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. 2022 Sep 7;27(18):5790.
doi: 10.3390/molecules27185790.

Al-Decorated C2N Monolayer as a Potential Catalyst for NO Reduction with CO Molecules: A DFT Investigation

Xinmiao Liu  1 , Yunjie Xu  1 , Li Sheng  1
Affiliations

Al-Decorated C2N Monolayer as a Potential Catalyst for NO Reduction with CO Molecules: A DFT Investigation

Xinmiao Liu et al. Molecules. .

Abstract

Developing efficient and economical catalysts for NO reduction is of great interest. Herein, the catalytic reduction of NO molecules on an Al-decorated C2N monolayer (Al-C2N) is systematically investigated using density functional theory (DFT) calculations. Our results reveal that the Al-C2N catalyst is highly selective for NO, more so than CO, according to the values of the adsorption energy and charge transfer. The NO reduction reaction more preferably undergoes the (NO)2 dimer reduction process instead of the NO direct decomposition process. For the (NO)2 dimer reduction process, two NO molecules initially co-adsorb to form (NO)2 dimers, followed by decomposition into N2O and Oads species. On this basis, five kinds of (NO)2 dimer structures that initiate four reaction paths are explored on the Al-C2N surface. Particularly, the cis-(NO)2 dimer structures (Dcis-N and Dcis-O) are crucial intermediates for NO reduction, where the max energy barrier along the energetically most favorable pathway (path II) is as low as 3.6 kcal/mol. The remaining Oads species on Al-C2N are then easily reduced with CO molecules, being beneficial for a new catalytic cycle. These results, combined with its low-cost nature, render Al-C2N a promising catalyst for NO reduction under mild conditions.

Keywords: Al-C2N catalyst; C2N monolayer; DFT calculation; NO catalytic reduction; nitric oxide.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
Optimized structures of the (a) pristine C2N cluster and (b) Al-C2N monolayer, respectively. Electron density difference plots (in 0.002 au) for (c) pristine C2N and (d) Al-C2N, respectively. Blue and yellow parts represent charge accumulation and depletion, respectively. All bond lengths are in Å.
Figure 2
Figure 2
Optimized adsorption configurations for the (a) NO (N-end), (b) NO (O-end), (c) CO, (d) ring-(NO)2 dimers, (e) cis-(NO)2 dimers (N-end), (f) cis-(NO)2 dimers (O-end), (g) trans-(NO)2 dimers (N-end), and (h) trans-(NO)2 dimers (O-end) on Al-C2N surface. All bond lengths are in Å.
Figure 3
Figure 3
The energy profile and corresponding structure for the NO direct decomposition process on Al-C2N. All bond lengths are in Å.
Figure 4
Figure 4
The energy profile and corresponding structure of the Dring dimer reduction process on Al-C2N; (a) (NO)2 → N2O + Oads (path Ia), (b) (NO)2 + CO → N2 + CO2 + Oads (path Ib). All bond lengths are in Å.
Figure 5
Figure 5
The energy profiles and corresponding structures of the Dcis-N and Dcis-O dimer reduction process on Al-C2N. All bond lengths are in Å.
Figure 6
Figure 6
The energy profiles and corresponding structures of the (a) Dtrans-N and (b) Dtrans-O dimer reduction process on Al-C2N. All bond lengths are in Å.
Figure 7
Figure 7
The energy profiles and corresponding structures for the step of (a) Oads + NO → NO2 and (b) Oads + CO → CO2 on Al-C2N, respectively. All bond lengths are in Å.
See this image and copyright information in PMC

References

    1. Liu Z.S., Yu F., Ma C.H., Dan J.M., Luo J., Dai B. A Critical Review of Recent Progress and Perspective in Practical Denitration Application. Catalysts. 2019;9:771. doi: 10.3390/catal9090771. - DOI
    1. Seitzinger S.P., Phillips L. Nitrogen stewardship in the Anthropocene. Science. 2017;357:350–351. doi: 10.1126/science.aao0812. - DOI - PubMed
    1. Janssens T.V.W., Vennestrom P.N.R. A molecular dance to cleaner air. Science. 2017;357:866–867. doi: 10.1126/science.aao2442. - DOI - PubMed
    1. Gholami Z., Luo G.H., Gholami F., Yang F. Recent advances in selective catalytic reduction of NOx by carbon monoxide for flue gas cleaning process: A review. Catal. Rev.-Sci. Eng. 2021;63:68–119. doi: 10.1080/01614940.2020.1753972. - DOI
    1. Toyao T., Jing Y., Kon K., Hayama T., Nagaoka S., Shimizu K.-i. Catalytic NO–CO Reactions over La-Al2O3 Supported Pd: Promotion Effect of La. Chem. Lett. 2018;47:1036–1039. doi: 10.1246/cl.180388. - DOI

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