Reductive Degradation of N⁃Nitrosodimethylamine in Water by Ultraviolet Advanced Reduction Processes

doi:10.19894/j.issn.1000-0518.210159

Chinese Journal of Applied Chemistry ›› 2022, Vol. 39 ›› Issue (3): 451-460.DOI: 10.19894/j.issn.1000-0518.210159

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Reductive Degradation of N⁃Nitrosodimethylamine in Water by Ultraviolet Advanced Reduction Processes

Xiao-Song ZHA¹^,²(), Lin ZHANG¹^,², Yuan-Jie WENG¹^,², Zhi-Liang FENG¹^,², Su-Wen JIN¹^,²

^1.School of Environmental Science and Engineering，Tan KahKee College，Xiamen University，Zhangzhou 363105，China
^2.Key Laboratory of Estuarine Ecological Security and Environmental Health of Fujian Province，Zhangzhou 363105，China

Received:2021-03-31 Accepted:2021-08-18 Published:2022-03-01 Online:2022-03-15
Contact: Xiao-Song ZHA
About author:xszha@xujc.com
Supported by:
the Natural Science Foundation of Fujian Province of China(2020J05017);the Natural Science Foundation of Zhangzhou City(ZZ2019J11)

Abstract

Abstract:

Two ultraviolet advanced reduction processes （UV/Na₂SO₃ and UV/Na₂S₂O₄） were used to reductively degrade N-nitrosodimethylamine （NDMA） in water and the effects of pH， light intensity， reductant dosage and dissolved oxygen on the removal efficiency of NDMA were investigated in this study. Moreover， the apparent kinetic constants under different reaction conditions were calculated and the reductive degradation mechanisms of NDMA by advanced reduction processes were inferred. The results show that the weak acid condition is favorable for the reductive degradation of NDMA by both UV/Na₂SO₃ and UV/Na₂S₂O₄ advanced reduction processes. Increasing the light intensity can significantly promote the reductive degradation of NDMA by both advanced reduction processes， while increasing the reductant dosage has little influence on the reductive degradation of NDMA. The removal efficiency of NDMA reaches 94.4% after 60 minutes of reaction when the light intensity is 8.7×10^-11 E/s， pH=6.76， and the Na₂SO₃ dosage is 10 mg/L. Dissolved oxygen can react with free reducing radicals， thus inhibit the reductive degradation of NDMA by advanced reduction processes. There are three possible reaction pathways for the reductive degradation of NDMA by advanced reduction processes： photohydrolysis， photolimination and photooxidation.

Key words: Ultraviolet advanced reduction processes, N-Nitrosodimethylamine, Reductive degradation

CLC Number:

O644.1

Xiao-Song ZHA, Lin ZHANG, Yuan-Jie WENG, Zhi-Liang FENG, Su-Wen JIN. Reductive Degradation of N⁃Nitrosodimethylamine in Water by Ultraviolet Advanced Reduction Processes[J]. Chinese Journal of Applied Chemistry, 2022, 39(3): 451-460.

Figures/Tables 9

Fig.1 The relationship between the absorbance of I3- and the reaction time

Fig.2 Comparison of the removal efficiency of NDMA in water by UV degradation and two ARPs （Initial reaction conditions： pH=6.2， ρ（DO）=7.85 mg/L， I0=7.56×10-11 E/s）

Fig.3 Effect of pH on removal of NDMA by ARPs： A.Na2S2O4 as reductant， B.Na2SO3 as reductant.（Initial reaction conditions： ρ（DO）=7.64 mg/L， I0=7.56×10-11 E/s， the dosage of reductant was 10 mg/L）

Fig.4 Effect of light intensity on removal of NDMA by ARPs： A.Na2S2O4 as reductant， B.Na2SO3 as reductant.（Initial reaction conditions： pH=6.76， ρ（DO）=7.94 mg/L， the dosage of reductant is 10 mg/L）

Fig.5 Effect of DO on removal of NDMA by ARPs： A. No reductant， B. Na2S2O4 as reductant， C. Na2SO3 as reductant. （Initial reaction conditions： pH=7.2， I0=7.56×10-11 E/s， the dosage of reductant is 10 mg/L）

Fig.6 Effect of the dosage of reductant on removal of NDMA by ARPs： A.Na2S2O4 as reductant， B.Na2SO3 as reductant.（Initial reaction conditions： pH=6.76， I0=7.56×10-11 E/s， ρ（DO）=7.81 mg/L）

Table 1 Kinetic equation of NDMA degradation by UV/Na2S2O4 and UV/Na2SO3 at different pH

pH值

pH value

动力学方程

Kinetic equation

表观速率常数

Observed rate constant/min^-1

R²

1.16

ln （ρ₀/ρ）=0.0142t+0.2538

ln （ρ₀/ρ）=0.0099t+0.2403

0.014 2

0.009 9

0.989 9

0.980 9

3.94

ln （ρ₀/ρ）=0.0188t+0.2146

ln （ρ₀/ρ）=0.0122t+0.1935

0.018 8

0.012 2

0.993 5

0.992 3

6.2

ln （ρ₀/ρ）=0.011t+0.2535

ln （ρ₀/ρ）=0.0079t+0.2449

0.011

0.007 9

0.998 7

0.976 7

9.72

ln （ρ₀/ρ）=0.0058t+0.3097

ln （ρ₀/ρ）=0.0085t+0.1779

0.005 8

0.008 5

0.979 3

0.977 5

12.25

ln （ρ₀/ρ）=0.0102t+0.1644

ln （ρ₀/ρ）=0.0108t+0.0753

0.010 2

0.010 8

0.972 3

0.980 4

Table 2 Kinetic equation of NDMA degradation by UV/Na2S2O4 and UV/Na2SO3 at different light intensity

光照强度

Intensity of illumination/（E·s^-1）

动力学方程

Kinetic equation

表观速率常数

Observed rate constant/min^-1

R²

1.12×10^-11

ln （ρ₀/ρ）=0.0054t+0.2259

ln （ρ₀/ρ）=0.0048t+0.156

0.005 4

0.004 8

0.978 5

0.949 5

7.56×10^-11

ln （ρ₀/ρ）=0.0112t+0.2273

ln （ρ₀/ρ）=0.009t+0.2406

0.011 2

0.009

0.958 8

0.911 6

8.70×10^-11

ln （ρ₀/ρ）=0.0425t+0.1639

ln （ρ₀/ρ）=0.0457t+0.0052

0.042 5

0.045 7

0.997 1

0.986 6

Table 3 Kinetic equation of NDMA degradation by UV/Na2S2O4 and UV/Na2SO3 at different DO

DO含量

ρ（DO）/（mg·L^-1）

动力学方程

Kinetic equation

表观速率常数

Observed rate constant/min^-1

8.05

ln （ρ₀/ρ）=0.0044t+0.2613

ln （ρ₀/ρ）=0.0026t+0.1299

0.004 4

0.002 6

0.968 8

0.997 4

0.85

ln （ρ₀/ρ）=0.007t+0.2483

ln （ρ₀/ρ）=0.0049t+0.1277

0.007

0.004 9

0.976 1

0.991 7

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Reductive Degradation of N⁃Nitrosodimethylamine in Water by Ultraviolet Advanced Reduction Processes

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