Direct nitrogen fixation by air oxidation catalyzed based on magnetic rotating sliding arc plasma

doi:10.3785/j.issn.1008-973X.2022.06.019

Journal of ZheJiang University (Engineering Science)

2022, Vol. 56

Issue (6): 1206-1211 DOI: 10.3785/j.issn.1008-973X.2022.06.019

Direct nitrogen fixation by air oxidation catalyzed based on magnetic rotating sliding arc plasma

Xing-jie LV(

),Hang CHEN,Ang-jian WU*(

),Xiao-dong LI

State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, China

Download:

HTML

PDF(2096KB) HTML
Export: BibTeX | EndNote (RIS)

Abstract

Three kinds of MoO₃/Al₂O₃ catalysts with different mass fractions (5%, 7.5% and 10%) were prepared by impregnation method using activated alumina (γ-Al₂O₃) as the carrier, and they were used for the research of plasma-catalyzed air oxidation and nitrogen fixation. In order to investigate the structural differences of catalysts with different mass fractions, the physical properties of the catalysts were characterized by XRD, SEM, and TEM. It was found that the catalyst structure was stable and distributed uniformly, which was beneficial to the catalytic experiment. The prepared MoO₃/Al₂O₃ catalyst was used to carry out a magnetically rotating gliding arc plasma-coupled catalytic air nitrogen fixation experiment, and experiment results showed that the catalyst had a promoting effect on nitrogen fixation. Under the optimal conditions, the output rate of ${{\text{NO}}_{{x}}}^{{-}}$ reached up to 1.17 mmol/min. Compared with the highest nitrogen fixation efficiency of 985 μmol/min in similar studies, it was slightly improved.

Key words： magnetic rotating sliding arc MoO₃/Al₂O₃ catalysts plasma coupling catalysis air oxidation nitrogen fixation plasma activated water

Received: 23 July 2021 Published: 30 June 2022

CLC:

TK 01+9

Fund: 国家自然科学基金资助项目（51976191，51806193）

Corresponding Authors: Ang-jian WU E-mail: 1293702293@qq.com;wuaj@zju.edu.cn

	Service
	E-mail this article
	Add to my bookshelf
	Add to citation manager
	E-mail Alert
	RSS
	Articles by authors
	Xing-jie LV
	Hang CHEN
	Ang-jian WU
	Xiao-dong LI

Cite this article:

Xing-jie LV,Hang CHEN,Ang-jian WU,Xiao-dong LI. Direct nitrogen fixation by air oxidation catalyzed based on magnetic rotating sliding arc plasma. Journal of ZheJiang University (Engineering Science), 2022, 56(6): 1206-1211.

URL:

https://www.zjujournals.com/eng/10.3785/j.issn.1008-973X.2022.06.019 OR https://www.zjujournals.com/eng/Y2022/V56/I6/1206

基于磁旋滑动弧等离子体催化的空气直接氧化固氮

以活性氧化铝（γ-Al₂O₃）为载体通过浸渍法制备不同质量分数（5%、7.5%和10%）的MoO₃/Al₂O₃催化剂，并进行等离子体催化空气的氧化固氮研究. 为了考察不同质量分数催化剂的结构差异，分别采用XRD、SEM和TEM表征催化剂的物理性质，结果表明催化剂结构稳定、分布均匀，有利于催化实验. 利用制备的MoO₃/Al₂O₃催化剂进行磁旋滑动弧等离子体耦合催化空气固氮实验，结果表明制备催化剂对固氮有促进作用，在最佳工况下， ${ {\text{NO}}_{{x}}}^{{-}}$的产出速率最高为1.17 mmol/min，相比同类研究中最高固氮效率 985 μmol /min有些许提升.

关键词： 磁旋滑动弧, MoO₃/Al₂O₃催化剂, 等离子体耦合催化, 空气氧化固氮, 等离子体活化水

Fig.1 Magnetic rotating sliding arc coupling catalytic experiment system

Fig.2 Schematic diagram of catalytic bed layout

Fig.3 XRD patterns of MoO₃/Al₂O₃ with different mass fractions

Fig.4 MoO₃/Al₂O₃ SEM of 5% mass fraction

Fig.5 MoO₃/Al₂O₃ TEM of 10% mass fraction

Fig.6

${{\mathrm{N}\mathrm{O}}_{x}}^{-}$

concentration in plasma activated water under different experimental conditions

Fig.7 Effect of plasma coupled catalytic nitrogen fixation with different mass fractions of MoO₃/Al₂O₃

Fig.8

${{\mathrm{N}\mathrm{O}}_{x}}^{-}$

concentration in plasma activated water and gas absorption bottle under different catalytic conditions


[1]	CHERKASOV N, IBHADON A O, FITZPATRICK P A review of the existing and alternative methods for greener nitrogen fixation[J]. Chemical Engineering and Processing: Process Intensification, 2015, 90: 24- 33 doi: 10.1016/j.cep.2015.02.004

[2]	CHEN J G, CROOKS R M, SEEFELDT L C, et al Beyond fossil fuel–driven nitrogen transformations[J]. Science, 2018, 360 (6391): eaar6611 doi: 10.1126/science.aar6611

[3]	ZHANG L, JI X Q, REN X, et al Efficient electrochemical N2 reduction to NH3 on MoN nanosheets array under ambient conditions [J]. ACS Sustainable Chemistry and Engineering, 2018, 6: 9550- 9554 doi: 10.1021/acssuschemeng.8b01438

[4]	LI R G Photocatalytic nitrogen fixation: an attractive approach for artificial photocatalysis[J]. Chinese Journal of Catalysis, 2018, 39: 1180- 1188 doi: 10.1016/S1872-2067(18)63104-3

[5]	HALBLEIB C M, LUDDEN P W Regulation of biological nitrogen fixation[J]. The Journal of Nutrition, 2000, 130 (5): 1081- 1084 doi: 10.1093/jn/130.5.1081

[6]	IWAMOTO M, AKIYAMA M, AIHARA K, et al Ammonia synthesis on wool-like Au, Pt, Pd, Ag, or Cu electrode catalysts in nonthermal atmospheric-pressure plasma of N2 and H2[J]. ACS Catalysis, 2017, 7 (10): 6924- 6929 doi: 10.1021/acscatal.7b01624

[7]	FRIDMAN A. Plasma Chemistry [M]. New York: Cambridge University Press, 2008: 848–857.

[8]	WANG W, PATIL B, HEIJKERS S, et al Nitrogen fixation by gliding arc plasma: better insight by chemical kinetics modelling[J]. ChemSusChem, 2017, 10 (10): 2145- 2157 doi: 10.1002/cssc.201700095

[9]	GALLAGHER M J, GEIGER R, POLEVICH A, et al On-board plasma-assisted conversion of heavy hydrocarbons into synthesis gas[J]. Fuel, 2010, 89 (6): 1187- 1192 doi: 10.1016/j.fuel.2009.11.039

[10]	PATIL B S, CHERKASOV N, LANG J, et al Low temperature plasma-catalytic NOx synthesis in a packed DBD reactor: effect of support materials and supported active metal oxides [J]. Applied Catalysis B: Environmental, 2016, 194: 123- 133 doi: 10.1016/j.apcatb.2016.04.055

[11]	HAN J R, JI X Q, REN X, et al MoO3 nanosheets for efficient electrocatalytic N2 fixation to NH3[J]. Journal of Materials Chemistry A, 2018, 6 (27): 12974- 12977 doi: 10.1039/C8TA03974G

[12]	KUMAR S, SINGH A, SINGH R, et al Facile h-MoO3 synthesis for NH3 gas sensing application at moderate operating temperature [J]. Sensors and Actuators B: Chemical, 2020, 325: 128974 doi: 10.1016/j.snb.2020.128974

[13]	WU H Y, LI X, CHENG Y, et al Plasmon-driven N2 photofixation in pure water over MoO3-x nanosheets under visible to NIR excitation [J]. Journal of Materials Chemistry A, 2020, 8 (5): 2827- 2835 doi: 10.1039/C9TA13038A

[14]	MUTEL B, DESSAUX O, GOUDMAND P Energy cost improvement of the nitrogen oxides synthesis in a low pressure plasma[J]. Revue de Physique Appliquée, 1984, 19 (6): 461- 464

[15]	LU W J, LU G Z, LUO Y, et al A novel preparation method of ZnO/MCM-41 for hydrogenation of methyl benzoate[J]. Journal of Molecular Catalysis A Chemical, 2002, 188: 225- 231 doi: 10.1016/S1381-1169(02)00335-7

[16]	BARAZZOUK S, TANDON R P, HOTCHANDANI S MoO3-based sensor for NO, NO2 and CH4 detection [J]. Sensors and Actuators B: Chemical, 2006, 119 (2): 691- 694 doi: 10.1016/j.snb.2006.01.026

[17]	YANG J, LI T Y, ZHONG C S, et al Nitrogen fixation in water using air phase gliding arc plasma[J]. Journal of The Electrochemical Society, 2016, 163 (10): E288- E292 doi: 10.1149/2.0221610jes

[18]	PENG P, CHEN P, ADDY M, et al In situ plasma-assisted atmospheric nitrogen fixation using water and spray-type jet plasma[J]. Chemical Communications, 2018, 54 (23): 2886- 2889 doi: 10.1039/C8CC00697K

[19]	PENG P, SCHIAPPACASSE C, ZHOU N, et al Plasma in situ gas–liquid nitrogen fixation using concentrated high-intensity electric field[J]. Journal of Physics D: Applied Physics, 2019, 52: 494001 doi: 10.1088/1361-6463/ab3ea6

No related articles found!

Viewed

Full text

Abstract

Cited

Shared

Discussed