方波脉冲电压提高光催化降解乙烯反应器性能
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国家自然科学基金项目(31171449)


Performance upgrade of reactor for ethylene photocatalytic degradation with pulsed direct current DC square-wave
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    摘要:

    为了解以活性炭纤维(activated carbon fiber,ACF)为载体负载Ag沉积TiO2的光电极膜材料((Ag+TiO2)/ACF)在方波脉冲电压(pulsed direct current DC square-wave,PDCSW)下光催化降解冷藏环境中乙烯的效率,该文以自行研制的乙烯反应器为研究对象,该反应器的电压源以数字信号处理器(digital signal processor,DSP)为核心,控制输出方波的幅值、占空比和频率等高精确参数值。试验对催化后的光电极膜材料进行X射线能谱分析(energy dispersive x-ray spectroscopy,EDS)表征,结果表明,方波脉冲作用后对光电极破坏较小,Ag的脱落情况不明显。试验展开直流电压源(direct-current power,DC)和方波脉冲电压源下光电催化降解乙烯效率的比较。结果表明,方波脉冲下乙烯降解速率常数K值2.296×10-4 min-1较直流下K值1.715×10-4 min-1更大,有较高的催化效率。研究了方波电压、占空比和频率对降解乙烯效率的影响,采用二次旋转组合试验和回归拟合,建立了乙烯降解速率常数(K)与参数关系的二次多项式数学模型,验证了模型的有效性,结果表明,随着方波电压不断增大,乙烯的降解速率呈现先增大后减小的趋势,占空比和频率对降解乙烯的影响呈现出与电压同样的变化趋势。利用数学模型找出最优参数组合,电压25.5 V,占空比23%,频率310 Hz,最优K值为0.0002783 min-1。该研究为方波脉冲电压辅助光催化技术的应用和进一步的研究提供科学依据。

    Abstract:

    Abstract: In the research, we designed a new-style reactor that included a digital signal controller as the core of voltage source for ethylene photocatalytic degradation, which could carefully control the parameters (voltage, duty cycle and frequency). Area external standard method was used to detect the ethylene content with the gas chromatograph flame ionization detector (GC-FID) every 30 min during the whole research. The photoelectrode film material, i.e. (silver+titanium dioxide)/activated carbon fiber ((Ag+TiO2)/ACF) was made by Ag particles adding, ultrasonication and 60Co-γ irradiation and so on. The (Ag+TiO2)/ACF photoelectrode under photoelectrocatalysis in the pulsed direct current square-wave (PDCSW) or direct current (DC) after 24 h were characterized by means of the energy diffraction spectrum (EDS). The characterization results showed that the Ag/Ti ratio sharply decreased from 1% to 0.24% after 24 hours' DC photoelectrocatalysis, while the ratio was 0.83% after 24 hours' PDCSW photoelectrocatalysis, and the latter exhibited higher activity than the former. The reason for the phenomenon was that the intermittent electric current could keep Ag particles close to the surface of TiO2 for a catalytic effective distance so as to provide a carrier accept electrons. The study compared the photocatalytic degradation efficiency of ethylene under 2 different conditions of PDCSW and DC photoelectrocatalysis, and the ethylene degradation efficiency was evaluated by the K value as the main index. The results showed that the K value of PDCSW was 2.296×10-4 min-1, which was obviously higher than that of DC, so the application of PDCSW to ethylene degradation efficiency would be of great significance. We tried to observe the variation tendency of the K value by adjusting these parameters (voltage, duty cycle and frequency) of pulse electric field in the PDC reactor system, and employed response surface methodology to analyze 3 single-factor experiments to find out the optimum assembly. The research adopted the method of quadratic rotation combination experiment and regression fitting to build up the quadratic multinomial mathematical model of the K value and the parameters, and verified the validity of the model. The 3 single-factor experiments showed that the K value increased at first and then decreased, and reached the maximum when the voltage was 20 V, the duty cycle was 20% and the frequency was 300 Hz. The degradation efficiency increased with the voltage changing from 0 to 20 V and decreased from 20 to 30 V, increased with the duty cycle changing from 0 to 20% and decreased from 20% to 80%, and increased with the frequency changing from 200 to 300 Hz and decreased from 300 to 400 Hz under the condition that the 2 other factors remained unchanged. Response surface analysis showed that the optimum assembly of the K value would achieve the highest efficiency when the voltage was 25.5 V, the duty cycle was 23% and the frequency was 310 Hz. The research can provide a basis for the application of pulsed direct current square-wave photocatalytic technology in the degradation of ethylene of fruit and vegetable in cold storage.

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崔晓雷,赵少杰,叶盛英,李利钦,李园.方波脉冲电压提高光催化降解乙烯反应器性能[J].农业工程学报,2015,31(18):289-295. DOI:10.11975/j. issn.1002-6819.2015.18.039

Cui Xiaolei, Zhao Shaojie, Ye Shengying, Li Liqin, Li Yuan. Performance upgrade of reactor for ethylene photocatalytic degradation with pulsed direct current DC square-wave[J]. Transactions of the Chinese Society of Agricultural Engineering (Transactions of the CSAE),2015,31(18):289-295. DOI:10.11975/j. issn.1002-6819.2015.18.039

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  • 收稿日期:2015-07-08
  • 最后修改日期:2015-08-03
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  • 在线发布日期: 2015-09-17
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