ZnIn2S4/g-C3N4光催化降解水中痕量药物卡马西平

朱琳; 卜龙利; 刘嘉栋

PDF(668 KB)

中国环境科学 ›› 2020, Vol. 40 ›› Issue (7) : 2917-2925.

水污染与控制

ZnIn₂S₄/g-C₃N₄光催化降解水中痕量药物卡马西平

朱琳¹, 卜龙利^1,2,3, 刘嘉栋^1,2,3

作者信息 +

Photocatalytic degradation of trace carbamazepine in river water by ZnIn₂S₄/g-C₃N₄ under solar irradiation

ZHU Lin¹, BO Long-li^1,2,3, LIU Jia-dong^1,2,3

Author information +

文章历史 +

摘要

本文采用水热合成法制备ZnIn₂S₄/g-C₃N₄复合催化剂应用于水中痕量药物卡马西平（CBZ）的太阳光催化降解，探究实际河水中固体颗粒（SS），无机盐（IS）和溶解性有机物（DOM）对催化剂活性的影响以及ZnIn₂S₄/g-C₃N₄/浮石负载型催化剂光催化CBZ效果.结果表明，质量比为20：1 ZnIn₂S₄/g-C₃N₄的光催化活性高于ZnIn₂S₄，ZnIn₂S₄与g-C₃N₄异质结构加速了电子-空穴对的分离并抑制其复合、ZnIn₂S₄/g-C₃N₄中孔的增多和比表面积的增加有效提高了催化剂活性.水质参数对催化剂活性的影响顺序为DOM>IS>SS，过滤后河水中CBZ的光催化速率常数比原水提高了13倍；125mg/L催化剂投加量和太阳光照射240min后，100μg/L的CBZ被完全降解.动态试验中CBZ的光催化效率随水流速度的增大而下降；流速5mL/min下循环4次，ZnIn₂S₄/g-C₃N₄/浮石光催化降解与矿化CBZ的效率分别为86.4%和43.9%.

Abstract

ZnIn₂S₄/g-C₃N₄ composite catalyst prepared by hydrothermal method was applied to catalyze trace carbamazepine (CBZ) in river water under solar irradiation. The effect of suspended solid (SS), inorganic salt (IS), and dissolved organic matter (DOM) in real river water on the catalytic activity of ZnIn₂S₄/g-C₃N₄ composite catalyst and the experimental effect in dynamic tests of ZnIn₂S₄/g-C₃N₄/pumice loaded catalyst to CBZ were both analyzed. It indicated that the catalytic activity of ZnIn₂S₄/g-C₃N₄ with mass ratio of 20:1 was higher than that of pure ZnIn₂S₄ in CBZ photocatalytic degradation. The heterogeneous structure of ZnIn₂S₄/g-C₃N₄ accelerated the separation of electron-hole pairs and simultaneously prohibited their recombination. An increase in the amount of mesopore and an increase in specific surface area of ZnIn₂S₄/g-C₃N₄ both could improve the catalytic activity of the catalyst effectively. The influence of water quality parameters on the catalyst activity in an increasing sequence was DOM>IS>SS, and the constant of photocatalytic rate of CBZ in filtered river water increased 13times than that in raw river water. CBZ of an initial concentration of 100μg/L was completely degraded with a dosage of 125mg/L catalyst and under 240min solar irradiation. In dynamic tests, the photocatalytic efficiency of CBZ decreased gradually with an increase in the flow rate of water. Under 4cycles with a flow rate of 5mL/min, the rate of removal and the rate of mineralization of CBZ by ZnIn₂S₄/g-C₃N₄/pumice catalyst were 86.4% and 43.9%, respectively.

导出引用

朱琳, 卜龙利, 刘嘉栋. ZnIn₂S₄/g-C₃N₄光催化降解水中痕量药物卡马西平[J]. 中国环境科学. 2020, 40(7): 2917-2925

ZHU Lin, BO Long-li, LIU Jia-dong. Photocatalytic degradation of trace carbamazepine in river water by ZnIn₂S₄/g-C₃N₄ under solar irradiation[J]. China Environmental Science. 2020, 40(7): 2917-2925

中图分类号： X703

参考文献

[1] 严清,张怡昕,高旭,等.典型医药活性物质在污水处理厂中的归趋及其风险评估[J]. 中国环境科学, 2014,34(3):672-680. Yan Q, Zhang Y X, Gao X, et al. Fate of pharmaceutically active compounds in a municipalwastewater treatment plantand risk assessment[J]. China Environmental Science, 2014,34(3):672-680.
[2] 李抒苡,孙傅,李丹,等.污水再生处理工艺中卡马西平的去除过程模拟及其生态风险评价[J]. 生态毒理学报, 2017,12(5):119-128. Li S Y, Sun F, Li D, et al. Modeling the removal of carbamazepine in wastewater reclamation processes and its ecological risk[J]. Asian Journal of Ecotoxicology, 2017,12(5):119-128.
[3] 何强,张峻华,古励,等.颗粒活性炭吸附去除尿中药活性化合物(PhACs)[J]. 环境工程学报, 2013,7(9):3307-3311. He Q, Zhang J H, Gu L, et al. Removal of pharmaceutically active compounds(PhACs) from huamn urine using granular activated carbon)[J]. Chinese Journal of Environmental Engineering, 2013,7(9):3307-3311.
[4] Ferrari B, Paxeus N, Lo G R, et al. Ecotoxicological impact of pharmaceuticals found in treated wastewaters:study of carbamazepine, clofibric acid, and diclofenac[J]. Ecotoxicol Environ Saf, 2003,55(3):359-370.
[5] Jarvis A L, Bernot M J, Bernot R J. The effects of the psychiatric drug carbamazepine on freshwater invertebrate communities and ecosystem dynamics[J]. Science of the Total Environment, 2014,496:461-470.
[6] Bo L, He K, Tan N, et al. Photocatalytic oxidation of trace carbamazepine in aqueous solution by visible-light-driven Znln₂S₄:Performance and mechanism[J]. Journal of Environmental Management, 2017,190:259-265.
[7] 冯奇奇,卜龙利,高波,等.ZnIn₂S₄可见光催化降解水中的双氯芬酸[J]. 环境工程学报, 2017,11(2):739-747. Feng Q Q, Bo L L, Gao B, et al. Photocatalytic degradation of aqueous diclofenac by ZnIn₂S₄under visible light[J]. Chinese Journal of[J] Environmental Engineering, 2017,11(2):739-747.
[8] 苏海英,王盈霏,王枫亮,等.g-C₃N₄/TiO₂复合材料光催化降解布洛芬的机制[J]. 中国环境科学, 2017,37(1):195-202. Su H Y, Wang Y F, Wang F L, et al. Preparation of g-C₃N₄/TiO₂ composites and the mechanism research of the photocatalysis degradation of ibuprofen[J]. China Environmental Science, 2017, 37(1):195-202.
[9] Ming L, Sun N, Xu L, et al. Fluoride ion-promoted hydrothermal synthesis of oxygenated g-C3N4 with high photocatalytic activity[J]. Colloids and Surfaces A:Physicochemical and Engineering Aspects, 2018,549:67-75.
[10] 尹竞,廖高祖,朱冬韵,等.g-C₃N₄/石墨烯复合材料的制备及光催化活性的研究[J]. 中国环境科学, 2016,36(3):735-740. Yin J, Liao G Z, Zhu D Y, et al. Preparation and photocatalytic activity of g-C₃N₄/rGO composite[J]. China Environmental Science, 2016,36(3):735-740.
[11] Chai B, Peng T, Zeng P, et al. Template-Free Hydrothermal Synthesis of ZnIn₂S₄Floriated Microsphere as an Efficient Photocatalyst for H₂Production under Visible-Light Irradiation[J]. The Journal of Physical Chemistry C, 2011,115(13):6149-6155.
[12] Tan S, Xing Z, Zhang J, et al. Meso-g-C₃N₄/g-C₃N₄nanosheets laminated homojunctions as efficient visible-light-driven photocatalysts[J]. International Journal of Hydrogen Energy, 2017, 42(41):25969-25979.
[13] Ding N, Zhang L, Zhang H, et al. Microwave-assisted synthesis of ZnIn₂S₄/g-C₃N₄heterojunction photocatalysts for efficient visible light photocatalytic hydrogen evolution[J]. Catalysis Communications, 2017,100:173-177.
[14] Guo F, Cai Y, Guan W, et al. Graphite carbon nitride/ZnIn₂S₄ heterojunction photocatalyst with enhanced photocatalytic performance for degradation of tetracycline under visible light irradiation[J]. Journal of Physics and Chemistry of Solids, 2017,110:370-378.
[15] Jo W, Natarajan T S. Fabrication and efficient visible light photocatalytic properties of novel zinc indium sulfide (ZnIn₂S₄)-graphitic carbon nitride (g-C₃N₄)/bismuth vanadate (BiVO₄) nanorod-based ternary nanocomposites with enhanced charge separation via Z-scheme transfer[J]. Journal of Colloid and Interface Science, 2016,482:58-72.
[16] 兰隽如,周晓琴,李子富,等.硅胶负载TiO₂催化剂的制备与光催化效果[J]. 环境工程, 2017,35(2):43-48. Lan J R, Zhou X Q, Li Z F, et al. Preparation and photocatalytic activity of silica gel supported TiO₂[J]. Environmenta Engineering, 2017,35(2):43-48.
[17] 张小玲,班云霄.LED联合玻璃纤维光催化填料对苯酚的降解研究[J]. 中国环境科学, 2018,38(8):2941-2946. Zhang X L, Ban Y X. Study on the degradation of phenol by UV-LED combined with glass fiber photocatalytic fillers[J]. China Environmental Science, 2018,38(8):2941-2946.
[18] 秦真波,夏大海,吴忠,等.磷酸盐无机涂料及其研究进展[J]. 表面技术, 2019,48(12):34-42. Qin Z B, Xia D H, Wu Z, et al. Phosphate Inorganic Coating and Its Research Progress[J]. Surface technology, 2019,48(12):34-42.
[19] Bo L, Han H, Liu H. Influence of water quality on photocatalytic degradation of trace carbamazepine in real water bodies[J]. Desalination and Water Treatment, 2018,124:240-247.
[20] Lin B, Li H, An H, et al. Preparation of 2D/2Dg-C₃N₄ nanosheet@ZnIn₂S₄nanoleaf heterojunctions with well-designed high-speed charge transfer nanochannels towards high-efficiency photocatalytic hydrogen evolution[J]. Applied Catalysis B:Environmental, 2018,220:542-552.
[21] Qiu P, Yao J, Chen H, et al. Enhanced visible-light photocatalytic decomposition of 2,4-dichlorophenoxyacetic acid over ZnIn₂S₄/g-C₃N₄ photocatalyst[J]. Journal of Hazardous Materials, 2016,317:158-168.
[22] Kheradmand A, Zhu Y, Zhang W, et al. Cobalt oxide on mesoporous carbon nitride for improved photocatalytic hydrogen production under visible light irradiation[J]. International Journal of Hydrogen Energy, 2019,44(33):17930-17942.
[23] Chang C, Fu Y, Hu M, et al. Photodegradation of bisphenol A by highly stable palladium-doped mesoporous graphite carbon nitride (Pd/mpg-C₃N₄) under simulated solar light irradiation[J]. Applied Catalysis B:Environmental, 2013,142-143:553-560.
[24] Chen Z, Li D, Zhang W, et al. Low-Temperature and Template-Free Synthesis of ZnIn₂S₄Microspheres[J]. Inorganic Chemistry, 2008, 47(21):9766-9772.
[25] Jrad A, Ben Nasr T, Turki-Kamoun N. Study of structural, optical and photoluminescence properties of indium-doped zinc sulfide thin films for optoelectronic applications[J]. Optical Materials, 2015,50:128-133.
[26] Cao S, Low J, Yu J, et al. Polymeric Photocatalysts Based on Graphitic Carbon Nitride[J]. Advanced Materials, 2015,27(13):2150-2176.
[27] Woo H, Park J, Kim J, et al. Hierarchical hybrid MnO/Pd-Fe₃O₄ and CoO/Pd-Fe₃O₄nanocomposites as efficient catalysts for hydroboration of styrene[J]. Catalysis Communications, 2017,100:52-56.
[28] Escudero C J, Iglesias O, Dominguez S, et al. Performance of electrochemical oxidation and photocatalysis in terms of kinetics and energy consumption. New insights into the p-cresol degradation[J]. Journal of Environmental Management, 2017,195:117-124.
[29] Dugandžić A M, Tomašević A V, Radišić M M, et al. Effect of inorganic ions, photosensitisers and scavengers on the photocatalytic degradation of nicosulfuron[J]. Journal of Photochemistry and Photobiology A:Chemistry, 2017,336:146-155.
[30] Zhao Q, Sun J, Li J, et al. Kinetics and mechanism of Horner-Wadsworth-Emmons reaction of weakly acidic phosphonate in solid-liquid phase-transfer catalysis system[J]. Catalysis Communications, 2013,36:98-103.
[31] Bo L, Liu H, Han H. Photocatalytic degradation of trace carbamazepine in river water under solar irradiation[J]. Journal of Environmental Management, 2019,241:131-137.