NH3-Mediated Reactive Capture and Conversion: Integrating CO2 Absorption from Flue Gas with CO Production via NH4HCO3 Electrolysis
Efficient carbon capture and utilization require strategies that minimize energy penalties of CO2 regeneration and compression. Reactive capture and conversion (RCC) address this challenge by integrating capture with direct electrochemical conversion. Here, we show an NH3-mediated tandem RCC system that couples capture of CO2 from simulated flue gas (10% v/v CO2 in N2) with electroreduction of NH4HCO3 to CO over a Ni single-atom catalyst (Ni-SAC). Speciation modeling and capture experiments revealed that a deep CO2 capture with C/N ratio of 0.65 was achieved using 2.5 M NH3 from simulated flue gas. Electrolysis of the resulting NH4HCO3 on the Ni- SAC delivered an 85% CO Faradaic efficiency at 100 mA/cm2 with excellent tolerance to NH3/NH4+ as confirmed by DFT calculations and ab initio molecular dynamics (AIMD) simulations. Further, the technoeconomic 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.
- Research Organization:
- Ames Laboratory (AMES), Ames, IA (United States); Iowa State Univ., Ames, IA (United States); Iowa State University, Ames, IA (United States); University of Oklahoma, Norman, OK (United States); Wichita State University, KS (United States)
- Sponsoring Organization:
- National Science Foundation; USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
- Grant/Contract Number:
- AC02-07CH11358; SC0018284; SC0025376
- OSTI ID:
- 3365166
- Journal Information:
- ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 4 Vol. 11; ISSN 2380-8195
- Publisher:
- American Chemical Society (ACS)Copyright Statement
- Country of Publication:
- United States
- Language:
- English
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