Citation: Wenyi Bian, Xueli Shen, Huang Tan, Xing Fan, Yunxia Liu, Haiping Lin, Youyong Li. The triggering of catalysis via structural engineering at atomic level: Direct propane dehydrogenation on Fe-N₃P-C[J]. Chinese Chemical Letters, ;2023, 34(3): 107289. doi: 10.1016/j.cclet.2022.03.012 shu

The triggering of catalysis via structural engineering at atomic level: Direct propane dehydrogenation on Fe-N₃P-C

Wenyi Bian ^{a, 1} ,
Xueli Shen ^{a, 1} ,
Huang Tan ^b ,
Xing Fan ^a ,
Yunxia Liu ^a ,
Haiping Lin ^{b, *,} ,
Youyong Li ^{a, c, *,}

a.
Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou 215123, China
b.
School of Physics and Information Technology, Shaanxi Normal University, Xi'an 710062, China
c.
Macao Institute of Materials Science and Engineering, Macau University of Science and Technology, Macau, China

hplin@snnu.edu.cn

yyli@suda.edu.cn

Received Date: 23 January 2022
Revised Date: 23 February 2022
Accepted Date: 3 March 2022
Available Online: 7 March 2022

Figures(6)

The on-purpose direct propane dehydrogenation (PDH) has received extensive attention to meet the ever-increasing demand of propylene. In this work, by means of density functional theory (DFT) calculations, we systematically studied the intrinsic coordinating effect of Fe single-atom catalysts in PDH. Interestingly, the N and P dual-coordinated single Fe (Fe-N₃P-C) significantly outperform the Fe-N₄C site in catalysis and exhibit desired activity and selectivity at industrial PDH temperatures. The mechanistic origin of different performance on Fe-N₃P-C and Fe-N₄C has been ascribed to the geometric effect. To be specific, the in-plane configuration of Fe-N₄ site exhibits low H affinity, which results in poor activity in CH bond activations. By contrast, the out-of-plane structure of Fe-N₃P-C site exhibits moderate H affinity, which not only promote the CH bond scission but also offer a platform for obtaining appropriate H diffusion rate which ensures the high selectivity of propylene and the regeneration of catalysts. This work demonstrates promising applications of dual-coordinated single-atom catalysts for highly selective propane dehydrogenation.
- Non-oxidative propane dehydrogenation,
- Propylene selectivity,
- Single-atom catalysis,
- Heteroatom-doped graphene,
- Fe catalyst
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The triggering of catalysis via structural engineering at atomic level: Direct propane dehydrogenation on Fe-N3P-C

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The triggering of catalysis via structural engineering at atomic level: Direct propane dehydrogenation on Fe-N₃P-C