The preparation of two-dimensional ultrathin g-C3N4 and the research of the photo-catalysis properties
SU Yue-han1, WANG Ying-fei1, ZHANG Qian-xin1, CHEN Tian-sheng1, SU Hai-ying1, CHEN Ping1, WANG Feng-liang1, LIU Hai-jin2, LÜ Wen-ying1, YAO Kun1, LIU Guo-guang1
1. School of Environmental Science and Engineering, Guangdong University of Technology, Guang zhou 510006, China;
2. School of Environment, Henan Normal University, Xin xiang 453007, China
In this study, the ultrathin g-C3N4 (UCN) with large specific surface area was successfully prepared. The characterizations of the UCN were carried out by transmission electron microscope (TEM), X-ray diffraction (XRD), Brunauer-Emmett-Teller (BET), ultraviolet-visible absorption spectrum (UV-vis) and fluorescence spectrophotometer (PL). The results showed that the as-prepared UCN sample consisted of the ultrathin two-dimension layers with abundant of pores, which could provide more active sites for photoreaction. In addition, the special structure of UCN could effectively expand its visible light absorption regions and inhibited the recombination of photo-induced carriers. The photocatalytic activity of the UCN was remarkably higher than that of g-C3N4 for the degradation of enrofloxacin (ENX) under simulated sunlight irradiation. 0.4g/L of UCN showed the optimal ENX degradation performance (81.7%), which was almost 4.1times higher reaction rate than that of pristine g-C3N4. Moreover, the photocatalytic degradation of ENX followed pseudo-first-order kinetics according to the Langmuir-Hinshelwood model. It showed best effects of the photocatalytic degradation of ENX when pH=5. The quenching experiment demonstrated that the contribution rate of O2·- was 66.4%, indicating that O2·- plays a major role in the photocatalytic degradation of ENX.
苏跃涵, 王盈霏, 张钱新, 陈天生, 苏海英, 陈平, 王枫亮, 刘海津, 吕文英, 姚琨, 刘国光. 二维超薄g-C3N4的制备及其光催化性能研究[J]. 中国环境科学, 2017, 37(10): 3748-3757.
SU Yue-han, WANG Ying-fei, ZHANG Qian-xin, CHEN Tian-sheng, SU Hai-ying, CHEN Ping, WANG Feng-liang, LIU Hai-jin, LÜ Wen-ying, YAO Kun, LIU Guo-guang. The preparation of two-dimensional ultrathin g-C3N4 and the research of the photo-catalysis properties. CHINA ENVIRONMENTAL SCIENCECE, 2017, 37(10): 3748-3757.
Dai G, Wang B, Fu C, et al. Pharmaceuticals and personal care products (PPCPs) in urban and suburban rivers of Beijing, China:occurrence, source apportionment and potential ecological risk[J]. Environmental Science Processes & Impacts, 2016,18(4):445-455.
[2]
Santiago S, Roll D M, Ray C, et al. Effects of soil moisture depletion on vegetable crop uptake of pharmaceuticals and personal care products (PPCPs)[J]. Environmental Science & Pollution Research, 2016,23(20):20257-20268.
[3]
Tao L, Yu S, Wei C. Occurrence, removal and risk assessment of pharmaceutical and personal care products (PPCPs) in an advanced drinking water treatment plant (ADWTP) around Taihu Lake in China[J]. Chemosphere, 2016,152:1-9.
Hirsch R, Ternes T, Haberer K, et al. Occurrence of antibiotics in the aquatic environment[J]. Science of the Total Environment, 1999,225(1/2):109-118.
Sacher F, Lange F T, Brauch H J, et al. Pharmaceuticals in groundwaters analytical methods and results of a monitoring program in Baden-Wurttemberg, Germany[J]. Journal of Chromatography A, 2002,938(1/2):199-210.
Cao S, Yu J. g-C3N4-Based photocatalysts for hydrogen generation[J]. Journal of Physical Chemistry Letters, 2014, 5(12):2101-2107.
[13]
Yan S C, Li Z S, Zou Z G. Photodegradation performance of g-C3N4fabricated by directly heating melamine[J]. Langmuir, 2009,25(17):10397-10401.
[14]
Zhang X, Xie X, Wang H, et al. Enhanced photoresponsive ultrathin graphitic-phase C3N4 nanosheets for bioimaging[J]. Journal of the American Chemical Society, 2012,135(1):18.
[15]
Dong F, Wu L, Sun Y, et al. Efficient synthesis of polymeric g-C3N4 layered materials as novel efficient visible light driven photocatalysts[J]. Journal of Materials Chemistry, 2011,21(39):15171-15174.
[16]
Yan S C, Li Z S, Zou Z G. Photodegradation of rhodamine B and methyl orange over boron-doped g-C3N4 under visible light irradiation[J]. Langmuir the Acs Journal of Surfaces & Colloids, 2010,26(6):3894-901.
[17]
Shiraishi Y, Kanazawa S, Sugano Y, et al. Highly selective production of hydrogen peroxide on graphitic carbon nitride (g-C3N4) photocatalyst activated by visible light[J]. Acs Catalysis, 2016,4(3):774-780.
[18]
Adesanya V O, Davey M P, Scott S A, et al. Water-assisted production of honeycomb-like g-C3N4 nanostructure with ultralong carrier lifetime and outstanding photocatalytic activity[J]. Nanoscale, 2015,7(6):2471-2479.
[19]
Shi L, Lin L, Wang F, et al. Enhanced visible-light photocatalytic activity and stability over g-C3N4/Ag2CO3 composites[J]. Journal of Materials Science, 2015,50(4):1718-1727.
[20]
Liu Q, Chen T, Guo Y, et al. Ultrathin g-C3N4, nanosheets coupled with carbon nanodots as 2D/0D composites for efficient photocatalytic H2 evolution[J]. Applied Catalysis B Environmental, 2016,193:248-258.
[21]
Li Y, Jin R, Xu F, et al. In situ, loading of Ag2WO4, on ultrathin g-C3N4, nanosheets with highly enhanced photocatalytic performance[J]. Journal of Hazardous Materials, 2016,313:219-228.
[22]
Song W, Cooper W J, Mezyk S P, et al. Free Radical Destruction of β-Blockers in Aqueous Solution[J]. Environmental Science & Technology, 2008,42(4):1256-1261.
[23]
Hu C, Peng T, Hu X, et al. Plasmon-induced photodegradation of toxic pollutants with Ag-AgI/Al2O3 under visible-light irradiation[J]. Journal of the American Chemical Society, 2010, 132(2):857.
[24]
Wang W, Yu Y, An T, et al. Visible-Light-Driven Photocatalytic Inactivation of E. coli K-12by Bismuth Vanadate Nanotubes:Bactericidal Performance and Mechanism[J]. Environmental Science & Technology, 2012,46(8):4599-4606.
[25]
Lu X, Xu K, Chen P, et al. Facile one step method realizing scalable production of g-C3N4nanosheets and study of their photocatalytic H2evolution activity[J]. Journal of Materials Chemistry A, 2014,2(44):18924-18928.
[26]
孟雅丽. g-C3N4的合成及其光催化研究[D]. 大连:大连理工大学, 2011.
[27]
Sarat S, Sammes N, Smirnova A. Bismuth oxide doped scandiastabilized zirconia electrolyte for the intermediate temperature solid oxide fuel cells[J]. Journal of Power Sources, 2006,160(2):892-896.
[28]
Cui Y, Zhang G, Lin Z, et al. Condensed and Low-defected graphitic carbon nitride with enhanced photocatalytic hydrogen evolution under visible light irradiation[J]. Applied Catalysis B Environmental, 2016,181:413-419.
[29]
Fina F, Callear S K, Carins G M, et al. Structural investigation of graphitic carbon nitride via XRD and neutron diffraction[J]. Chemistry of Materials, 2015,27(7):2612-2618.
[30]
Zhang Y, Han C, Zhang G, et al. PEG-assisted synthesis of crystal TiO2, nanowires with high specific surface area for enhanced photocatalytic degradation of atrazine[J]. Chemical Engineering Journal, 2015,268:170-179.
[31]
Wang Y, Li Y, Bai X, et al. Facile synthesis of Y-doped graphitic carbon nitride with enhanced photocatalytic performance[J]. Catalysis Communications, 2016,84(33):179-182.
[32]
Maeda K, Kuriki R, Zhang M, et al. The effect of the pore-wall structure of carbon nitride on photocatalytic CO2 reduction under visible light[J]. Journal of Materials Chemistry A, 2014,2(36):15146-15151.
[33]
Wang F, Chen P, Feng Y, et al. Facile synthesis of N-doped carbon dots/g-C3N4, photocatalyst with enhanced visible-light photocatalytic activity for the degradation of indomethacin[J]. Applied Catalysis B:Environmental, 2017,207:103-113.
[34]
Cao S W, Liu X F, Yuan Y P, et al. Artificial photosynthetic hydrogen evolution over g-C3N4 nanosheets coupled with cobaloxime[J]. Physical Chemistry Chemical Physics Pccp, 2013, 15(42):18363.
[35]
Niu P, Zhang L, Liu G, et al. Graphene-Like carbon nitride nanosheets for improved photocatalytic activities[J]. Advanced Functional Materials, 2012,22(22):4763-4770.
[36]
Kim Y H, Ogata T, Nakano Y. Kinetic analysis of palladium (Ⅱ) adsorption process on condensed-tannin gel based on redox reaction models[J]. Water Research, 2007,41(14):3043-3050.
[37]
Mendret J, Hatat-Fraile M, Rivallin M, et al. Influence of solution pH on the performance of photocatalytic membranes during dead-end filtration[J]. Separation & Purification Technology, 2013,118(6):406-414.
[38]
Zhu B, Xia P, Ho W, et al. Isoelectric point and adsorption activity of porous g-C3N4[J]. Applied Surface Science, 2015, 344:188-195.
Ng J, Wang X, Sun D D. One-pot hydrothermal synthesis of a hierarchical nanofungus-like anatase TiO2 thin film for photocatalytic oxidation of bisphenol A[J]. Applied Catalysis B Environmental, 2011,110(45):260-272.
[42]
Hu X, Ji H, Chang F, et al. Simultaneous photocatalytic Cr(VI) reduction and 2,4,6-TCP oxidation over g-C3N4, under visible light irradiation[J]. Catalysis Today, 2014,224(4):34-40.
[43]
Wu D, Wang B, Wang W, et al. Visible-light-driven BiOBr nanosheets for highly facet-dependent photocatalytic inactivation of Escherichia coli[J]. Journal of Materials Chemistry A, 2015,3(29):15148-15155.
