Fu-li Sun¹, Cun-biao Lin¹, Wei Zhang¹, Qing Chen², Wen-xian Chen¹, Xiao-nian Li¹, Gui-lin Zhuang^1*

1 H-PSI Computational Chemistry Lab, Institute of Industrial Catalysis, State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P.R. China.

2 Surface Lab 10, Institute of Physics, Chinese Academy of Sciences, P.R. China.

* Corresponding authors emails: glzhuang@zjut.edu.cn

DOI10.24435/materialscloud:hd-qb [version v1]

Publication date: Nov 20, 2023

How to cite this record

Fu-li Sun, Cun-biao Lin, Wei Zhang, Qing Chen, Wen-xian Chen, Xiao-nian Li, Gui-lin Zhuang, Dual activation and C-C coupling on single atom catalyst for CO₂ photoreduction, Materials Cloud Archive 2023.178 (2023), https://doi.org/10.24435/materialscloud:hd-qb

Description

An excellent single-atomic photocatalyst, Ti@C₄N₃, is theoretically found to effectively convert CO₂ to C₂H₆ by density functional theory (DFT) calculations and non-adiabatic molecular dynamics (NAMD) simulations. The Ti@C₄N₃ photocatalyst has remarkable stability both thermally, chemically, and mechanically. Electronically, it has strong absorption properties, suitable band positions, and a long photogenerated electron lifetime, allowing photogenerated electrons to migrate to the surface. Notably, the high-valence active site effectively activates two CO₂ through dual activation: Under light irradiation, the weakly adsorbed CO₂ undergoes photo-induced activation by the photoelectron of conduction band minimum (CBM); without light, the high Lewis acidity of the Ti site induces CO₂ activation through back-donating π-bond. Contrast simulation results uncovered that dual activation of CO₂ is attributed to the thermal and photonic synergy. Furthermore, two activated CO₂ species under light easily couple to form oxalate with the barrier of 0.19 eV, and further reduced to C₂H₆ with a low activation energy of 1.09 eV.

Materials Cloud sections using this data

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All-date.zip MD5md5:502f23474c9762a3fac9254166199035	21.9 MiB	This file contains material structure data and analysis data. For a more detailed introduction, please refer to README.txt.
README.txt MD5md5:fc9f1d2a7807a96f498c52800793eb80	1.3 KiB	README file explaining the contents of all others.

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External references

Keywords

dual activation CO2 photoreduction single-atom catalyst C-C coupling