EFFECT OF TEMPERATURE ON BENZENE AND TOLUENE OXIDATION IN A BARRIER DISCHARGE
Abstract
The results on the influence of the temperature of the reactor walls on the direct single-stage oxidation of benzene and toluene in a plasma-chemical reactor with a barrier discharge are presented. The main products of benzene oxidation are phenols and dihydric phenols. During oxidation with toluene, cresols, benzaldehyde and benzyl alcohol are mainly formed. The conducted studies on the influence of the temperature of the reactor walls made it possible to establish the dependence on the main parameters of the oxidation of hydrocarbons in a barrier discharge. The conversion of benzene during oxidation with oxygen increases from 0.2 to 0.4% wt., during oxidation with air it changes from 0.4 to 0.6% wt. with an increase in the temperature of the reactor walls. The conversion of toluene during oxidation with oxygen increases from 1 to 3% wt., during oxidation with air it changes from 0.4 to 0.6% wt. with an increase in the temperature of the reactor walls. It has been established that with an increase in the temperature of the reactor walls in experiments on the oxidation of benzene with air, the content of phenol and pyrocatechol in the mixture practically does not change. An increase in the temperature of the reactor walls in the case of benzene oxidation with air leads to a decrease in the hydroquinone content in the mixture of reaction products, and in the case of benzene oxidation with oxygen, to an increase in the hydroquinone content. In experiments on the oxidation of toluene with air in a barrier discharge, the content of benzyl alcohol and cresols increases, while the content of benzoic aldehyde decreases. During the oxidation of toluene in air, the tendency to increase the content of benzyl alcohol, cresols, and decrease the content of benzyl aldehyde with an increase in the temperature of the reactor walls remains. Comparing our previous results on the oxidative conversion of benzene and the temperature effect in experiments on the oxidation of toluene in a barrier discharge, we can conclude that it is expedient to use temperature to control the process of one-stage oxidation of aromatic hydrocarbons in plasma.
For citation:
Leshchik A.V., Ochered'ko A.N., Ryabov A.Yu., Petrenko T.V., Kudryashov S.V. Effect of temperature on benzene and toluene oxidation in a barrier discharge. ChemChemTech [Izv. Vyssh. Uchebn. Zaved. Khim. Khim. Tekhnol.]. 2023. V. 66. N 11. P. 18-24. DOI: 10.6060/ivkkt.20236611.10t.
References
Wang B., Wang N., Sun Y., Xiao H., Fu M., Li Sh., Liang H., Qiao Zh., Ye D. Dielectric barrier discharge plasma modified Pt/CeO2 catalysts for toluene oxidation: Effect of discharge time. Appl. Surf. Sci. 2023. V. 614. P. 156162. DOI: 10.1016/j.apsusc.2022.156162.
Artemyev Yu.M., Artemyeva M.A., Li-sogurskaya O.F. Photocatalytic oxidation of toluene on niobium (V) oxide. Zhurn.Prikll. Khim. 1995. V. 68. N 6. P. 956-961 (in Russian).
Xu N., Fu W., He C. Benzene removal using non-thermal plasma with CuO/AC catalyst: reaction condition optimization and decomposition mechanism. Plasma Chem. Plasma Process. 2014. V. 34. N 6. P. 1387–1402. DOI: 10.1007/s11090-014-9580-y.
Kim H.H., Teramoto Y., Ogata A., Takagi H., Nanba T. Plasma Catalysis for Environmental Treatment and En-ergy Applications. Plasma Chem. Plasma Process. 2016. V. 36. P. 45–72. DOI: 10.1007/s11090-015-9652-7.
Teramoto Y., Kim H.H., Negishi N., Ogata A. The Role of Ozone in the Reaction Mechanism of a Bare Zeolite-Plasma Hybrid System. Catalysts. 2015. V. 5. N 2. P. 838-850. DOI: 10.3390/catal5020838.
Sekiguchi H., Ando M., Kojima H. Study of hydroxylation of benzene and toluene using a micro-DBD plasma reactor. J. Phys. D: Appl. Phys. 2005. V. 38. N 11. P. 1722. DOI: 10.1088/0022-3727/38/11/013.
Ascenzi D., Franceschi P., Guella G., Tosi P. Phenol production in benzene/air plasmas at atmospheric pres-sure. Role of radical and ionic routes. J. Phys. Chem. A. 2006. V. 110. N 25. P. 7841–7847. DOI: 10.1021/jp062406p.
Dey G.R., Sharma A., Pushpa K.K., Das T.N. Variable products in dielectric-barrier discharge assisted benzene oxidation. J. Hazard. Mater. 2010. V. 178. N 1–3. P. 693–698. DOI: 10.1016/j.jhazmat.2010.01.143.
Lee D.W., Lee J.H., Chun B.H., Lee K.Y. The Characteristics of direct hydroxylation of benzene to phenol with molecular oxygen enhanced by pulse DC corona at atmospheric pressure. Plasma Chem. Plasma Process. 2003. V. 23. N 3. P. 519–539. DOI: 10.1023/A:1023287016525.
Liu, Y.J., Jiang X.Z., Wang L. One-step hydroxylation of benzene to phenol induced by glow discharge plasma in an aqueous solution. Plasma Chem. Plasma Process. 2007. V. 27. N 4. P. 496–503. DOI: 10.1007/s11090-007-9059-1.
Najafpoor A.A., Jafari, A.J., Hosseinzadeh A., Jazani R.K., Bargozin H. Optimization of non-thermal plasma efficiency in the simultaneous elimination of benzene, toluene, ethyl-benzene, and xylene from polluted air-streams using response surface methodology. Environ. Sci. Pollut. Res. 2018. V. 25. N 1. P. 233–241. DOI: 10.1007/s11356-017-0373-8.
Li J., Bai S.P., Shi X.C., Han S.L., Zhu X.M., Chen W.C., Pu Y.K. Effects of temperature on benzene oxida-tion in dielectric barrier discharges. Plasma Chem. Plasma Process. 2008. V. 28. N 1. P. 39–48. DOI: 10.1007/s11090-007-9115-x.
Franceschi P., Guella G., Scarduelli G., Tosi P., Dilecce G., Benedictis S.D. Chemical processes in the atmospheric pressure plasma treatment of benzene. Plasma Process. Polym. 2007. V. 4. N 5. P. 548–555. DOI: 10.1002/ppap.200700004.
Ogata A., Shintani N., Yamanouchi K., Mizuno K., Kushiyama S., Yamamoto T. Effect of water vapor on benzene decomposition using a nonthermal-discharge plasma reactor. Plasma Chem. Plasma Process. 2000. V. 20. N 4. P. 453–467. DOI: 10.1023/A:1007075721610.
Shutov D.A., Ivanov A.N., Rybkin V.V., Manukyan A.S. Comparative study of the electrical and physical pa-rameters of glow discharge under water solutions of anionic and cationic surfactants. ChemChemTech [Izv. Vyssh. Uchebn. Zaved. Khim. Khim. Tekhnol.]. 2020. V. 63. N 2. P. 91-98 (in Russian). DOI: 10.6060/ivkkt.20206302.6194.
Ochered’ko A.N., Kudryashov S.V., Ryabov A.Yu., Leshchik A.V. Direct Oxidation of Benzene to Phenol in a Dielectric-Barrier Discharge Reactor. High Energy Chem. V. 56. N 4. P. 284–288. DOI: 10.1134/S0018143922040129.
Samoilovich V.G., Gibalov V.I., Kozlov K.V. Physical chemistry of a barrier discharge. M.: MGU. 1989. 174 p. (in Russian).
Cvetanovic R.J. Evaluated chemical kinetic data for the reactions of atomic oxygen O(3P) with unsaturated hy-drocarbons. J. Phys. Chem. Ref. Data. 1987. V. 16. P. 261–326. DOI: 10.1063/1.555783.
Nguyen T. L., Peeters J., Vereecken L. Theoretical reinvestigation of the O(3P)+C6H6 reaction: quantum chemical and statistical rate calculations. J. Phys. Chem. A. 2007. V. 111. N 19. P. 3836–3849. DOI: 10.1021/jp0660886.
Parker J.K., Davis S.R. Photochemical reactions of oxygen atoms with toluene, m -xylene, p -xylene, and mesitylene: an infrared matrix isolation investigation. J. Phys. Chem. A. 2000. V. 104. N 17. P. 4108–4114. DOI: 10.1021/jp992832t.
Kogelschatz U. Dielectric-barrier discharges: their history, discharge physics, and industrial applications. Plasma Chem. Plasma Process. 2003. V. 23. N 1. P. 1–46. DOI:10.1023/A:1022470901385.