化工新型材料

化工新型材料 ›› 2023, Vol. 51 ›› Issue (4) : 269-274. DOI: 10.19817/j.cnki.issn1006-3536.2023.04.048

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光催化铁掺杂石墨相氮化碳活化过硫酸盐处理酚类废水的研究

作者信息 +

Study on photocatalytic treatment of phenolic wastewater by iron-doped graphite phase carbon nitride activated persulfate

Zuo Yifan, Ma Huiqiang, Li Shuang, Li Cong

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文章历史 +

Received		Published
2021-12-30		2023-04-20
Issue Date	Revised Date
2023-04-27	2021-12-30

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摘要

以九水合硝酸铁[Fe(NO₃)₃·9H₂O]和三聚氰胺为原料,采用热聚合法制备Fe-C₃N₄,通过X射线衍射、X射线光电子能谱对其进行表征。考察了光催化Fe-C₃N₄活化过硫酸钠(PS)去除苯酚的效果,并对铁掺杂石墨相氮化碳的制备条件进行了优选。结果表明:Fe-C₃N₄中存在Fe—N键,铁掺杂成功且合成良好,无任何杂质。相对于单独PS和g-C₃N₄+PS,Fe-C₃N₄+PS共同作用可高效去除苯酚,去除率可达到88.2%,苯酚去除效果随催化剂投加量的增大而提高。同时在过硫酸钠与苯酚的摩尔比为100∶1,Fe-C₃N₄催化剂浓度为2g/L,同时反应全程放置于250W高压钠灯下同步照射的条件下,Fe-C₃N₄焙烧温度580℃,焙烧时间4h,铁掺杂量5%时,体系对苯酚的去除率最高,反应240min达到97.4%。因此,铁掺杂g-C₃N₄明显改善了g-C₃N₄对可见光的利用率,对优化苯酚废水去除的效果明显。

Abstract

Fe-C₃N₄ was prepared by thermal polymerization with iron nitrate 9 hydrate [Fe(NO₃)₃·9H₂O] and melamine as raw materials,and characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS).The removal effect of phenol by photocatalytic Fe-C₃N₄ activated sodium persulfate (PS) was investigated,and the preparation conditions of Fe-doped graphite phase carbon nitride were optimized.The results showed that Fe—N bond existed in the prepared material Fe-C₃N₄,the iron doping was successful,and the synthesis was good without any impurities.Compared with PS alone and g-C₃N₄+PS,Fe-C₃N₄+PS could effectively remove phenol,and the removal rate could reach 88.2%.The removal efficiency of phenol increased with the increase of catalyst dosage.Meanwhile,when the mole ratio of sodium persulfate to phenol was 100∶1,the concentration of Fe-C₃N₄ catalyst was 2g/L,and the reaction was placed in 250W high pressure sodium lamp under synchronous irradiation,the roasting temperature of Fe-C₃N₄ preparation was 580℃,the roasting time was 4h,and the iron doping ratio was 5%,the system presented the highest removal rate of phenol,reaching 97.4% at 240min.The Fe-doped g-C₃N₄ significantly improved the utilization rate of g-C₃N₄ to visible light,and had an obvious effect on the optimization of phenol wastewater removal.

关键词

Fe-C₃N₄催化剂 / 光催化 / 过硫酸盐 / 苯酚

Key words

Fe-C₃N₄ catalyst / photocatalytic / persulfate / phenol

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光催化铁掺杂石墨相氮化碳活化过硫酸盐处理酚类废水的研究[J]. 化工新型材料, 2023, 51(4): 269-274 DOI:10.19817/j.cnki.issn1006-3536.2023.04.048

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参考文献

原文顺序 | 出版日期 | 本文引用

[1] 肖怡.活化过硫酸盐高级氧化法处理苯酚废水的试验研究[D].沈阳:沈阳建筑大学,2016.
[2] 张帆,刘媛,贺盛福,等.处理含酚废水的研究进展[J].现代化工,2015,35(1):67-72.
[3] 杨彩玲,魏瑞霞.酚废水处理技术的研究进展[J].河北理工大学学报,2010,31(1):102-105.
[4] 丁朋晓,张连英,陈文波.含酚废水处理技术现状与进展[J].甘肃科技,2013,29(6):25-27.
[5] Zhang Y,Zhuang Y,Geng J,et al.Reduction of antibiotic resistance genes in municipal wastewater effluent by advanced oxidation processes[J].Science of the Total Environment,2016,550:184-191.
[6] Ling S K,Wang S,Peng Y.Oxidative degradation of dyes in water using Co²⁺/H₂O₂ and Co²⁺/peroxymonosulfate[J].Journal of Hazardous Materials,2010,178(1-3):385-389.
[7] Lee J,Von Gunten U,Kim J H.Persulfate-based advanced oxidation:critical assessment of opportunities and roadblocks[J].Environmental Science & Technology,2020,54(6):3064-3081.
[8] Zhang Y,Chen S.Research on the advanced oxidation technology based on dyeing waste-water treatment[J].IOP Conference Series:Earth and Environmental Science,2020,495(1):012080.
[9] Tan C,Gao N,Chu W,et al.Degradation of diuron by persulfate activated with ferrous ion[J].Separation & Purification Technology,2012,95:44-48.
[10] 张瑛洁,李大鹏,曹天静,等.零价铁活化过硫酸铵氧化降解苯酚的研究[J].工业水处理,2012,32(9):13-16.
[11] 刘淑荣.4-氨基安替比林直接光度法测定废水中挥发酚的改进[J].福建分析测试,2005(1):2128-2129.
[12] Anandan S,Vinu A,Mori T,et al.Photocatalytic degradation of 2,4,6-trichlorophenol using lanthanum doped ZnO in aqueous suspension[J].Catalysis Communications,2007,8(9):1377-1382.
[13] Tonda S,Kumar S,Kandula S,et al.Fe-doped and-mediated graphitic carbon nitride nanosheets for enhanced photocatalytic performance under natural sunlight[J].Journal of Materials Chemistry A,2014,2(19):6772-6780.
[14] Hu S,Ma L,You J,et al.Enhanced visible light photocatalytic performance of g-C₃N₄ photocatalysts co-doped with iron and phosphorus[J].Applied Surface Science,2014,311:164-171.
[15] Gao Y,Zhang Z,Li S,et al.Insights into the mechanism of heterogeneous activation of persulfate with a clay/iron-based catalyst under visible LED light irradiation[J].Applied Catalysis B:Environmental,2016,185:22-30.
[16] 王坤,徐舸,许延恒.热聚合法制备Fe/g-C₃N₄及其性能研究[J].山东化工,2021,50(13):6-7.
[17] 吴文倩,邓德明.铁掺杂氮化碳的制备及其可见光催化性能[J].武汉大学学报(理学版),2017,63(3):227-233.
[18] 姜鹏程,王周福,王玺堂,等.不同气氛下类石墨相氮化碳的合成及热稳定性能[J].材料导报,2021,35(6):6048-6053.
[19] Dong F,Wang Z,Sun Y,et al.Engineering the nanoarchitecture and texture of polymeric carbon nitride semiconductor for enhanced visible light photocatalytic activity[J].Journal of Colloid and Interface Science,2013,401:70-79.
[20] Ge L,Han C,Liu J,et al.Enhanced visible light photocatalytic activity of novel polymeric g-C₃N₄ loaded with Ag nanoparticles[J].Applied Catalysis A:General,2011,409:215-222.