Commercial exploitations of phosphogypsum and CO2 are the research hotspots and difficulties. A coupled reaction and separation airlift loop reactor, which integrates four consecutive processes (i.e., dissolution of slightly soluble raw material, impurity separation, product preparation, and product separation) for reactive crystallization, was proposed to continuously prepare high-value products (i.e., (NH4)2SO4 and nano-sized CaCO3) using waste to treat waste (i.e., phosphogypsum and CO2) at ambient conditions by a one-step method. The technical feasibilities of the coupled reactor were verified, and principal influencing factors on the CaCO3 product quality were systematically investigated and optimized. Additionally, the coupled fluid hydrodynamics dependent on the two individual airlift loop reactors were also inspected. This work shed some new light on the practical resource utilization of phosphogypsum and waste CO2 in tandem at a low cost, and a solid basis for the rational design, optimization, and scale-up of such promising reactors was provided.
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