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文献速递|华中农业大学WR:可见光照射下亚硫酸盐与腐植酸的活化对废水处理的新启示

  • 2026-02-07 16:32:35
文献速递|华中农业大学WR:可见光照射下亚硫酸盐与腐植酸的活化对废水处理的新启示
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第一作者:Yanting Pan

通讯作者:冯雄汉 教授

通讯单位:华中农业大学资源与环境学院

DOI:10.1016/j.watres.2024.121773

全文速览

亚硫酸盐(S(IV))作为过硫酸盐的替代品,已经证明了它的成本效益和环保特性,在高级氧化工艺(AOPs)中越来越受到关注。溶解有机物 (DOM) 常见于各种环境中,通常被视为亚硫酸盐高级氧化工艺的干扰因素。然而,人们较少关注受激发的 DOM 对亚硫酸盐活化的促进作用,而亚硫酸盐活化可能会产生各种反应中间产物。本研究重点研究了利用可见光(VL)激发腐植酸(HA)活化亚硫酸盐,以高效降解多种常见有机污染物,其效果优于过氧化二硫酸盐(PDS)和过氧化单硫酸盐(PMS)系统。淬灭实验和电子顺磁共振(EPR)分析表明,HA 的三重态(3HA*)通过能量转移激活亚硫酸盐,从而产生 SO4--、O2--和 1O2。在降解洛克沙砷(ROX)过程中发现的最重要的活性物种是 1O2,这是一种非辐射途径,对污染物降解具有高选择性。这种非辐射途径在基于亚硫酸盐的传统 AOP 中并不常见。此外,各种无机阴离子(如 NO3-、Cl-、SO42-、CO32- 和 PO43-)的共存对 ROX 的降解影响不大。此外,来自不同天然水体的 DOM 在光照条件下也能有效活化 S(IV),这为将亚硫酸盐高级氧化技术应用于不同地点和水体的有机污染修复提供了新的可能性。总之,这项研究为基于亚硫酸盐的 AOPs 的潜在应用提供了前景广阔的见解,在光激发 HA 的促进下,亚硫酸盐 AOPs 可作为一种新策略在各种环境中有效降解有机污染物。

图文摘要
引言

在本研究中,我们介绍了一种利用 VL 激发亚硫酸盐活化 HA 来降解有机污染物的新方法。通过淬灭试验和电子顺磁共振表征,我们确定了系统中的活性物种并提出了其潜在机制。同时,我们还系统地研究了操作参数和水成分对 ROX 降解的影响。为了进一步评估真实水体中溶解有机物对光活化的影响,我们在天然水中引入亚硫酸盐进行 ROX 降解实验。此外,为了有效利用亚硫酸盐,本研究选择了 CaSO3 作为 S(IV)的来源。 这有效地抑制了 ROS 和亚硫酸盐之间的不良反应。研究结果清楚地表明,VL 激发 HA 活化亚硫酸盐的创新技术在水污染处理中的应用前景十分广阔。

同位素标记技术
图文导读

Fig. 1The variation in ROX degradation percentage across different systems (a) and the corresponding pseudo-second-order kinetic fittings (b); the consumption kinetics of S(IV) across different systems (c); and the variation of dissolved oxygen in the S(IV)/HA/VL system (d). Experimental conditions: [S(IV)] = 1 mM, HA = 5 mg C/L, [ROX] = 5 mg/L, [initial pH] = 6.0 ± 0.05, T = 25 °C.

Fig. 2Effects of operating parameters on ROX degradation in S(IV)/HA/VL system. (a) initial pH; (b) S(IV) concentration; (c) HA concentration. Experimental conditions: [ROX] = 5 mg/L, [HA] = 1 – 10 mg C/L, [S(IV)] = 0.25 – 2 mM, [initial pH] = 3.0 – 9.0, T = 25 °C.

Fig. 3Effect of AN(a), TBA (b), EtOH (c), SOD (d), FFA (e) and NaN3 (f) on ROX degradation in the S(IV)/HA/VL system. Experimental conditions: [ROX] = 5 mg/L, [S(IV)] = 1 mM, [HA] = 5 mg C/L, [initial pH] = 6.0 ± 0.05, T = 25 °C.

Fig. 4DMPO (a) and TEMP (b) spin-trapping EPR spectra of HA /S(IV) /VL system. Experimental conditions: [S(IV)] = 1 mM, [HA] = 5 mg C/L, [initial pH] = 6.0 ± 0.05, T = 25 °C.

Fig. 5Effect of different atmospheric conditions (a) and TMP (b) on the oxidation of ROX. Experimental conditions: [ROX] = 5 mg/L, [S(IV)] = 1 mM, [HA] = 5 mg C/L, [initial pH] = 6.0 ± 0.05, T = 25 °C.

Fig. 6Effects of inorganic ions on ROX degradation (a) and the removal rate of ROX (b). Experimental conditions:(a) [ROX] = 5 mg/L, [S(IV)] = 1 mM, [HA] = 5 mg C/L, [initial pH] = 6.0 ± 0.05, inorganic ions = 5 mmol L−1T = 25 °C;(b) [ROX] = 5 mg/L, [S(IV)] = 1 mM, [HA] = 5 mg C/L, [initial pH] = 6.0 ± 0.05, inorganic ions = 0 - 20 mmol L1T = 25 °C.

研究意义

总之,本研究开发了一种使用 VL 激发的腐植酸(HA)作为亚硫酸盐活化剂来活化 S(IV)的创新方法。结果表明,在 S(IV)/VL 系统中加入 HA 能显著促进各种污染物的降解。虽然在反应过程中,HA 的浓度和芳香度逐渐降低,但在七次循环实验中,HA 也表现出了良好的活化效力可循环性。1O2 是光照 HA 活化 S(IV)体系中的主要活性物种,它是一种非自由基途径,具有很强的选择性,因此在降解过程中不易受到水基质的干扰。同时,CaSO3 的持续释放特性使基于 S(IV)的高级氧化过程对环境的适应性更强。天然水中的 DOM 在光照条件下也具有活化 S(IV)的强大能力,凸显了这种方法的广泛应用前景。鉴于自然环境中无处不在的光照 DOM,这项研究为原位水修复提供了一种前景广阔的技术。

文献信息

Yanting Pan, Feng Zhang, Wenfeng Tan, Xionghan Feng, New insight into wastewater treatment by activation of sulfite with humic acid under visible light irradiation, Water Research, 2024, https://doi.org/10.1016/j.watres.2024.121773

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  1. CONNECT:[ UseTime:0.000972s ] mysql:host=127.0.0.1;port=3306;dbname=h_mffb;charset=utf8mb4
  2. SHOW FULL COLUMNS FROM `fenlei` [ RunTime:0.001470s ]
  3. SELECT * FROM `fenlei` WHERE `fid` = 0 [ RunTime:0.002134s ]
  4. SELECT * FROM `fenlei` WHERE `fid` = 63 [ RunTime:0.000652s ]
  5. SHOW FULL COLUMNS FROM `set` [ RunTime:0.001299s ]
  6. SELECT * FROM `set` [ RunTime:0.000495s ]
  7. SHOW FULL COLUMNS FROM `article` [ RunTime:0.001513s ]
  8. SELECT * FROM `article` WHERE `id` = 467785 LIMIT 1 [ RunTime:0.001018s ]
  9. UPDATE `article` SET `lasttime` = 1770767585 WHERE `id` = 467785 [ RunTime:0.005565s ]
  10. SELECT * FROM `fenlei` WHERE `id` = 64 LIMIT 1 [ RunTime:0.005709s ]
  11. SELECT * FROM `article` WHERE `id` < 467785 ORDER BY `id` DESC LIMIT 1 [ RunTime:0.001196s ]
  12. SELECT * FROM `article` WHERE `id` > 467785 ORDER BY `id` ASC LIMIT 1 [ RunTime:0.003429s ]
  13. SELECT * FROM `article` WHERE `id` < 467785 ORDER BY `id` DESC LIMIT 10 [ RunTime:0.002291s ]
  14. SELECT * FROM `article` WHERE `id` < 467785 ORDER BY `id` DESC LIMIT 10,10 [ RunTime:0.001791s ]
  15. SELECT * FROM `article` WHERE `id` < 467785 ORDER BY `id` DESC LIMIT 20,10 [ RunTime:0.002212s ]
0.158342s