Optimization of Process Parameters for Ammonia Synthesis by Nanosecond Pulsed Dielectric Barrier Discharge Plasma

doi:10.19894/j.issn.1000-0518.220204

Chinese Journal of Applied Chemistry ›› 2023, Vol. 40 ›› Issue (2): 268-276.DOI: 10.19894/j.issn.1000-0518.220204

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Optimization of Process Parameters for Ammonia Synthesis by Nanosecond Pulsed Dielectric Barrier Discharge Plasma

Yang LIU, Hai-Bao ZHANG(), Qiang CHEN

Laboratory of Plasma Physics and Materials，Beijing Institute of Graphic Communication，Beijing 102600，China

Received:2022-06-08 Accepted:2022-10-12 Published:2023-02-01 Online:2023-02-27
Contact: Hai-Bao ZHANG
About author:hbzhang@bigc.edu.cn
Supported by:
the National Natural Science Foundation of China(11875090);Beijing Municipal National Science Foundation(1192008);Beijing Municipal Education Commission Project(KM202010015003)

Abstract

Abstract:

Ammonia （NH₃） as an important chemical raw material has a direct influence on the development of agriculture， national economy and people's livelihood. It is a high temperature， high pressure， high energy consumption and heavy pollution process in the industrial synthesis of ammonia. Low-temperature plasma technology is a sustainable and promising technology for ammonia synthesis， which has become a research hotspot at home and abroad. In this work， nitrogen and hydrogen are used as raw materials， and nanosecond pulsed dielectric barrier discharge is used to synthesize ammonia at low temperature and atmospheric pressure. The effects of factors such as pulse peak voltage， pulse repetition frequency， total gas flow rate， and N₂∶H₂ volume ratio on the synthesis rate and energy yield of ammonia synthesis are investigated systematically through a single-factor experiment. Furthermore， through the orthogonal experimental evaluation， it is determined that the order of factors affecting the synthesis rate is： pulse peak voltage>pulse repetition frequency>gas volume ratio>gas total flow rate. The order of factors affecting the energy yield is： pulse peak voltage>gas volume ratio>pulse repetition frequency>total gas flow rate. Combined with these two parts of experiments， the optimal conditions for ammonia synthesis are finally obtained： Pulse peak voltage 16 kV， pulse repetition frequency 6 kHz， pulse rising edge 100 ns， V（N₂）∶V（H₂）=1∶1， and total gas flow rate 200 mL/min. Under this condition， the highest NH₃ synthesis rate is up to 923.08 μmol/h and the energy yield is 0.30 g/kWh， respectively.

Key words: Ammonia synthesis, Plasma, Dielectric barrier discharge, Nanosecond pulsed discharge, Orthogonal experiment

CLC Number:

O646.9

Yang LIU, Hai-Bao ZHANG, Qiang CHEN. Optimization of Process Parameters for Ammonia Synthesis by Nanosecond Pulsed Dielectric Barrier Discharge Plasma[J]. Chinese Journal of Applied Chemistry, 2023, 40(2): 268-276.

Figures/Tables 11

References 42

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Horizontal factor	A	B	C	D
Horizontal factor	Peak voltage/ kV	Power frequency/ kHz	Total gas flow/ （mL·min^-1）	V（N₂）∶V（H₂）
1	8	2	200	1∶3
2	10	3	180	1∶2
3	12	4	160	1∶1
4	14	5	140	2∶1
5	16	6	120	3∶1

Horizontal factor	A	B	C	D
Horizontal factor	Peak voltage/ kV	Power frequency/ kHz	Total gas flow/ （mL·min^-1）	V（N₂）∶V（H₂）
1	8	2	200	1∶3
2	10	3	180	1∶2
3	12	4	160	1∶1
4	14	5	140	2∶1
5	16	6	120	3∶1

Experiment number	A	B	C	D	Ammonia synthesis rate/ （μmol·h^-1）	Energy yield/ （g?kWh^-1）
Experiment number	Peak voltage/kV	Power frequency/kHz	Total gas flow/（mL·min^-1）	V（N₂）∶V（H₂）	Ammonia synthesis rate/ （μmol·h^-1）	Energy yield/ （g?kWh^-1）
1	8	2	200	1∶3	135.75	0.28
2	8	3	160	2∶1	107.14	0.30
3	8	4	120	1∶2	190.48	0.36
4	8	5	180	3∶1	239.20	0.30
5	8	6	140	1∶1	350.88	0.28
6	10	2	120	2∶1	180.45	0.32
7	10	3	180	1∶2	272.73	0.23
8	10	4	140	3∶1	194.81	0.20
9	10	5	200	1∶1	483.22	0.30
10	10	6	160	1∶3	441.72	0.26
11	12	2	140	1∶2	221.13	0.26
12	12	3	200	3∶1	218.45	0.20
13	12	4	160	1∶1	442.26	0.29
14	12	5	120	1∶3	413.79	0.25
15	12	6	180	2∶1	545.45	0.26
16	14	2	160	3∶1	244.90	0.29
17	14	3	120	1∶1	371.13	0.38
18	14	4	180	1∶3	413.79	0.18
19	14	5	140	2∶1	383.80	0.13
20	14	6	200	1∶2	666.67	0.27
21	16	2	180	1∶1	423.53	0.26
22	16	3	140	1∶3	365.48	0.20
23	16	4	200	2∶1	456.85	0.20
24	16	5	160	1∶2	692.31	0.24
25	16	6	120	3∶1	264.71	0.09
NH₃ synthesis rate/（μmol·h^-1）
k₁	204.69	241.15	392.19	354.11
k₂	314.59	266.99	378.94	408.70
k₃	368.22	339.64	364.24	414.20
k₄	416.06	442.46	303.22	334.74
k₅	440.58	453.89	246.02	232.41
Range R₁	235.89	212.74	146.17	181.79
Order of factors	A＞B＞D＞C
Energy yield/（g?kWh^-1）
k₁	0.30	0.28	0.25	0.23
k₂	0.26	0.26	0.25	0.27
k₃	0.25	0.25	0.22	0.30
k₄	0.25	0.24	0.21	0.24
k₅	0.20	0.23	0.21	0.22
Range R₂	0.10	0.05	0.04	0.08
Order of factors	A＞D＞B＞C

Experiment number	A	B	C	D	Ammonia synthesis rate/ （μmol·h^-1）	Energy yield/ （g?kWh^-1）
Experiment number	Peak voltage/kV	Power frequency/kHz	Total gas flow/（mL·min^-1）	V（N₂）∶V（H₂）	Ammonia synthesis rate/ （μmol·h^-1）	Energy yield/ （g?kWh^-1）
1	8	2	200	1∶3	135.75	0.28
2	8	3	160	2∶1	107.14	0.30
3	8	4	120	1∶2	190.48	0.36
4	8	5	180	3∶1	239.20	0.30
5	8	6	140	1∶1	350.88	0.28
6	10	2	120	2∶1	180.45	0.32
7	10	3	180	1∶2	272.73	0.23
8	10	4	140	3∶1	194.81	0.20
9	10	5	200	1∶1	483.22	0.30
10	10	6	160	1∶3	441.72	0.26
11	12	2	140	1∶2	221.13	0.26
12	12	3	200	3∶1	218.45	0.20
13	12	4	160	1∶1	442.26	0.29
14	12	5	120	1∶3	413.79	0.25
15	12	6	180	2∶1	545.45	0.26
16	14	2	160	3∶1	244.90	0.29
17	14	3	120	1∶1	371.13	0.38
18	14	4	180	1∶3	413.79	0.18
19	14	5	140	2∶1	383.80	0.13
20	14	6	200	1∶2	666.67	0.27
21	16	2	180	1∶1	423.53	0.26
22	16	3	140	1∶3	365.48	0.20
23	16	4	200	2∶1	456.85	0.20
24	16	5	160	1∶2	692.31	0.24
25	16	6	120	3∶1	264.71	0.09
NH₃ synthesis rate/（μmol·h^-1）
k₁	204.69	241.15	392.19	354.11
k₂	314.59	266.99	378.94	408.70
k₃	368.22	339.64	364.24	414.20
k₄	416.06	442.46	303.22	334.74
k₅	440.58	453.89	246.02	232.41
Range R₁	235.89	212.74	146.17	181.79
Order of factors	A＞B＞D＞C
Energy yield/（g?kWh^-1）
k₁	0.30	0.28	0.25	0.23
k₂	0.26	0.26	0.25	0.27
k₃	0.25	0.25	0.22	0.30
k₄	0.25	0.24	0.21	0.24
k₅	0.20	0.23	0.21	0.22
Range R₂	0.10	0.05	0.04	0.08
Order of factors	A＞D＞B＞C

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Optimization of Process Parameters for Ammonia Synthesis by Nanosecond Pulsed Dielectric Barrier Discharge Plasma

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