Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced by high gravity technology

doi:10.1007/s11705-020-1998-6

Front. Chem. Sci. Eng.

2021, Vol. 15

Issue (5) : 1197-1205 https://doi.org/10.1007/s11705-020-1998-6

RESEARCH ARTICLE

Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced by high gravity technology

Weizhou Jiao(

), Shengjuan Shao, Peizhen Yang, Kechang Gao, Youzhi Liu

Shanxi Province Key Laboratory of Higee-Oriented Chemical Engineering, National Demonstration Center for Experimental Comprehensive Chemical Engineering Education, North University of China, Taiyuan 030051, China

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Abstract

This study investigated the indirect oxidation of nitrobenzene (NB) by hydroxyl radicals (·OH) in a rotating packed bed (RPB) using competitive kinetics method with p-nitrochlorobenzene as a reference compound. The rate constants of NB with ·OH are calculated to be between (1.465±0.113) × 10⁹ L/(mol·s) and (2.497±0.192) × 10⁹ L/(mol·s). The experimental data are fitted by the modified Arrhenius equation, where the activation energy is 4877.74 J/mol, the order of NB concentration, rotation speed, and initial pH is 0.2425, 0.1400 and 0.0167, respectively. The ozonation process of NB could be enhanced by RPB, which is especially effective for highly concentrated NB-containing wastewater under alkaline conditions. The high gravity technology can accelerate ozone mass transfer and self-decomposition of ozone to produce more ·OH, resulting in an increase in the indirect oxidation rate of NB by ·OH and consequently effective degradation of NB in wastewater.

Keywords high gravity technology hydroxyl radicals nitrobenzene reaction kinetics

Corresponding Author(s): Weizhou Jiao

Just Accepted Date: 31 December 2020 Online First Date: 05 February 2021 Issue Date: 30 August 2021

Cite this article:

Weizhou Jiao,Shengjuan Shao,Peizhen Yang, et al. Kinetics and mechanism of nitrobenzene degradation by hydroxyl radicals-based ozonation process enhanced by high gravity technology[J]. Front. Chem. Sci. Eng., 2021, 15(5): 1197-1205.

URL:

https://academic.hep.com.cn/fcse/EN/10.1007/s11705-020-1998-6
https://academic.hep.com.cn/fcse/EN/Y2021/V15/I5/1197

Fig.1 Flow chart of the ozonation process in the RPB.

Fig.2 Effect of temperature on k_·OH,NB. pH= 11.0, N = 700 r/min, C_NB = C_p_-CNB = 200 mg/L,

C O 3

= 40 mg/L, V_L = 100 L/h, Q_G = 75 L/h; T = 293 K, k_·OH,NB = (1.898±0.145) × 10⁹ L/(mol·s), T = 313 K, k_·OH,NB = (2.184±0.168) × 10⁹ L/(mol·s); T = 333 K, k_·OH,NB = (2.385±0.183) × 10⁹ L/(mol·s).

Fig.3 Effect of initial solution pH on k_·OH,NB. T = 293 K, N = 700 r/min, C_NB = C_p_-CNB = 200 mg/L,

C O 3

= 40 mg/L, V_L = 100 L/h, Q_G = 75 L/h; pH= 7.0, k_·OH,NB = (1.465±0.113) × 10⁹ L/(mol·s), pH= 9.0, k_·OH,NB = (1.553±0.119) × 10⁹ L/(mol·s); pH= 11.0, k_·OH,NB = (1.857±0.143) × 10⁹ L/(mol·s), pH= 13.0, k_·OH,NB = (1.851±0.145) × 10⁹ L/(mol·s).

Fig.4 Effect of rotor speed on k_·OH,NB. T = 293 K, pH= 11.0, C_NB = C_p_-CNB = 200 mg/L,

C O 3

= 40 mg/L, V_L = 100 L/h, Q_G = 75 L/h; N = 300 r/min, k_·OH,NB = (1.713±0.132) × 10⁹ L/(mol·s), N = 500 r/min, k_·OH,NB = (1.802±0.139) × 10⁹ L/(mol·s); N = 700 r/min, k_·OH,NB = (1.898±0.145) × 10⁹ L/(mol·s), N = 900 r/min, k_·OH,NB = (1.915±0.148) × 10⁹ L/(mol·s).

Fig.5 Effect of initial NB concentration on k_·OH,NB. T = 293 K, pH= 11.0, N = 700 r/min,

C O 3

= 40 mg/L, V_L= 100 L/h, Q_G = 75 L/h; C_NB = C_p_-CNB = 100 mg/L, k_·OH,NB = (1.735±0.134) × 10⁹ L/(mol·s); C_NB = C_p_-CNB = 200 mg/L, k_·OH,NB = (1.898±0.145) × 10⁹ L/(mol·s); C_NB = C_p_-CNB = 300 mg/L, k_·OH,NB = (2.254±0.173) × 10⁹ L/(mol·s); C_NB = C_p_-CNB = 400 mg/L, k_·OH,NB = (2.395±0.184) × 10⁹ L/(mol·s); C_NB = C_p_-CNB = 500 mg/L, k_·OH,NB = (2.497±0.192) × 10⁹ L/(mol·s).

Fig.6 The curves of lnk_·OH,NB against 1/T and lnC_OH^–.

Fig.7 The curves of ln k_·OH,NB against ln N and ln C_NB.

Rate constant	Number	pH	Temperature/°C	Reference
$k O 3,?NB$ /(L?mol⁻¹?s⁻¹)
?(1.8±0.2)–(2.2±0.2)	1	2.0	10–20	Beltrán [13]
?0.09±0.02	2	2.0	21–25	Hoigné [14]
?0.732−5.261	3	1.0–7.0	20–60	This study
k_·OH,NB× 10^–9/(L?mol⁻¹?s⁻¹)
?2.2	4	10.5	22–25	Hoigné [41]
?0.82±0.3	5	10.5	18–25	Matthews [39]
?(1.465±0.113)–(2.497±0.192)	6	7.0–13.0	20–60	This study

Tab.1 Rate constants for direct and indirect reactions of NB with O₃ and ·OH

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