This study focuses on the applicability of single-atom Mo-doped graphitic carbon nitride (GCN) nanosheets which are specifically engineered with high surface area (exfoliated GCN), NH
2 rich edges, and maximum utilization of isolated atomic Mo for propylene carbonate (PC) production through CO
2 cycloaddition of propylene oxide (PO). Various operational parameters are optimized, for example, temperature (130 °C), pressure (20 bar), catalyst (Mo
2GCN), and catalyst mass (0.1 g). Under optimal conditions, 2% Mo-doped GCN (Mo
2GCN) has the highest catalytic performance, especially the turnover frequency (TOF) obtained, 36.4 h
−1 is higher than most reported studies. DFT simulations prove the catalytic performance of Mo
2GCN significantly decreases the activation energy barrier for PO ring-opening from 50–60 to 4.903 kcal mol
−1. Coexistence of Lewis acid/base group improves the CO
2 cycloaddition performance by the formation of coordination bond between electron-deficient Mo atom with O atom of PO, while NH
2 surface group disrupts the stability of CO
2 bond by donating electrons into its low-level empty orbital. Steady-state process simulation of the industrial-scale consumes 4.4 ton h
−1 of CO
2 with PC production of 10.2 ton h
−1. Techno-economic assessment profit from Mo
2GCN is estimated to be 60.39 million USD year
−1 at a catalyst loss rate of 0.01 wt% h
−1.
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