NO<sub><i>x</i></sub> removal by non-thermal plasma reduction: experimental and theoretical investigations

doi:10.1007/s11705-022-2165-z

Front. Chem. Sci. Eng.

2022, Vol. 16

Issue (10) : 1476-1484 https://doi.org/10.1007/s11705-022-2165-z

RESEARCH ARTICLE

NO_x removal by non-thermal plasma reduction: experimental and theoretical investigations

Yue Liu^1,², Ji-Wei Wang^1,², Jian Zhang³, Ting-Ting Qi^1,², Guang-Wen Chu^1,²(

), Hai-Kui Zou^1,², Bao-Chang Sun^1,²(

)

¹. State Key Laboratory of Organic–Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China
². Research Center of the Ministry of Education for High Gravity Engineering and Technology, Beijing University of Chemical Technology, Beijing 100029, China
³. Daqing Refining & Chemical Company, PetroChina Co., Ltd., Daqing 163411, China

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Abstract

Green and efficient $N O x$ removal at low temperature is still desired. $N O x$ removal via non-thermal plasma (NTP) reduction is one of such technique. This work presents the experimental and theoretical study on the $N O x$ removal via NTP reduction (NTPRD) in dielectric barrier discharge reactor (DBD). The effect of $O 2$ molar fraction on $N O x$ species in the outlet of DBD, and effects of $N H 3$ /NO molar ratio and discharge power of DBD on $N O x$ removal efficiency are investigated. Results indicate that anaerobic condition and higher discharge power is beneficial to direct removal of $N O x$ , and the $N O x$ removal efficiency can be up to 98.5% under the optimal operating conditions. It is also found that adding $N H 3$ is favorable for the reduction of $N O x$ to $N 2$ at lower discharge power. In addition, the $N O x$ removal mechanism and energy consumption analysis for the NTPRD process are also studied. It is found that the reduced active species ( $N ∗$ , $N −$ , N⁺, $N 2 ∗$ , $N H 2 +$ , etc.) generated in the NTPRD process play important roles for the reduction of $N O x$ to $N 2$ . Our work paves a novel pathway for $N O x$ removal from anaerobic gas in industrial application.

Keywords _x removal NTP reduction mechanism energy consumption

Corresponding Author(s): Guang-Wen Chu,Bao-Chang Sun

About author:

Tongcan Cui and Yizhe Hou contributed equally to this work.

Online First Date: 27 June 2022 Issue Date: 17 October 2022

Cite this article:

Yue Liu,Ji-Wei Wang,Jian Zhang, et al. NO_x removal by non-thermal plasma reduction: experimental and theoretical investigations[J]. Front. Chem. Sci. Eng., 2022, 16(10): 1476-1484.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-022-2165-z
https://academic.hep.com.cn/fcse/EN/Y2022/V16/I10/1476

Fig.1 Schematic diagram of the DBD.

Fig.2 Experimental setup for the NTPRD process.

Fig.3 Outlet

N O x

molar fractions change with O₂ molar fraction.

Fig.4

N O x

removal efficiency changed with the NH₃/NO molar ratio.

Fig.5

N O x

removal efficiency changed with discharge power.

Fig.6 Transformation diagram and major species in NTPRD process.

Tab.1 Equations generating free radicals and their

G

values (in N₂) [35–37] ^a)

Species	$G A i ∗$ /(molecules·100 eV^–1)	$C A i ∗$ /(molecules·cm^–3)
N₂^*	0.290	2.43 × 10¹³
N^* (²D)	0.885	7.42 × 10¹³
N^* (²P)	0.295	2.47 × 10¹³
N^* (⁴S)	1.18	9.89 × 10¹³
N₂⁺	2.27	1.90 × 10¹⁴
N⁺ + N	0.690	5.78 × 10¹³
NH	0.700	2.54 ×10¹¹
NH₂	5.40	1.96× 10¹²
O(³P) + O(¹D)	1.82	1.15 × 10¹³
O₂^*	0.077	4.88 × 10¹¹
O(³P) + O^*	0.180	1.14 × 10¹²
O(³P) + O⁺ + e	0.800	5.07 × 10¹²
O(¹D) + O⁺ + e	0.430	2.73 × 10¹²
O₂⁺ + e	2.07	1.31× 10¹³

Tab.2

G A i ∗

and

C A i ∗

values of free radicals (aerobic condition)

Species	$G A i ∗$ /(molecules·100 eV^–1)	$C A i ∗$ /(molecules·cm^–3)
N₂^*	0.290	2.61 × 10¹³
N^*(²D)	0.885	7.98 × 10¹³
N^*(²P)	0.295	2.66 × 10¹³
N^*(⁴S)	1.18	1.06 × 10¹⁴
N₂⁺	2.27	2.05 × 10¹⁴
N⁺ + N	0.690	6.22 × 10¹³
NH	0.700	2.54 × 10¹¹
NH₂	5.40	1.96 × 10¹²

Tab.3

G A i ∗

and

C A i ∗

values of free radicals (anaerobic condition)

Tab.4 Main reactions and corresponding k_i in NO transformation

No.	Main reaction	k_i/(cm³·s^–1)	$C A i ∗$ /(mol·cm^–3)	R_i/(mol·s^–1·cm^–3)	S_i
1	N⁺ + NO — NO⁺ + N	4.10 × 10^–10	9.60 × 10^–11	1.41 × 10^–27	0.2696
2	N⁺ + NO — N₂⁺ + O	5.00 × 10^–11	9.60 × 10^–11	1.71 × 10^–28	0.0329
3	O₂⁺ + NO — NO⁺ + O₂	3.50 × 10^–10	2.18 × 10^–11	2.72 × 10^–28	0.0522
4	NO + O⁺ — NO⁺ + O	1.00 × 10^–12	1.30 × 10^–11	4.63 × 10^–31	0.0001
5	N₂^* + NO — N₂ + NO	1.50 × 10^–10	4.04 × 10^–11	2.16 × 10^–28	0.0415
6	N^* + NO — N₂ + O	7.00 × 10^–11	3.28 × 10^–10	8.21 × 10^–28	0.1574
7	NO + N — N₂ + O	3.25 × 10^–11	9.60 × 10^–11	1.11 × 10^–28	0.0214
8	NO + NH₂ — N₂ + H₂O	1.40 × 10^–11	3.25 × 10^–12	1.62 × 10^–30	0.0003
9	NO + NH₂ — N₂H + OH	5.15 × 10^–11	3.25 × 10^–12	5.98 × 10^–30	0.0011
10	NO + NH — N₂ + OH	5.15 × 10^–11	4.21 × 10^–13	7.75 × 10^–31	0.0001
11	NO + O — NO₂	1.00 × 10^–31	2.95 × 10^–11	1.05 × 10^–49	0.0000
12	O^* + NO — N + O₂	1.70 × 10^–10	2.56 × 10^–11	1.55 × 10^–28	0.0298
13	N^* + O₂ — NO + O	2.00 × 10^–12	3.28 × 10^–10	2.05 × 10^–28	0.3936

Tab.5 R_i and S_i of the NO reactions (aerobic condition)

No.	Main reaction	k_i/(cm³·s^–1)	$C A i ∗$ /(mol·cm^–3)	R_i/(mol·s^–1·cm^–3)	S_i
1	N⁺ + NO — NO⁺ + N	4.10 × 10^–10	1.03 × 10^–10	1.51 × 10^–27	0.5143
2	N^* + NO — N₂⁺ + O	7.00 × 10^–11	3.53 × 10^–10	8.83 × 10^–28	0.3003
3	N₂^* + NO — N₂ + NO	1.50 × 10^–10	4.34 × 10^–11	2.33 × 10^–28	0.0791
4	N⁺ + NO — N₂⁺ + O	5.00 × 10^–11	1.03 × 10^–10	1.84 × 10^–28	0.0627
5	NO + N — N₂ + O	3.25 × 10^–11	1.03 × 10^–10	1.20 × 10^–28	0.0408
6	NO + NH₂ — N₂H + OH	5.15 × 10^–11	3.25 × 10^–12	5.98 × 10^–30	0.0020
7	NO + NH₂ — N₂ + H₂O	1.40 × 10^–11	3.25 × 10^–12	1.62 × 10^–30	0.0006
8	NO + NH — N₂ + OH	5.15 × 10^–11	4.21 × 10^–13	7.75 × 10^–31	0.0003

Tab.6 R_i and S_i of the NO reactions (anaerobic condition)

Fig.7 (a) Effect of O₂ molar fraction on energy efficiency; (b) effect of NH₃/NO molar ratio on energy efficiency; (c) effect of discharge power on energy efficiency.

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