Research progress in the application and degradation mechanism of perfluorooctanoic acid photocatalytic materials
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摘要:
全氟辛酸（PFOA）是一种广泛存在于环境介质中的典型全氟化合物，具有高毒性、难降解等特点，严重威胁生态环境安全及人类遗传、免疫、神经和生殖健康，其环境危害和风险防控引起广泛关注。光催化技术具有反应条件温和、处理效率高、应用成本低且无二次污染等优势，在PFOA的降解处理方面具有广阔应用前景。为研发活性强、可见光吸收性能好、稳定性高的新型光催化材料，实现水中PFOA的高效降解，系统梳理了近20年来PFOA光催化降解材料制备的相关研究，对不同光催化降解材料的降解特性及存在问题进行全面分析；结合现有材料对PFOA的光催化降解，总结光催化降解材料的反应机理及活性增强机制，阐明PFOA的光催化降解路径。
Abstract:Perfluorooctanoic acid (PFOA) is a typical perfluorinated compound widely existing in the environment. It is highly toxic and difficult to degrade, which seriously threatens eco-environmental safety and human genetic, immune, neurological and reproductive health. Hence, considerable attention has been drawn to its environmental hazard and risk prevention and control. With mild conditions, high treatment efficiency, low application cost, free secondary pollution and other advantages, photocatalytic technology has a broad application prospect in the field of PFOA degradation. In order to develop new photocatalytic materials with strong activity, good visible light absorption performance, and high stability, and achieve efficient degradation of PFOA in water, research progress in the preparation of photocatalytic degradation materials of PFOA in the past twenty years was systematically reviewed. The degradation characteristics and existing problems of different photocatalytic degradation materials were comprehensively analyzed. The reaction mechanism and activity enhancement mechanism of photocatalytic degradation materials were summarized, combined with the existing materials of photocatalytic degradation of PFOA, and eventually the photocatalytic degradation pathway of PFOA was clarified.
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Key words:
- perfluorooctanoic acid /
- photocatalysis /
- advanced oxidation /
- degradation mechanism /
- progress
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图 3 传统光响应异质结光催化剂下几种不同类型的电子-空穴对分离示意
Figure 3. Schematic diagram of separation of several different types of electron-hole pairs under conventional photoresponsive heterojunction photocatalysts
表 1 TiO2基材料对PFOA的光催化降解效果
Table 1. Photocatalytic degradation effect of PFOA by TiO2-based materials
降解材料 光类型 光波长/nm 光强度/W 反应条件 反应时
间/h降解
率/%脱氟
率/%TiO2[20] UV 310~400 75 V=50 mL，C0=1.5 mmol/L，pH=1.0，Ccat=2 g/L 24 — 47 TNTs[37] UV 254 400 V=2 L，C0=50 mg/L，pH=4.0，Ccat=0.125 g/L 24 59 — 掺杂金属 Pb-TiO2[13] UV 254 400 C0=50 mg/L，pH=5.0，Ccatalyst=0.5 g/L 12 99.9 22.4 Pt-TiO2[38] UV 365 125 V=120 mL，C0=60 mg/L，pH=3.0，Ccat=0.5 g/L 7 100 34.8 Cu-TiO2[26] UV 254 400 C0=50 mg/L，pH=5.0，Ccat=0.5 g/L 12 91 19 负载碳材料 TiO2-MWCNTs(10:1)[30] UV 365 300 V=250 mL，C0=30 mg/L，pH=2.0，Ccat=1.6 g/L 8 94 — rGO-TiO2[32] UV或可见光 200~600 150 C0=0.24 mmol/L，pH=3.8，Ccat=0.1 g/L 12 93±7 62 构建异质结 Fe/TNTs@AC[34] UV 254 30 V=40 mL，C0=100 mg/L，pH=7.0，Ccat=1.0 g/L 4 >90 62 Sb2O3-TiO2[35] UV 200~280 4 C0=10 mg/L，pH=4.4，Ccat=0.25 g/L 2 81.7 — Ce/TiO2/g-C3N4[24] 可见光 420~800 300 C0=4 mg/L，pH=2.0，Ccat=1.0 g/L 3 94.4 38.6 Ti3C2/TiO2[39] UV 254 4.5 C0=20 μmol/L，Ccat=0.2 g/L 16 >99.9 49.0 注：—表示文献中未提及。V为反应体系容积；C0为PFOA初始浓度；pH为反应最佳条件下pH；Ccat为反应最佳条件下催化剂用量。 
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表 2 In2O3基材料对PFOA的光催化降解效果
Table 2. Photocatalytic degradation effect of PFOA by In2O3-based materials
降解材料 光类型 光波长/nm 光强度/W 反应条件 反应时
间/h降解
率/%脱氟
率/%In2O3[18] UV 254 23 V=400 mL，C0=0.1 mmol/L，pH=3.8，Ccat=0.5 g/L 4 83.1 66.3 3%Pt/IONRs[49] UV 254 500 V=200 mL，C0=200 mg/L，pH=1.85，Ccat=0.4 g/L 1 98 — g-C3N4-In2O3[45] UV 254 500 V=50 mL，C0=200 mg/L，Ccat=0.4 g/L — 91（1 h） 96（3 h） In2O3-GR[46] UV 254 15 V=100 mL，C0=30 mg/L，Ccat=0.4 g/L 3 100 60.9 0.86%CeO2/In2O3[47] UV 254 500 V=200 mL，pH=2.84，C0=100 mg/L，Ccat=0.4 g/L 1 100 53.3 MnOx-In2O3[50] 太阳光 500 V=50 mL，C0=50 mg/L，pH=3.8，Ccat=0.5 g/L 3 99.8 17.4 注：同表1。
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表 3 Bi基材料对PFOA的光催化降解效果
Table 3. Photocatalytic degradation effect of PFOA by Bi-based materials
降解材料 光类型 光波长/nm 光强度/W 反应条件 反应时
间/h降解
率/%脱氟
率/%BiOX 0.95BiOI-0.05Br[53] UV 254 300 V=30 mL，C0=20 mg/L，Ccat=0.4 g/L 2 96 — BiOI/Bi5O7I[64] 模拟太阳光 400~760 800 V=40 mL，pH=3.0，C0=15 mg/L，Ccat=0.5 g/L 6 80 60 BiOCl[55] UV 254 10 V=200 mL，pH=4.8，C0=0.02 mmol/L，Ccat=0.5 g/L 24 59.3 52.5 BiOCl0.2I0.8[65] 可见光 420~700 300 V=100 mL，C0=50 μmol/L，Ccat=1 g/L 6 65.56 — BiOCl/BiPO4[66] UV 254 2 V=50 mL，C0=20 mg/L，Ccat=0.5 g/L 45 100 — Zn-AlLDHs-BiOCl[57] UV <350 50 V=200 mL，pH=2.0，C0=0.5 mg/L，Ccat=0.5 g/L 6 90 — BFO 0.5% rGO-Pb-BFO[63] UV 254 5 V=80 mL，pH=2.0，C0=100 mg/L，Ccat=0.05~0.4 g/L 8 69.6 37.6 BiOHP 9% BiOHP/CS[59] UV 254 18 V=40 mL，pH=7.0，C0=0.2 mg/L，Ccat=1.0 g/L — >90（1 h） 32.5（4 h） 注：同表1。
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表 4 其他类型材料对PFOA的光催化降解效果
Table 4. Photocatalytic degradation effect of PFOA by other types of materials
降解材料 光类型 光波长/nm 光强度/W 反应条件 反应时间/h 降解率/% 脱氟率/% Ga2O3 商业 UV 254 14 V=150 mL，C0=500 μg/L，pH=4.8，Ccat=0.5 g/L 3 38 — 束状[22] — 100(45 min) 61(3 h) InOOH[68] UV 254 18 V=200 mL，C0=20 mg/L，Ccat=0.25 g/L 3 83.4 — ZnO ZnO[19] UV 254 28 V=1 L，C0=100 mg/L，pH=3.1，Ccat=0.2 g/L 4 18.2 — ZnO/rGO[78] 太阳光 — V=100 mL，C0=100 mg/L，Ccat=1 g/L 100 90.91 — Bi5O7I-ZnO[79] 可见光 420~700 500 V=50 mL，pH=4.0，C0=1 mg/L，Ccat=0.5 g/L 6 91 52.2 HPW HPW[23] UV 254 200 V=22 mL，C0=1.35 mmol/L，Ccat=6.68 mmol/L 24 100 88 HPW-BPS[71] UV 185 8 V=500 mL，pH=3.0-4.0，C0=5 mg/L，Ccat=0.2 g/L 4 53 — Fe基 Fe-沸石[73] UV 300~400 4 V=100 mL，pH=3.0，C0=48 μmol/L，Ccat=1 g/L 6 >99 38 FeO/CS[74] 太阳光 6 V=160 mL，pH=7.0，C0=0.2 mg/L，Ccat=1.0 g/L 4 95.2 57.20 CeO2@NiAl-LDHs[69] 可见光 400~600 500 V=50 mL，pH=9.0，C0=50 mg/L，Ccat=0.5 g/L 5 90.2 — 注：同表1。
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