Durable and Active Fe–N–C Assisted by Fe Nanoparticle and Graphitic Layers for Efficient Carbamate Decomposition During Amine‐Based Carbon Capture

Abstract A feasible Fe–N–C catalysts (Fe/Fe SA @GNC) with multiple Fe species and well‐graphitized carbon layers is prepared to boost the carbamate decomposition kinetics for energy‐saving CO 2 capture with amine solvent. Fe precursor carbothermic reaction creates the graphitic layers doped with pyridinic‐N, which significantly enhances the activity of the coordinated Fe sites. Furthermore, the enclosed Fe nanoparticles originate from excess Fe precursor firmed the atomically dispersed Fe–N–C sites in graphitic layers. The as‐prepared catalysts exhibit superior activity for carbamate decomposition under relatively mild conditions. The maximum desorption rate soar to 5.4 CO 2 mmol min −1 , marking 440% increment compared to the catalyst‐free reaction. Notably, the Fe/Fe SA @GNC delivered exceptional stability and durability after 20 cycles in alkaline organic solutions, significantly superior to single‐atom Fe–N–C without Fe NPs. Bench‐scale testing with continuous CO 2 absorption and desorption presented a 19.5% increase of CO 2 capture efficiency and a 40.7% decrease of heat duty with only 0.1 wt.% dosage of Fe/Fe SA @GNC. The role of Fe–N–C sites is demonstrated in the process of proton transfer and C−N breaking during solvent regeneration (CO 2 desorption). Thus, the Fe/Fe SA @GNC catalytic carbamate decomposition offered an appealing technology solution to the high heat duty challenge associated with CO 2 chemisorption using amine‐based solvent.