用于催化 CO2 循环加成的具有集成钼原子的碎片 g-C3N4 框架上高度暴露的 ?NH2 边缘：DFT 和技术经济评估,Small

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用于催化 CO2 循环加成的具有集成钼原子的碎片 g-C3N4 框架上高度暴露的 ?NH2 边缘：DFT 和技术经济评估
Small ( IF 13.0 ) Pub Date : 2022-11-20 , DOI: 10.1002/smll.202204336
Kien Tiek Wong _{1,

2} , Boris Brigljević _{3,

4} , Jeong Hyeon Lee ₃ , So Yeon Yoon _{1,

2} , Seok Byum Jang _{1,

2} , Choe Earn Choong _{1,

2} , Inwook Nah ₅ , Hyeongjun Kim ₃ , Hyun-Seog Roh ₆ , Sang Kyu Kwak _{3,

7} , Hankwon Lim ₃ , Min Jang _{1,

2}

Affiliation

本研究的重点是单原子 Mo 掺杂石墨碳氮化物 (GCN) 纳米片的适用性，这些纳米片经过专门设计，具有高表面积（剥离的 GCN）、 NH ₂丰富的边缘，以及分离原子 Mo 对碳酸亚丙酯的最大利用（ PC) 通过环氧丙烷 (PO) 的CO _{2环加成生产。}优化了各种操作参数，例如温度 (130 °C)、压力 (20 bar)、催化剂 (Mo ₂ GCN) 和催化剂质量 (0.1 g)。在最佳条件下，2% Mo 掺杂的 GCN (Mo ₂ GCN) 具有最高的催化性能，尤其是获得的转换频率 (TOF)，为 36.4 h ^-1高于大多数报道的研究。DFT 模拟证明，Mo ₂ GCN 的催化性能显着降低了 PO 开环的活化能势垒，从 50–60 降低到 4.903 kcal mol ^-1。路易斯酸/碱基团的共存通过在缺电子的Mo原子与PO的O原子之间形成配位键来提高CO _{2环加成性能，而}NH ₂表面基团通过将电子提供给其低位来破坏CO 2 键的_稳定性级空轨道。工业规模的稳态过程模拟消耗 4.4 ton h ⁻¹的 CO ₂和 PC 生产 10.2 ton h ⁻¹. 在催化剂损失率为 0.01 wt% h ^{-1时，来自 Mo}₂ GCN 的技术经济评估利润估计为 6039 万美元年^-1。

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Highly Exposed ?NH2 Edge on Fragmented g-C3N4 Framework with Integrated Molybdenum Atoms for Catalytic CO2 Cycloaddition: DFT and Techno-Economic Assessment

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), NH₂ rich edges, and maximum utilization of isolated atomic Mo for propylene carbonate (PC) production through CO₂ cycloaddition of propylene oxide (PO). Various operational parameters are optimized, for example, temperature (130 °C), pressure (20 bar), catalyst (Mo₂GCN), and catalyst mass (0.1 g). Under optimal conditions, 2% Mo-doped GCN (Mo₂GCN) 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 Mo₂GCN 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 CO₂ cycloaddition performance by the formation of coordination bond between electron-deficient Mo atom with O atom of PO, while NH₂ surface group disrupts the stability of CO₂ 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 CO₂ with PC production of 10.2 ton h⁻¹. Techno-economic assessment profit from Mo₂GCN is estimated to be 60.39 million USD year⁻¹ at a catalyst loss rate of 0.01 wt% h⁻¹.

更新日期：2022-11-20

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