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The latest studies on the reactivity of inorganic-polymeric networks in selected cement-based materials and the focus toward nano- and atomic levels of grafting of polymers on interfaces represent some of the success stories of materials chemistry. Recent developments are reviewed and discussed, with particular emphasis on macro-defect-free (MDF) materials. Experimental evidence of next-nearest-neighbor (NNN) interactions has led to the definition of the scope and model of Al(Fe)–O–P cross-linking under mechanochemical synthesis conditions, in a system combining the most common (Portland) cement and commercially available polyphosphates. Current approaches to synthesis of MDF materials, together with the atomic-level interpretations of both the formed functional interfaces and the adverse influence of moisture, are discussed.

Contribution of materials chemistry to the knowledge of macro-defect-free (MDF) materials