Abstract
Efficient carbon capture and utilization require strategies that minimize energy penalties of CO(2) regeneration and compression. Reactive capture and conversion (RCC) address this challenge by integrating capture with direct electrochemical conversion. Here, we show an NH(3)-mediated tandem RCC system that couples capture of CO(2) from simulated flue gas (10% v/v CO(2) in N(2)) with electroreduction of NH(4)HCO(3) to CO over a Ni single-atom catalyst (Ni-SAC). Speciation modeling and capture experiments revealed that a deep CO(2) capture with C/N ratio of 0.65 was achieved using 2.5 M NH(3) from simulated flue gas. Electrolysis of the resulting NH(4)HCO(3) on the Ni-SAC delivered an 85% CO Faradaic efficiency at 100 mA/cm(2) with excellent tolerance to NH(3)/NH(4) (+) as confirmed by DFT calculations and ab initio molecular dynamics (AIMD) simulations. Further, the techno-economic analysis established a levelized total cost of CO manufacturing of $25.43/kmol, gauging the practical viability. Overall, this study holds great potential to decarbonize the chemical manufacturing industry while reducing synthetic production costs.