Enhanced adsorption and photocatalytic degradation of perfluorooctanoic acid in water using iron (hydr)oxides/carbon sphere composite

Enhanced adsorption and photocatalytic degradation of perfluorooctanoic acid in water using iron (hydr)oxides/carbon sphere composite
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使用铁(氢)氧化物/碳球复合材料增强吸附和光催化降解水中的全氟辛酸

DOI:
10.1016/j.cej.2020.124230
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发表时间:
2020-05
影响因子:
15.1
通讯作者:
Zhao Dongye
Zhao Dongye
中科院分区:
工程技术1区
文献类型:
--
作者:
Xu Tianyuan;Ji Haodong;Gu Yu;Tong Tianyi;Xia Yabei;Zhang Lizhi;Zhao Dongye

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全氟辛酸(PFOA)已在水生系统中被广泛检测到。然而,一直缺乏降解PFAS的具有成本效益的技术。采用一步水热法制备并测试了由氧化铁和碳球组成的吸附型光催化剂(FeO/CS)。表征结果表明,碳球的存在影响了铁(氢)氧化物的晶体形成,形成了水铁矿和碳球相互修饰的混合相。在模拟太阳光下,FeO/CS能够有效地吸附并降解PFOA。当Fe:Glucose摩尔比为1:1时,制备的FeO/CS(1:1)对PFOA的吸附容量和光催化活性最高。当投加量为1.0 g/L时,FeO/CS(1:1)在1 h内几乎完全吸附了200 µ g/L的PFOA;当负载PFOA的FeO/CS(1:1)在中性pH条件下接受模拟日光照射时,4h内95.2%的预浓缩PFOA被光降解,57.2%被脱氟。有效的降解也再生了材料,允许重复使用材料而无需化学再生。结果表明:1)CS促进了Fe2O3的形成,使PFOA通过双核和双齿络合作用吸附; 2)Fe2O3-CS杂化结构,使PFOA能够多点协同吸附,并增加了太阳光照射下PFOA的直接电子提取。此外,自由基dotOH自由基在PFOA降解中发挥了重要作用。最后,根据实验结果和密度泛函理论计算,提出了光降解机理。
Perfluorooctanoic acid (PFOA) has been widely detected in aquatic systems. Yet, cost-effective technologies for degrading PFAS have been lacking. We prepared and tested an adsorptive photocatalyst consisting of iron (hydr)oxides and carbon spheres (FeO/CS) through a one-step hydrothermal process. Characterization results revealed that the presence of carbon spheres affected the crystal formation of iron (hydr)oxides, and resulted in mutually modified mixed phases ferrihydrite and carbon spheres. FeO/CS was able to effectively adsorb and then degrade the pre-sorbed PFOA under simulated solar light. FeO/CS(1:1), prepared at an Fe:Glucose molar ratio of 1:1, showed the highest PFOA adsorption capacity and photoactivity. At a dosage of 1.0 g/L, FeO/CS(1:1) adsorbed nearly all 200 µg/L of PFOA within 1 h, and when the PFOA-laden FeO/CS(1:1) was subjected to simulated solar light at neutral pH, 95.2% of pre-concentrated PFOA was photodegraded and 57.2% defluorinated in 4 h. The efficient degradation also regenerated the material, allowing for repeated uses of the material without chemical regeneration. The much enhanced adsorption and photocatalytic activity of FeO/CS was attributed to: 1) CS facilitated formation of ferrihydrite, leading to adsorption of PFOA via binuclear and bidentate complexation, and 2) a hybrid ferrihydrite-CS structure, enabling multi-point, corporative adsorption of PFOA, and increasing direct electron extraction from PFOA under solar light irradiation. Moreover,radical dotOH radicals played an important role in PFOA degradation. Lastly, a photodegradation mechanism is proposed based on experimental findings and density functional theory calculations.
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