Pseudorotaxane complexes between β-CD and mPEG derivatives bearing a carboxylic acid function (mPEG–COOH) were synthesized and investigated for their dispersing properties in a cement-based mortar. The formation of mPEG–COOH derivatives and their pseudorotaxanes was investigated by 1D nuclear magnetic resonance, diffusion ordered spectroscopy, and thermogravimetric analysis experiments. Mortar tests clearly indicate that mPEG–COOH@β-CD-interpenetrated supramolecules show excellent dispersing abilities. In addition, the supramolecular complexes show a retarding effect, analogously to other known β-CD-based superplasticizers in which the β-CD is covalently grafted on a polymeric backbone.

Water-soluble tetrasulfonate resorcin[4]arene ( 1a and 1c ) and pyrogallol[4]arene ( 1b ) macrocycles were synthesized and investigated for their dispersing properties in cement-based mortars. Mortar tests clearly show that these polyhydroxylated macrocycles (nonpolymeric) work as cement dispersants. Setting time determinations indicate that the macrocycles 1a and 1b show a retarding effect that is reminiscent of the behavior of superplasticizers (SPs) functionalized with polyhydroxylated β-CDs. Finally, the addition of sulfate anions to the cement paste does not affect the dispersing abilities of 1b , probably due to the sulfate anion capture by H-bonding interactions with its OH groups at the upper rim.

This article is focused on the research and development of new cellulose ether derivatives as innovative superplasticizers for mortar systems. Several synthetic strategies have been pursued to obtain new compounds to study their properties on cementitious systems as new bio-based additives. The new water-soluble admixtures were synthesized using a complex carboxymethylcellulose-based backbone that was first hydrolyzed and then sulfo-ethylated in the presence of sodium vinyl sulphonate. Starting with a complex biopolymer that is widely known as a thickening agent was very challenging. Only by varying the hydrolysis times and temperatures of the reactions was achieved the aimed goal. The obtained derivatives showed different molecular weight (Mw) and anionic charges on their backbones. An improvement in shear stress and dynamic viscosity values of CEM II 42.5R cement was observed with the samples obtained with a longer time of higher temperature hydrolysis and sulfo-ethylation. Investigations into the chemical nature of the pore solution, calorimetric studies and adsorption experiments clearly showed the ability of carboxymethyl cellulose superplasticizer (CMC SP) to interact with cement grains and influence hydration processes within a 48-h time window, causing a delay in hydration reactions in the samples. The fluidity of the cementitious matrices was ascertained through slump test and preliminary studies of mechanical and flexural strength of the hardened mortar formulated with the new ecological additives yielded values in terms of mechanical properties. Finally, the computed tomography (CT) images completed the investigation of the pore network structure of hardened specimens, highlighting their promising structure porosity.

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