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The unique properties and sustainability advantages of sulfur polymer cement have led to efforts to use them as alternatives to traditional Portland cement. The current study explores the impact of environmental stresses on the strength development of polymer composite SunBG90, a material composed of animal and plant fats/oils vulcanized with 90 wt. % sulfur. The environmental stresses investigated include low temperature (−25 °C), high temperature (40 °C), and submersion in water, hexanes, or aqueous solutions containing strong electrolyte, strong acid, or strong base. Samples were analyzed for the extent to which exposure to these stresses influenced the thermo-morphological properties and the compressional strength of the materials compared to identical materials allowed to develop strength at room temperature. Differential scanning calorimetry (DSC) analysis revealed distinct thermos-morphological transitions in stressed samples and the notable formation of metastable γ-sulfur in hexane-exposed specimens. Powder X-ray diffraction confirmed that the crystalline domains identified by DSC were primarily γ-sulfur, with ~5% contribution of γ-sulfur in hexane-exposed samples. Compressive strength testing revealed high strength retention other than aging at elevated temperatures, which led to ~50% loss of strength. These findings reveal influences on the strength development of SunBG90, lending important insight into possible use as an alternative to OPC. 

Abstract Poly(methyl methacrylate) (PMMA) is an important commodity polymer having a wide range of applications. Currently, only about 10% of PMMA is recycled. Herein, a simple two‐stage process for the chemical upcycling of PMMA is discussed. In this method PMMA is modified by transesterification with a bio‐derived, olefin‐bearing terpenoid, geraniol. In the second stage, olefin‐derivatized PMMA is reacted with sulfur to form a network composite by an inverse vulcanization mechanism. Inverse vulcanization of PGMA with elemental sulfur (90 wt.%) yielded the durable compositePGMA‐S. This composite was characterized by NMR spectrometry, IR spectroscopy, elemental analysis, thermogravimetric analysis, and differential scanning calorimetry. Composite water uptake, compressional strength analysis, flexural strength analysis, tensile strength analysis, and thermal recyclability are presented with comparison to current commercial structural materials.PGMA‐Sexhibits a similar compressive strength (17.5 MPa) to that of Portland cement.PGMA‐Sdemonstrates an impressive flexural strength of 4.76 MPa which exceeds the flexural strength (>3 MPa) of many commercial ordinary Portland cements. This study provides a way to upcycle waste PMMA through combination with a naturally‐occurring olefin and industrial waste sulfur to yield composites having mechanical properties competitive with ecologically detrimental legacy building materials. 

Ordinary Portland Cement (OPC) production consumes tremendous amounts of fresh water and energy and releases vast quantities of CO2 into the atmosphere. Not only would an alternative to OPC whose production requires no water, releases little CO2, and consumes less energy represent a transformative advance in the pursuit of industrial decarbonization, but the greater availability of safe drinking water would lead to significantly improved public health, particularly among vulnerable populations most at risk from contaminated water supply. For any OPC alternative to be adopted on any meaningful scale, however, its structural capabilities must meet or exceed those of OPC. An inverse vulcanization of brown grease, sunflower oil, and elemental sulfur (5:5:90 weight ratio) was successfully modified to afford the high-sulfur-content material SunBG90 in quantities > 1 kg, as was necessary for standardized ASTM and ISO testing. Water absorption (ASTM C140) and thermal conductivity (ISO 8302) values for SunBG90 (<1 wt% and 0.126 W·m−1·K−1, respectively) were 84% and 94% lower than those for OPC, respectively, suggesting that SunBG90 would be more resistant against freeze-thaw and thermal stress damage than OPC. Consequently, not only does SunBG90 represent a more environmentally friendly material than OPC, but its superior thermomechanical properties suggest that it could be a more environmentally robust material on its own merits, particularly for outdoor structural applications involving significant exposure to water and seasonal or day/night temperature swings.