不同前驱体CNX-CS催化剂的构筑及其性能
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摘要
分别以三聚氰胺、尿素、硫脲为前驱体,采用高温焙烧法制备出不同的g-C_3N_4(CNX)材料,通过共混交联法将g-C_3N_4与壳聚糖(CS)进行复合,制得易再生、高稳定性的CNX-CS催化剂材料。采用扫描电镜(SEM)、X射线衍射图谱(XRD)、傅里叶变换红外(FTIR)等进行了表征,并对其进行了光催化性能评价。结果表明,来自于不同前驱体的g-C_3N_4均匀的分散在CS基质表面,复合过程中各自的结构得到了保持。以硫脲为前驱体的CNT-CS催化剂材料表现出最佳的吸附性能和催化性能协同作用,在5次循环实验之后降解率仍能达到95%,质量损失不超过10%。反应后的催化剂可通过简单加入氢氧化钠和过氧化氢进行再生。该研究对于易再生g-C_3N_4基催化剂的设计和水处理方面应用提供了良好基础。
This study fabricated graphitic carbon nitride materials with different precursors via high temperature calcination using melamine,urea and thiourea as precursors,then graphitic carbon nitride with different were mixed with chitosan to obtain the CNX-CS catalyst material which is easy to regenerate and has high stability.The prepared material was characterized by scanning electron microscopy(SEM),thermogravimetric analysis(TGA),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR).The results show that graphitic carbon nitride prepared by different precursors is uniformly distributed on the chitosan matrix,and the structure is maintained during the fabrication process.The CNT-CS catalyst whose precursor is thiourea showed the best synergistic effect of adsorption and catalysis.After 5 cycles in the test,the rate of dissolution can still reach 95%,the mass change less than 10%.The reacted catalyst can be regenerated by simply adding sodium hydroxide and hydrogen peroxide.This study provides a good basis for the design and water treatment applications of easily regenerated g-C_3N_4-based catalysts.
This study fabricated graphitic carbon nitride materials with different precursors via high temperature calcination using melamine,urea and thiourea as precursors,then graphitic carbon nitride with different were mixed with chitosan to obtain the CNX-CS catalyst material which is easy to regenerate and has high stability.The prepared material was characterized by scanning electron microscopy(SEM),thermogravimetric analysis(TGA),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR).The results show that graphitic carbon nitride prepared by different precursors is uniformly distributed on the chitosan matrix,and the structure is maintained during the fabrication process.The CNT-CS catalyst whose precursor is thiourea showed the best synergistic effect of adsorption and catalysis.After 5 cycles in the test,the rate of dissolution can still reach 95%,the mass change less than 10%.The reacted catalyst can be regenerated by simply adding sodium hydroxide and hydrogen peroxide.This study provides a good basis for the design and water treatment applications of easily regenerated g-C_3N_4-based catalysts.
引文
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[21]Yang L,Jiang L,Hu D.Swelling induced regeneration of Ti O2-impregnated chitosan adsorbents under visible light[J].Carbohydr Polym,2016,140:433-441.
[2]Jonidi-Jafari A,Shirzad-Siboni M,Yang J K,et al.Photocatalytic degradation of diazinon with illuminated Zn O-Ti O2composite[J].Journal of the Taiwan Institute of Chemical Engineers,2015,50:100-107.
[3]Verma A,Chhikara I,Dixit D.Photocatalytic treatment of pharmaceutical industry wastewater over Ti O2using immersion well reactor:synergistic effect coupling with ultrasound[J].Desalination and Water Treatment,2013,52(34/35/36):6591-6597.
[4]张金水,王博,王心晨.氮化碳聚合物半导体光催化[J].化学进展,2014(1):19-29.
[5]张金水,王博,王心晨.石墨相氮化碳的化学合成及应用[J].物理化学学报,2013(9):1865-1876.
[6]Zhu J,Xiao P,Li H,et al.Graphitic carbon nitride:synthesis,properties,and applications in catalysis[J].ACS Applied Materials&Interfaces,2014,6(19):16449-16465.
[7]Ye S,Wang R,Wu M Z,et al.A review on g-C3N4for photocatalytic water splitting and CO2reduction[J].Applied Surface Science,2015,358:15-27.
[8]Chen X.Ordered mesoporous SNA-15 type graphitic carbon nitride:A semiconductor host structure for photocatalytic hydrogen evolution with visible light[J].Chemistry of Materials,2009,21(18):4093-4095.
[9]Wang X,Chen X,Thomas A,et al.Metal-containing carbon nitride compounds:A new functional organic-metal hybrid material[J].Advanced Materials,2009,21(16):1609-1612.
[10]Wang Y X,Wang H,Chen F Y,et al.Facile synthesis of oxygen doped carbon nitride hollow microsphere for photocatalysis[J].Applied Catalysis B:Environmental,2017,206:417-425.
[11]赵春禄,刘辉,刘振儒.壳聚糖的化学改性及其吸附性能的研究[J].环境化学,2005(2):209-212.
[12]杨晋青,叶盛权,郭祀远.磁性壳聚糖微球的制备及其应用[J].现代食品科技,2008(10):1079-1082.
[13]徐静,闻宏亮,欧阳建波,等.氧化石墨烯-壳聚糖复合材料对甲烯蓝的吸附动力学[J].上海大学学报:自然科学版,2013(4):400-404.
[14]孙胜玲,王丽,吴瑾,等.壳聚糖及其衍生物对金属离子的吸附研究(下)[J].高分子通报,2005(6):34-38.
[15]Amaral I F,Granja P L,Barbosa M A.Chemical modification of chitosan by phosphorylation:an XPS,FTIR and SEM study[J].Journal of Biomaterials Science,Polymer Edition,2005,16(12):1575-1593.
[16]Zhou L,Wang Y,Liu Z,et al.Characteristics of equilibrium,kinetics studies for adsorption of Hg(II),Cu(II),and Ni(II)ions by thiourea-modified magnetic chitosan microspheres[J].J Hazard Mater,2009,161(2/3):995-1002.
[17]王红英,常凯,钱斯日古楞,等.磁性壳聚糖微球的制备及其性能[J].大连工业大学学报,2011(2):105-108.
[18]唐星华,周爱玲.壳聚糖及其衍生物对金属离子吸附研究进展[J].江西化工,2007(1):1-5.
[19]宋艳艳,孔维宝,宋昊,等.磁性壳聚糖微球的研究进展[J].化工进展,2012(2):345-354.
[20]Nishad P A,Bhaskarapillai A,Velmurugan S.Nano-titania-crosslinked chitosan composite as a superior sorbent for antimony(III)and(V)[J].Carbohydr Polym,2014,108:169-175.
[21]Yang L,Jiang L,Hu D.Swelling induced regeneration of Ti O2-impregnated chitosan adsorbents under visible light[J].Carbohydr Polym,2016,140:433-441.