Promoting effect of Ti in the Ti-modified γ-Fe2O3 catalyst on its performance in the selective catalytic reduction of NO with ammonia, a DFT calculation study

ZHOU Wen-bo; NIU Sheng-li; WANG Dong; LU Chun-mei; HAN Kui-hua; LI Ying-jie; ZHU Ying

Volume 48 Issue 10

Oct. 2020

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Article Navigation > Journal of Fuel Chemistry and Technology > 2020 > 48(10): 1224-1235

ZHOU Wen-bo, NIU Sheng-li, WANG Dong, LU Chun-mei, HAN Kui-hua, LI Ying-jie, ZHU Ying. Promoting effect of Ti in the Ti-modified γ-Fe2O3 catalyst on its performance in the selective catalytic reduction of NO with ammonia, a DFT calculation study[J]. Journal of Fuel Chemistry and Technology, 2020, 48(10): 1224-1235.

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ZHOU Wen-bo, NIU Sheng-li, WANG Dong, LU Chun-mei, HAN Kui-hua, LI Ying-jie, ZHU Ying. Promoting effect of Ti in the Ti-modified γ-Fe₂O₃ catalyst on its performance in the selective catalytic reduction of NO with ammonia, a DFT calculation study[J]. Journal of Fuel Chemistry and Technology, 2020, 48(10): 1224-1235.

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Promoting effect of Ti in the Ti-modified γ-Fe₂O₃ catalyst on its performance in the selective catalytic reduction of NO with ammonia, a DFT calculation study

1.
School of Energy and Power Engineering, Shandong University, Jinan 250061, China
2.
Brook Byers Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA 30332, United States
3.
Advanced Materials Institute, Qilu University of Technology(Shandong Academy of Science), Jinan 250014, China

Funds:

The National Natural Science Foundation of China 51576117

The National Natural Science Foundation of China 21906090

Important Project in the Scientific Innovation of Shandong Province 2019JZZY020305

More Information

Corresponding author: NIU Sheng-li, E-mail:nsl@sdu.edu.cn
Received Date: 2020-08-26
Rev Recd Date: 2020-09-23

Available Online: 2021-01-23

Publish Date: 2020-10-10

Abstract

Abstract

The promoting effect of a typical transition metal Ti in the Ti-modified γ-Fe₂O₃ catalyst on its performance in the selective catalytic reduction (SCR) of NO with ammonia was investigated by density functional theory (DFT) calculation. Various doping models of single Ti and double Ti at different Fe sites on the γ-Fe₂O₃(001) surface were constructed; the surface doping formation energy was calculated, the adsorption characteristics of O₂, NO and NH₃ molecules on γ-Fe₂O₃ (001) surface before and after Ti doping were compared, and the reaction mechanism was analyzed. The results illustrate that single Ti atom tends to be doped at octahedral Feoct site, whereas two Ti atoms at two Feoct sites. The adsorption of O₂ onto the catalyst surface can be enhanced through the Ti doping; moreover, the enhancement increases with an increase in the doping content of Ti. Both single Ti and double Ti doping inhibit the N-terminal adsorption of NO on the catalyst surface. Ti can enhance the Lewis acid sites and promote the adsorption of NH₃, which is beneficial to SCR reaction. The doping of Ti increases the energy barrier of NO₂ formation and reduces the SCR reaction of γ-Fe₂O₃ at low temperature. The doping of Ti can inhibit the formation of NH and N, avoid the excessive oxidation of NH₃, and improve the utilization of NH₃, which are beneficial to the SCR reaction by suppressing the N₂O produced by the E-R mechanism and enhancing the selectivity to N₂. As a result, the Ti doping can significantly improve catalytic performance of γ-Fe₂O₃ in the NH₃-SCR of NO.
- NH₃-SCR,
- γ-Fe₂O₃,
- Ti doping,
- DFT

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References(37)

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