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Abstract Rapid decarbonization of the cement industry is critical to meeting climate goals. Oversimplification of direct air capture benefits from hydrated cement carbonation has skewed the ability to derive decarbonization solutions. Here, we present both global cement carbonation magnitude and its dynamic effect on cumulative radiative forcing. From 1930–2015, models suggest approximately 13.8 billion metric tons (Gt) of CO₂was re-absorbed globally. However, we show that the slow rate of carbonation leads to a climate effect that is approximately 60% smaller than these apparent benefits. Further, we show that on a per kilogram (kg) basis, demolition emissions from crushing concrete at end-of-life could roughly equal the magnitude of carbon-uptake during the demolition phase. We investigate the sensitivity of common decarbonization strategies, such as utilizing supplementary cementitious materials, on the carbonation process and highlight the importance of the timing of emissions release and uptake on influencing cumulative radiative forcing. Given the urgency of determining effective pathways for decarbonizing cement, this work provides a reference for overcoming some flawed interpretations of the benefits of carbonation. 

Abstract Population and development megatrends will drive growth in cement production, which is already one of the most challenging-to-mitigate sources of CO₂emissions. However, availabilities of conventional secondary cementitious materials (CMs) like fly ash are declining. Here, we present detailed generation rates of secondary CMs worldwide between 2002 and 2018, showing the potential for 3.5 Gt to be generated in 2018. Maximal substitution of Portland cement clinker with these materials could have avoided up to 1.3 Gt CO₂-eq. emissions (~44% of cement production and ~2.8% of anthropogenic CO₂-eq. emissions) in 2018. We also show that nearly all of the highest cement producing nations can locally generate and use secondary CMs to substitute up to 50% domestic Portland cement clinker, with many countries able to potentially substitute 100% Portland cement clinker. Our results highlight the importance of pursuing regionally optimized CM mix designs and systemic approaches to decarbonizing the global CMs cycle. 

Methods to sequester and store atmospheric CO2 are critical to combat climate change. Alkaline-rich bioashes are potential carbon fixing materials. This work investigates potential co-benefits from mineralizing carbon in biomass ashes and partially replacing high embodied greenhouse gas (GHG) Portland cement (PC) in cement-based materials with these ashes. Specifically, rice hull ash (RHA), wheat straw ash (WSA), and sugarcane bagasse ash (SBA) were treated to mineralize carbon, and their experimental carbon content was compared to modeled potential carbonation. To understand changes in the cement-based storage materials, mortars made with CO2-treated WSA and RHA were experimentally compared to PC-only mortars and mortars made with ashes without prior CO2 treatment. Life cycle assessment methodology was applied to understand potential reductions in GHG emissions. The modeled carbonation was ∼18 g-CO2/kg-RHA and ∼180 g-CO2/kg-WSA. Ashes oxidized at 500 °C had the largest measured carbon content (5.4 g-carbon/kg-RHA and 35.3 g-carbon/kg-WSA). This carbon appeared to be predominantly residual from the biomass. Isothermal calorimetry showed RHA-PC pastes had similar heat of hydration to PC-pastes, while WSA-PC pastes exhibited an early (at ∼1.5 min) endothermic dip. Mortars with 5 % and 15 % RHA replacement had 1–12 % higher compressive strength at 28 days than PC-only mortars, and milled WSA mortars with 5 % replacement had 3 % higher strength. A loss in strength was noted for the milled 15 % WSA, the CO2-treated 5 %, and the 15 % WSA mortars. Modeled reductions in GHG emissions from CO2-treated ashes were, however, marginal (<1 %) relative to the untreated ashes. 

Population growth and urbanization over the coming decades are anticipated to drive unprecedented demand for infrastructure materials and energy resources. Unfortunately, factors such as the degree of resource consumption, the energy-intensive nature of production, and the chemical-reaction driven emissions make infrastructure materials production industries among the greatest contributors to anthropogenic CO2 emissions. Yet there is an often-overlooked potential environmental benefit to infrastructure materials: most remain in use for decades and their long service lives can facilitate extended storage of carbon. In this perspective, we present an overview of recent technological advancements that can support infrastructure materials acting as a global, distributed carbon sink and discuss areas for further research and development. We present mechanisms to quantify the extent to which the embodied carbon will be removed from the carbon cycle for a long enough period of time to provide carbon sequestration and climate benefit. We conclude that it is possible to unlock the vast potential to engineer a carbon sequestration system that simultaneously meets societal need for expanding infrastructure systems; however, complexities in how these systems are engineered must be systematically and quantitatively incorporated into materials design.