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

doi:10.1007/s11705-022-2165-z

Frontiers of Chemical Science and Engineering

2022, Vol. 16

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

本期目录

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

全文: PDF(11004 KB) HTML

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.

Key words： _x removal NTP reduction mechanism energy consumption

收稿日期: 2021-10-06 出版日期: 2022-10-17

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

引用本文:

. [J]. Frontiers of Chemical Science and Engineering, 2022, 16(10): 1476-1484.
Yue Liu, Ji-Wei Wang, Jian Zhang, Ting-Ting Qi, Guang-Wen Chu, Hai-Kui Zou, Bao-Chang Sun. NO_x removal by non-thermal plasma reduction: experimental and theoretical investigations. Front. Chem. Sci. Eng., 2022, 16(10): 1476-1484.

链接本文:

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

Fig.1

Fig.2

Fig.3

Fig.4

Fig.5

Fig.6

Tab.1

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

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

Tab.4

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

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

Fig.7

1	Q Yu, H Wang, T Liu, L Xiao, X Jiang, X Zheng. High-efficiency removal of NOx using a combined adsorption-discharge plasma catalytic process. Environmental Science & Technology, 2012, 46( 4): 2337– 2344 https://doi.org/10.1021/es203405c
2	I A Resitoglu, A Keskin. Hydrogen applications in selective catalytic reduction of NOx emissions from diesel engines. International Journal of Hydrogen Energy, 2017, 42( 36): 23389– 23394 https://doi.org/10.1016/j.ijhydene.2017.02.011
3	F Gholami, M Tomas, Z Gholami, M Vakili. Technologies for the nitrogen oxides reduction from flue gas: a review. Science of the Total Environment, 2020, 714 : 136712.1– 136712.26
4	P Talebizadeh, M Babaie, R Brown, H Rahimzadeh, Z Ristovski, M Arai. The role of non-thermal plasma technique in NOx treatment: a review. Renewable & Sustainable Energy Reviews, 2014, 40 : 886– 901 https://doi.org/10.1016/j.rser.2014.07.194
5	C Liang, Y Cai, K Li, Y Luo, Z Qian, G W Chu, J F Chen. Using dielectric barrier discharge and rotating packed bed reactor for NOx removal. Separation and Purification Technology, 2020, 235 : 116141 https://doi.org/10.1016/j.seppur.2019.116141
6	R F Ilmasani, J W Woo, D Creaser, L Olsson. Influencing the NOx stability by metal oxide addition to Pd/BEA for passive NOx adsorbers. Industrial & Engineering Chemistry Research, 2020, 59( 21): 9830– 9840 https://doi.org/10.1021/acs.iecr.9b06976
7	R K Srivastava, R E Hall, S Khan, K Culligan, B W Lani. Nitrogen oxides emission control options for coal-fired electric utility boilers. Journal of the Air & Waste Management Association, 2005, 55( 9): 1367– 1388 https://doi.org/10.1080/10473289.2005.10464736
8	D Li, X Tang, H H Yi, D Ma, F Gao. NOx removal over modified carbon molecular sieve catalysts using a combined adsorption-discharge plasma catalytic process. Industrial & Engineering Chemistry Research, 2015, 54( 37): 9097– 9103 https://doi.org/10.1021/acs.iecr.5b01672
9	C Zhang, Y Gao, Q Yan, Q Wang. Fundamental investigation on layered double hydroxides derived mixed metal oxides for selective catalytic reduction of NOx by H2. Catalysis Today, 2020, 355 : 450– 457 https://doi.org/10.1016/j.cattod.2019.07.006
10	M Seneque, F Can, D Duprez, X Courtois. NOx selective catalytic reduction (NOx-SCR) by urea: evidence of the reactivity of HNCO, including a specific reaction pathway for NOx reduction involving NO + NO2. ACS Catalysis, 2016, 6( 7): 4064– 4067 https://doi.org/10.1021/acscatal.6b00785
11	S M Ma, Y C Zhao, J P Yang, S B Zhang, J Y Zhang, C G Zheng. Research progress of pollutants removal from coal-fired flue gas using non-thermal plasma. Renewable & Sustainable Energy Reviews, 2017, 67 : 791– 810 https://doi.org/10.1016/j.rser.2016.09.066
12	A M Harling, D J Glover, J C Whitehead, K Zhang. Novel method for enhancing the destruction of environmental pollutants by the combination of multiple plasma discharges. Environmental Science & Technology, 2008, 42( 12): 4546– 4550 https://doi.org/10.1021/es703213p
13	L W Chen, Y D Meng, J Shen, X S Shu, S D Fang, X Y Xiong. Coal pyrolysis to acetylene using dc hydrogen plasma torch: effects of system variables on acetylene concentration. Journal of Physics. D, Applied Physics, 2009, 42( 5): 055505 https://doi.org/10.1088/0022-3727/42/5/055505
14	J Ma, B G Su, G D Wen, Q L Ren, Y W Yang, Q W Yang, H B Xing. Kinetic modeling and experimental validation of the pyrolysis of propane in hydrogen plasma. International Journal of Hydrogen Energy, 2016, 41( 48): 22689– 22697 https://doi.org/10.1016/j.ijhydene.2016.09.044
15	B Wang, X Wang, B Zhang. Dielectric barrier micro-plasma reactor with segmented outer electrode for decomposition of pure CO2. Frontiers of Chemical Science and Engineering, 2021, 15( 3): 687– 697 https://doi.org/10.1007/s11705-020-1974-1
16	Y K Kwon, D H Han. Microwave effect in the simultaneous removal of NOx and SO2 under electron beam irradiation and kinetic investigation of NOx removal rate. Industrial & Engineering Chemistry Research, 2010, 49( 17): 8147– 8156 https://doi.org/10.1021/ie100570q
17	J H Park, J W Ahn, K H Kim, Y S Son. Historic and futuristic review of electron beam technology for the treatment of SO2 and NOx in flue gas. Chemical Engineering Journal, 2019, 355 : 351– 366 https://doi.org/10.1016/j.cej.2018.08.103
18	J S Chang, S Masuda. Mechanism of pulse corona induced plasma chemical process for removal of NOx and SO2 from combustion gases. In IEEE Industry Applications Society Meeting, 1988, 2 : 1628– 1635
19	Y H Lee, J W Chung, Y R Choi, J S Chung, M H Cho, W Namkung. NOx removal characteristics in plasma plus catalyst hybrid process. Plasma Chemistry and Plasma Processing, 2004, 24( 2): 137– 154 https://doi.org/10.1023/B:PCPP.0000013195.87201.4a
20	G B Zhao, S V B Garikipati, X D Hu, M D Argyle, M Radosz. Effect of reactor configuration on nitric oxide conversion in nitrogen plasma. AIChE Journal, 2005, 51( 6): 1813– 1821 https://doi.org/10.1002/aic.10451
21	M R Khani, E Barzideh Pour, S Rashnoo, X Tu, B Ghobadian, B Shokri, A Khadem, S I Hosseini. Real diesel engine exhaust emission control: indirect non-thermal plasma and comparison to direct plasma for NOx, THC, CO, and CO2. Journal of Environmental Health Science & Engineering, 2020, 18( 2): 743– 754 https://doi.org/10.1007/s40201-020-00500-0
22	H Pan, Y Qiang. Promotion of non-thermal plasma on catalytic reduction of NOx by C3H8 over Co/BEA catalyst at low temperature. Plasma Chemistry and Plasma Processing, 2014, 34( 4): 811– 824 https://doi.org/10.1007/s11090-014-9522-8
23	G Yu, Z Yan, D Ye, X L Wang, P Gu, Y Q Xu. A Study on the NO removal mechanism through the plasma reaction of NO/N2 system. Journal of Engineering Thermophysics, 2003, 24( 02): 354– 356
24	C E Stere, W Adress, R Burch, S Chansai, A Goguet, W G Graham, F De Rosa, V Palma, C Hardacre. Ambient temperature hydrocarbon selective catalytic reduction of NOx using atmospheric pressure nonthermal plasma activation of a Ag/Al2O3 catalyst. ACS Catalysis, 2014, 4( 2): 666– 673 https://doi.org/10.1021/cs4009286
25	H Wang, Y Y Cao, Z W Chen, Q Q Yu, S J Wu. High-efficiency removal of NOx over natural mordenite using an enhanced plasma-catalytic process at ambient temperature. Fuel, 2018, 224 : 323– 330 https://doi.org/10.1016/j.fuel.2018.03.065
26	X L Gong, R Zhao, J Q Qin, H M Wang, D Wang. Ultra-efficient removal of NO in a MOFs-NTP synergistic process at ambient temperature. Chemical Engineering Journal, 2019, 358 : 291– 298 https://doi.org/10.1016/j.cej.2018.09.222
27	B M Penetrante, M C Hsiao, B T Merritt, G E Vogtlin, P H Wallman. Comparison of electrical discharge techniques for nonthermal plasma processing of NO in N2. IEEE Transactions on Plasma Science, 1995, 23( 4): 679– 687 https://doi.org/10.1109/27.467990
28	H Mätzing. Chemical kinetics of flue gas cleaning by irradiation with electrons. Advances in Chemical Physics, 2007, 80 : 315– 402 https://doi.org/10.1002/9780470141298.ch4
29	C Willis, A W Boyd. Excitation in the radiation chemistry of inorganic gases. International Journal for Radiation Physics and Chemistry, 1976, 8( 1-2): 71– 111 https://doi.org/10.1016/0020-7055(76)90061-9
30	J J Lowke, R Morrow. Theoretical analysis of removal of oxides of sulphur and nitrogen in pulsed operation of electrostatic precipitators. IEEE Transactions on Plasma Science, 1995, 23( 4): 661– 671 https://doi.org/10.1109/27.467988
31	C Willis, A W Boyd, M J Young, D A Armstrong. Radiation chemistry of gaseous oxygen: experimental and calculated yields. Canadian Journal of Chemistry, 1970, 48( 10): 1505– 1514 https://doi.org/10.1139/v70-246
32	B M Penetrante, M C Hsiao, B T Merritt, G E Vogtlin, P H Wallman, A Kuthi, C P Burkhart, J R Bayless. Electron-impact dissociation of molecular nitrogen in atmospheric-pressure nonthermal plasma reactors. Applied Physics Letters, 1995, 67( 21): 3096– 3098 https://doi.org/10.1063/1.114876
33	J T Herron, D S Green. Chemical kinetics database and predictive schemes for nonthermal humid air plasma chemistry. Part II. Neutral species reactions. Plasma Chemistry and Plasma Processing, 2001, 21( 3): 459– 481 https://doi.org/10.1023/A:1011082611822
34	G B Zhao, X D Hu, M D Argyle, M N Radosz. Atom radicals and N2(A3∑u+) found to be responsible for nitrogen oxides conversion in nonthermal nitrogen plasma. Industrial & Engineering Chemistry Research, 2004, 43( 17): 5077– 5088 https://doi.org/10.1021/ie049795z
35	G Michalski, R Jost, D Sugny, M Joyeux, M Thiemens. Dissociation energies of six NO2 isotopologues by laser induced fluorescence spectroscopy and zero point energy of some triatomic molecules. Journal of Chemical Physics, 2004, 121( 15): 7153– 7161 https://doi.org/10.1063/1.1792233
36	X Tang, Y Hou, C Y Ng, B Ruscic. Pulsed field-ionization photoelectron-photoion coincidence study of the process N2 + hν → N+ + N + e–: bond dissociation energies of N2 and N2+. Journal of Chemical Physics, 2005, 123( 7): 074330 https://doi.org/10.1063/1.1995699
37	F Mansouri, A Khavanin, A J Jafari, H Asilian, H R Ghomi, S M Mousavi. Energy efficiency improvement in nitric oxide reduction by packed DBD plasma: optimization and modeling using response surface methodology (RSM). Environmental Science and Pollution Research International, 2020, 27( 14): 16100– 16109 https://doi.org/10.1007/s11356-020-07870-w
38	J S Chang, P C Looy, K Nagai, T Yoshioka, A Maezawa. Pilot plant tests of a corona discharge-electron beam hybrid combustion flue gas cleaning system. IEEE Transactions on Industry Applications, 1994, 21( 1): 131– 137
39	B M Penetrante, M C Hsiao, B T Merritt, G E Vogtlin, P H Wallman, M Neiger, O Wolf, T Hammer, S Broer. Pulsed corona and dielectric-barrier discharge processing of NO in N2. Applied Physics Letters, 1996, 68( 26): 3719– 3721 https://doi.org/10.1063/1.115984
40	Y S Mok, M N Chang, M H Cho, I S Nam. Decomposition of volatile organic compounds and nitric oxide by nonthermal plasma discharge processes. IEEE Transactions on Plasma Science, 2002, 30( 1): 408– 416 https://doi.org/10.1109/TPS.2002.1003889

Viewed

Full text

Abstract

Cited

Shared

Discussed