeric additives, such as citrus pectin or polyacrylamide (PAAM) modified with sago starch, neem flower, or rambutan peel, on the physiochemical and biological properties of the developed materials was assessed. The addition of modified PAAM shortened the setting process of bone cements and decreased their compressive strength. On the other hand, the addition of citrus pectin significantly enhanced the mechanical strength of the material from 4.46 to 7.15 MPa. The improved mechanical properties of the bone cement containing citrus pectin were attributed to the better homogenization of cementitious pastes and pectin cross-linking by Ca2+ ions. In vitro tests performed on L929 cells showed that 10% extracts from α-TCP cements modified with pectin are more cytocompatible than control cements without any additives. Cements containing PAAM with plant-derived modifiers show some degree of cytotoxicity for the highly concentrated 10% extracts, but for diluted extracts, cytotoxicity was reduced, as shown by a resazurin reduction test and live/dead staining. All the developed bone substitutes exhibited in vitro bioactivity, making them promising candidates for further biological studies. This research underscores the advantageous properties of the obtained biomaterials and paves the way for subsequent more advanced in vitro and in vivo investigations. [ABSTRACT FROM AUTHOR]