Degradation of organic dyes by nanosecond pulsed discharge plasma
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摘要: 随着印染行业的快速发展，印染废水的排放与日俱增。由于废水中的有机物具有成分复杂、难以降解的特点，若未经有效处理直接排放，会对生态环境造成严重的污染和危害。试验设计了一种多针-网式反应器循环处理有机组分为酸性红73（AR73）的模拟废水，其采用自行设计的基于TLT（Transmission Line Transformer）的高压重频纳秒脉冲电源驱动。电源可以产生峰值电压为50 kV，脉宽40 ns，上升沿20 ns的纳秒脉冲信号，工作频率可达500 Hz。试验考察了峰值电压、放电频率、染料初始质量浓度及作用时间等因素对AR73降解效果的影响。为评价处理效果，采用紫外分光光度法分别测量了废水中剩余染料浓度、过氧化氢浓度等指标。结果表明，在初始浓度30 mg/L，循环流量3.4 L/min，放电间距30 mm，峰值电压44.26 kV，放电频率200 Hz条件下处理30 min，AR73降解率可以达到83.20%，单次脉冲注入能量为11.73 mJ，过氧化氢浓度为47.36 μmol/L，反应器脱色能效（G50）可以达到31.07 g·kW−1·h−1。增大放电电压可以进一步提高AR73降解率，溶液中活性物质浓度提高，但是能量效率有所下降。Abstract: Organic compounds (especially dyes compounds) are major pollutants in the industrial wastewater and have gained a great concern due to their hazardous influence on the environment and mankind’s health. A multiple pin-plane type pulsed corona discharge reactor was used to degrade Brilliant Crocein(Acid Red 73, AR73) continuously. The reactor was energized by a repetitive TLT based nanosecond pulsed power source. The source can produce pulses with a peak voltage of 50 kV, a pulse width of 40 ns, and a risetime of 20 ns at a repetition rate of up to 500 Hz. To evaluate the discharge performance, residual dye concentration and hydrogen peroxide (H2O2) were analyzed by UV spectrophotometry. The high voltage of 44.26 kV amplitude and frequency of 200 Hz were applied to the needles while wastewater film was used as the ground electrode. When the initial concentration of AR73 was 30 mg/L and the flow rate was 3.4 L/min, the degradation percentage of AR73 could reach up to 83.20% after 30 minutes of treatment with the needle-water distance of 30 mm. Under this condition, the input energy per pulse was 11.73 mJ, the concentration of H2O2 was up to 47.36 μmol/L, and the energy yield for 50% dye removal was 31.07 g·kW−1·h−1. Increasing the discharge voltage could further increase the degradation rate of AR73, and the active species generation in the solution was enhanced, but the energy efficiency decreased.
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Key words:
- nanosecond pulsed /
- corona discharge /
- non-thermal plasma /
- dye degradation /
- advanced oxidation
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图 1 电晕放电试验装置示意图
Figure 1. Schematic diagram of the corona discharge reactor experimental setup
图 6 不同交流输入下储能电容电压和放电峰值电压
Figure 6. Charging voltage and peak voltage with different AC input
图 7 不同放电电压下酸性红73降解率随时间的变化曲线
Figure 7. Evolution of AR73 degradation efficiency with treatment time under various discharge voltages
图 8 不同放电电压下过氧化氢浓度随时间的变化曲线
Figure 8. Evolution of H2O2 concentration with treatment time under various discharge voltages
图 9 不同放电电压下AR73降解率随能量密度变化曲线
Figure 9. Effects of Esi on degradation of AR73 under various discharge voltages
图 10 不同放电频率下酸性红73降解率随时间的变化曲线
Figure 10. Evolution of AR73 degradation efficiency with treatment time under various discharge frequencies
图 11 不同频率下的单次脉冲能量
Figure 11. Relation between energy per pulse and with discharge frequency
图 12 不同放电频率下过氧化氢浓度随时间的变化曲线
Figure 12. Evolution of H2O2 concentration with treatment time under various discharge frequencies
图 13 不同放电频率下AR73降解率随能量密度变化曲线
Figure 13. Effects of Esi on degradation of AR73 under various discharge frequencies
图 14 不同初始质量浓度下酸性红73降解率随时间的变化曲线
Figure 14. Effects of initial concentration on the degradation of AR73 with treatment time
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