CNB-BA光催化剂的制备及其性能研究
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摘要
文章以尿素和四苯硼化钠作为前驱体,采用热聚合法制备了CNB,利用焙烧法制备了CNB与巴比妥酸(BA)不同质量比率的CNB-BA复合光催化剂。通过甲基橙等染料的光催化降解,考察了CNB-BA的紫外光催化活性。结果表明:在所有CNB-BA样品中,CNB-BA_(0.03)光催化剂具有最高的紫外光催化活性,在该优化条件下,紫外光照射45 min,CNB-BA_(0.03)光催化降解甲基橙降解率达到89.61%。光催化机理表明:·O_2~-和h~+在光催化降解过程中起明显作用,尤其是·O_2~-在光催化过程中起最主要作用。
Using urea and four benzene boron sodium as precursor, CNB was prepared by a thermal polymerization. The composite photocatalysts of CNB-BA were prepared by the method of roasting with different mass ratio of barbituric acid(BA) to CNB. With methyl orange as model compounds in photocatalytic reaction, the UV photocatalytic activity was evaluated. The results show that the composite photocatalyst of CNB-BA_(0.03) is the highest UV photocatalytic activity, and under the optimization condition, the rate of photocatalytic degradation of methyl orange can reach 89.61% with UV-irradiation of 45 min. The photocatalytic mechanism shows that ·O_2~- and h~+, especially ·O_2~-, jointly dominated the photodegradation process of methyl orange under UV light irradiation.
Using urea and four benzene boron sodium as precursor, CNB was prepared by a thermal polymerization. The composite photocatalysts of CNB-BA were prepared by the method of roasting with different mass ratio of barbituric acid(BA) to CNB. With methyl orange as model compounds in photocatalytic reaction, the UV photocatalytic activity was evaluated. The results show that the composite photocatalyst of CNB-BA_(0.03) is the highest UV photocatalytic activity, and under the optimization condition, the rate of photocatalytic degradation of methyl orange can reach 89.61% with UV-irradiation of 45 min. The photocatalytic mechanism shows that ·O_2~- and h~+, especially ·O_2~-, jointly dominated the photodegradation process of methyl orange under UV light irradiation.
引文
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[2]张坤,师瑞娟,崔玉民,等.复合催化剂SiO2/CNI的制备及其光催化性能研究[J].化工新型材料,2017,45(4):180-183.Zhang Kun,Shi Ruijuan,Cui Yumin,et al.Study on preparation and photocatalytic performance of SiO2/CNI composite catalyst[J].New Chemical Materials,2017,45(4):180-183.
[3]张金水,王博,王心晨,等.石墨相氮化碳的化学合成及应用[J].物理化学学报,2013,29(9):1865-1876.Zhang Jinshui,Wang Bo,Wang Xinchen,et al.Chemical synthesis and application of carbon nitride in graphite phase[J].Acta Physico-Chimica Sinica,2013,29(9):1865-1876.
[4]Yan S C,Li Z S,Zou Z G.Photodegradation of Rhodamine B and methyl orange over boron-doped g-C3N4under visible light irradiation[J].Langmuir,2010,26(6):3894-3901.
[5]Wang Y,Di Y,Antonietti M,et al.Excellent visible-light photocatalysis of fluorinated polymeric carbon nitride solids[J].Chemistry of Materials,2010,22(18):5119-5121.
[6]崔玉民,肖依,朱良俊,等.三氧化二铟/B元素掺杂的gC3N4催化剂的制备及性能研究[J].环境污染与防治,2017,39(5):490-493.Cui Yumin,Xiao Yi,Zhu Liangjun,et al.Study on preparation and photocatalytic property of In2O3/CNB[J].Environmental Pollution and Prevention,2017,39(5):490-493.
[7]张文保,崔玉民,李慧泉,等.Bi2O3/g-C3N4复合催化剂的制备及其性能研究[J].阜阳师范学院学报:自然科学版,2015,32(1):29-34.Zhang Wenbao,Cui Yumin,Li Huiquan,et al.Study on the preparation and properties of Bi2O3/g-C3N4composite photocatalysts[J].Journal of Fuyang Teachers College:Natural Science Edition,2015,32(1):29-34.
[8]Lin Z,Wang X.Nanostructure engineering and doping of conjugated carbon nitride semiconductors for hydrogen photosynthesis[J].Angewandte Chemie International Edition,2013,52(6):1735-1738.
[9]崔玉民,李慧泉,凡素华,等.对苯二甲酸协同Bi2O3/Co3O4光催化降解甲基橙的研究[J].稀有金属,2015,39(1):55-61.Cui Yumin,Li Huiquan,Fan Suhua,et al.Photocatalytic degradation of methyl orange enhanced by terephthalic acid using Bi2O3/Co3O4as heterogeneous catalysts[J].Chinese Journal of Rare Metals,2015,39(1):55-61.
[10]Chang C,Fu Y,Hu M,et al.Carbon self-doping induced high electronic conductivity and photoreactivity of g-C3N4[J].Appl Catal,2013,65(12):553-560.
[11]Hollmann D,Karnahl M,Tschierlei S,et al.Structure-activity relationships in bulk polymeric and sol-gel-derived carbon nitrides during photocatalytic hydrogen production[J].Chem Mater,2014,26(5):1727-1733.
[12]Qin Jiani,Wang Sibo,Ren He,et al.Carbon nitride nanowires were prepared by constant pressure benzene heat synthesis[J].Applied Catalysis B:Environmental,2015,179:1-8.
[13]Li Xuefei,Zhang Jian,Shen Longhai,at al.Preparation and characterization of graphitic carbon nitride through pyrolysis of melamine[J].Applied Physics A-Materials Science&Processing,2009,94(2):387-392.
[14]Thomas A.Graphitic carbon nitride materials:variation of structure and morphology and their use as metal-free catalysts[J].Journal of Materials Chemistry,2008,41(9):4893-4908.
[15]Wang Xinchen,Blechert Siegfried,Antonietti Markus.Polymeric graphitic carbon nitride for heterogeneous photocatalysis[J].ACS Catalysis,2012,2:1596-1606.
[16]Wang Xinchen,Thomas A,Fu Xianzhi,et al.Three-dimensional photomobility of crosslinked azo benzene liquid-crystalline polymer fiber[J].Adv Mater,2009,21:1609-1612.
[17]Cao J,Xu B Y,Lin H,et al.Novel heterostructured Bi2S3/BiOI photocatalyst:facile preparation,characterization and visible light photocatalytic performance[J].Dalton Transactions,2012,41(6):11482-11489.
[18]Li H Q,Cui Y M,Hong W S.High photocatalytic performance of BiOI/Bi2WO6toward toluene and Reactive Brilliant Red[J].Applied Surface Science,2013,264(6):581-588.
[19]Liu G M,Zhao J C,Hidaka H.ESR spin-trapping detection of radical intermediates in the TiO2-assisted photo-oxidation of sulforhodamine B under visible irradiation[J].J Photochem Photobiol A:Chem,2000,133(1/2):83-89.
[20]Cao J,Xu B Y,Lin H L,et al.Chemical etching preparation of BiOI/BiOBr heterostructures with enhanced photocatalytic properties for organic dye removal[J].Chemical Engineering Journal,2012,185/186(4):91-97.
[21]Liu G M,Li X,Zhao J C.Photooxidation mechanism of dye alizarin red in TiO2dispersions under visible illumination:an experimental and theoretical examination[J].J Mol Cata A:Chem,2000,153(1/2):211-218.
[22]崔玉民,孙倩,李慧泉,等.C3N4/ZnO/Fe2O3复合光催化剂的制备及性能[J].阜阳师范学院学报:自然科学版,2015,32(1):24-38.Cui Yumin,Sun Qian,Li Huiquan,et al.Preparation and properties of C3N4/ZnO/Fe2O3of heterogeneous photocatalyst[J].Journal of Fuyang Teachers College:Natural Science Edition,2015,32(1):29-34.
[23]崔玉民,李慧泉,苗慧,等.氧化锌制备及其光催化活性研究[J].化工新型材料,2015,43(5):100-102.Cui Yumin,Li Huiquan,Miao Hui,et al.A study on the preparation and photocatalytic activity of zinc oxide[J].New Chemical Materials,2015,43(5):100-102.
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