Elucidation of photodegradation of p-chlorophenol in a biophotoelectric reductive degradation system by density functional theory calculations

Elucidation of photodegradation of p-chlorophenol in a biophotoelectric reductive degradation system by density functional theory calculations
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通过密度泛函理论计算阐明生物光电还原降解系统中对氯苯酚的光降解

DOI:
10.1016/j.ibiod.2020.104969
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发表时间:
2020-07
影响因子:
4.8
通讯作者:
Xiao Xiang
Xiao Xiang
中科院分区:
环境科学与生态学2区
文献类型:
--
作者:
Liu Peng-Cheng;Ma Xiao-Lin;Li Ting-Ting;Yan Feng;Wu Li-Jun;Xiao Xiang

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半导体厌氧光催化是修复易还原难降解污染物的一种很有前途的方法。为了维持光还原的运行,必须提供空穴清除剂。细菌作为洞穴清道夫已经引起了人们的极大关注。因此,将纳米Ag3PO4与单胞菌MR-1复合,建立了生物光电还原降解体系(BPRDS)。通过降解对氯苯酚(p-CP)来评价BPRDS的光降解性能。结果表明,在厌氧光激发条件下,p-CP可被BPRDS降解,但不能被Shewanellacells或纳米Ag3PO4降解。阻断细胞外电子传递OFS。单胞菌MR-1能抑制BPRDS对EP-CP的降解,表明生物电子参与了厌氧光降解过程。核黄素剂量显著降低光降解效率。密度泛函理论计算表明,生物电子释放的是Ys。一株MR-1可以转移到纳米Ag3PO4的光生空穴中,发挥生物空穴清除剂的作用。空穴和羟基自由基清除剂不能阻止p-CP在BPRDS中的降解,这意味着p-CP是通过光还原而不是光氧化来去除的。结果表明,EAB可以作为厌氧光降解污染物的生物空穴清除剂,为BPRDS在环境修复中的应用奠定了基础。
Anaerobic photocatalysis of semiconductors is a promising approach for the remediation of refractory pollutants which are readily reduced rather than oxidized. To sustain the operation of photoreduction, hole scavengers must be supplied. Bacteria as hole scavengers have attracted great attention. Thus, a bio-photoelectric reductive degradation system (BPRDS) was established by integrating nano-Ag3PO4andShewanella oneidensisMR-1. Photodegradation performance of BPRDS was evaluated via degradingp-chlorophenol (p-CP). Results showed thatp-CP could be degraded by BPRDS under anaerobic photoexcitation conditions, but not be decomposed byShewanellacells or nano-Ag3PO4. Block of extracellular electron transfer ofS. oneidensisMR-1 could reducep-CP degradation in BPRDS, implying bio-electrons were involved in anaerobic photodegradation process. Dose of riboflavin decreased the photodegradation efficiency significantly. DFT calculations revealed that bio-electrons released byS. oneidensisMR-1 could be transferred to photogenerated holes of nano-Ag3PO4to exert biological hole scavengers. Hole and hydroxyl radical scavengers could not prevent degradation ofp-CP in BPRDS, implyingp-CP was removed via photoreduction rather than photooxidation. Our results demonstrate that EAB can act as biological hole scavengers for anaerobic photodegradation of pollutants, which will contribute to the application of BPRDS for environmental remediation.
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发表时间: 2016-02
影响因子: 9.9
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