多孔MoS_2/g-C_3N_4材料对水环境中四环素的降解
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摘要
通过浸渍-高温煅烧法制备多孔MoS_2/g-C_3N_4光催化剂,采用X射线衍射(XRD)、透射电子显微镜(TEM)、扫描电子显微镜(SEM)、N2吸附-解吸、紫外-可见光(UV-vis)漫反射吸收光谱对材料进行表征;并在可见光照射下,对四环素(TC)进行光催化降解。结果表明,催化剂量为2.0 g·L-1、pH为5.0时,对TC的去除效果最好,可见光照射180 min,MoS_2/g-C_3N_4(1.0%-MC)复合材料对TC的降解率可达80.6%。反应完成后,复合材料循环利用5次,其降解效率仍保持在70.0%以上。浸渍-高温煅烧法所制备的MoS_2/g-C_3N_4光催化剂具有良好的应用前景。
The unique porous MoS_2/g-C_3N_4 heterojunction photocatalyst was successfully constructed by a facile impregnation and calcination method. The obtained MoS_2/g-C_3N_4 composites were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), N2 adsorptiondesorption, and ultraviolet-visible(UV-vis) diffuse reflection spectroscopy. Then it was used to photocatalytic degrade tetracycline(TC) under visible light irradiation. The results showed that the optimum TC degradation effect was achieved at MoS_2/g-C_3N_4(1.0%-MC) dosage of 2.0 g·L-1 and pH 5.0. After 180 min visible light irradiation, the removal rate of TC reached 80.6%. The used MoS_2/g-C_3N_4 could be recycled for 5 times, and its degradation rate for TC maintained above 70.0%. The MoS_2/g-C_3N_4 composites prepared by facile impregnation and calcination method have a good application prospect.
The unique porous MoS_2/g-C_3N_4 heterojunction photocatalyst was successfully constructed by a facile impregnation and calcination method. The obtained MoS_2/g-C_3N_4 composites were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), N2 adsorptiondesorption, and ultraviolet-visible(UV-vis) diffuse reflection spectroscopy. Then it was used to photocatalytic degrade tetracycline(TC) under visible light irradiation. The results showed that the optimum TC degradation effect was achieved at MoS_2/g-C_3N_4(1.0%-MC) dosage of 2.0 g·L-1 and pH 5.0. After 180 min visible light irradiation, the removal rate of TC reached 80.6%. The used MoS_2/g-C_3N_4 could be recycled for 5 times, and its degradation rate for TC maintained above 70.0%. The MoS_2/g-C_3N_4 composites prepared by facile impregnation and calcination method have a good application prospect.
引文
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[2] WAMMER K H, SLATTERY M T, STEMIG A M, et al. Tetracycline photolysis in natural waters:Loss of antibacterial activity[J]. Chemosphere, 2011, 85:1505-1510.
[3] DAGHRIR R, DROGUI P. Tetracycline antibiotics in the environment:A review[J]. Environmental Chemistry Letters, 2013,11:209-227.
[4] JIANG W T, CHANG P H, WANG Y S, et al. Sorption and desorption of tetracycline on layered manganese dioxide birnessite[J]. International Journal of Environmental Science&Technology, 2015, 12(5):1695-1704.
[5]邓玉,倪福全.水环境中抗生素残留及其危害[J].南水北调与水利科技, 2011, 9(3):96-100.
[6] KIM I, TANAKA H. Photodegradation characteristics of PPCPs in water with UV treatment[J]. Environment International,2009, 35(5):793-802.
[7] LóPEZ-PE?ALVER J J, SáNCHEZ-POLO M, GóMEZ-PACHECO C V, et al. Photodegradation of tetracyclines in aqueous solu?tion byusingUV andUV/H2O2oxidationprocesses[J].JournalofChemicalTechnology&Biotechnology,2010,85(10):1325-1333.
[8] HOMEM V, SANTOS L. Degradation and removal methods of antibiotics from aqueous matrices:A review[J]. Journal of Envi?ronmental Management, 2011, 92(10):2304-2347.
[9] LI J, LIU E, MA Y, et al. Synthesis of MoS2/g-C3N4nanosheets as 2D heterojunction photocatalysts with enhanced visible light activity[J]. Applied Surface Science, 2016, 364:694-702.
[10] CAO Y, GAO Q, LI Q, et al. Synthesis of 3D porous MoS2/g-C3N4heterojunction as a high efficiency photocatalyst for boost?ing H2evolution activity[J]. RSC Advances, 2017, 7(65):40727-40733.
[11] MBOULA V M, HéQUET V, GRU Y, et al. Assessment of the efficiency of photocatalysis on tetracycline biodegradation[J].Journal of Hazardous Material, 2012, 209-210(4):355-364.
[12] HU J, CHENG W, HUANG S, et al. First-principles modeling of nonlinear optical properties of C3N4polymorphs[J]. Applied Physics Letters, 2006, 89(26):841-853.
[13] CHEN Y, LIN B, WANG H, et al. Surface modification of g-C3N4by hydrazine:Simple way for noble-metal free hydrogen evo?lution catalysts[J]. Chemical Engineering Journal, 2016, 286:339-346.
[14] PATNAIK S, MARTHA S, PARIDA K M. An overview of the structural, textural and morphological modulations of g-C3N4to?wards photocatalytic hydrogen production[J]. RSC Advances, 2016, 6(52):46929-46951.
[15] LU D, WANG H, ZHAO X, et al. Highly efficient visible-light-induced photoactivity of Z-scheme g-C3N4/Ag/MoS2ternary photocatalysts for organic pollutant degradation and production of hydrogen[J]. ACS Sustainable Chemistry&Engineering,2017, 5(2):1436-1445.
[16] LI H, YIN Z, HE Q, et al. Fabrication of single-and multilayer MoS2film-based field-effect transistors for sensing NO at room temperature[J]. Small, 2012, 8(1):63-67.
[17] HWANG H, KIM H, CHO J. MoS2nanoplates consisting of disordered graphene-like layers for high rate lithium battery an?ode materials[J]. Nano Letters, 2013, 11(11):4826-4830.
[18] HOU Y D, LAURSEN A B, ZHANG J S, et al. Layered nanojunctions for hydrogen-evolution catalysis[J]. Angewandte Che?mie International Edition, 2013, 52(13):3621-3625.
[19] ANSARI S A, CHO M H. Simple and large scale construction of MoS2-g-C3N4heterostructures using mechanochemistry for high performance electrochemical supercapacitor and visible light photocatalytic applications[J]. Scientific Reports, 2017, 7:43055-43065.
[20] LI N, ZHOU J, SHENG Z, et al. Molten salt-mediated formation of g-C3N4-MoS2, for visible-light-driven photocatalytic hydro?gen evolution[J]. Applied Surface Science, 2017, 430:218-224.
[21] TIAN Y, GE L, WANG K, et al. Synthesis of novel MoS2/g-C3N4, heterojunction photocatalysts with enhanced hydrogen evolu?tion activity[J]. Materials Characterization, 2014, 87(17):70-73.
[22] LI Q, ZHANG N, YANG Y, et al. High efficiency photocatalysis for pollutant degradation with MoS2/C3N4heterostructures[J].Langmuir, 2014, 30(29):8965-8972.
[23] AHMADI M, RAMEZANI M H, JAAFARZADEH N, et al. Enhanced photocatalytic degradation of tetracycline and real phar?maceutical wastewater using MWCNT/TiO2nano-composite[J]. Journal of Environmental Management, 2017, 186:55-63.
[24] WANG P, YAP P S, LIM T T. C-N-S tridoped TiO2for photocatalytic degradation of tetracycline under visible-light irradia?tion[J]. Applied Catalysis A:General, 2011, 399(1):252-261.
[25] WANG Y, ZHANG H, CHEN L. Ultrasound enhanced catalytic ozonation of tetracycline in a rectangular air-lift reactor[J].Catalysis Today, 2011, 175(1):283-292.
[2] WAMMER K H, SLATTERY M T, STEMIG A M, et al. Tetracycline photolysis in natural waters:Loss of antibacterial activity[J]. Chemosphere, 2011, 85:1505-1510.
[3] DAGHRIR R, DROGUI P. Tetracycline antibiotics in the environment:A review[J]. Environmental Chemistry Letters, 2013,11:209-227.
[4] JIANG W T, CHANG P H, WANG Y S, et al. Sorption and desorption of tetracycline on layered manganese dioxide birnessite[J]. International Journal of Environmental Science&Technology, 2015, 12(5):1695-1704.
[5]邓玉,倪福全.水环境中抗生素残留及其危害[J].南水北调与水利科技, 2011, 9(3):96-100.
[6] KIM I, TANAKA H. Photodegradation characteristics of PPCPs in water with UV treatment[J]. Environment International,2009, 35(5):793-802.
[7] LóPEZ-PE?ALVER J J, SáNCHEZ-POLO M, GóMEZ-PACHECO C V, et al. Photodegradation of tetracyclines in aqueous solu?tion byusingUV andUV/H2O2oxidationprocesses[J].JournalofChemicalTechnology&Biotechnology,2010,85(10):1325-1333.
[8] HOMEM V, SANTOS L. Degradation and removal methods of antibiotics from aqueous matrices:A review[J]. Journal of Envi?ronmental Management, 2011, 92(10):2304-2347.
[9] LI J, LIU E, MA Y, et al. Synthesis of MoS2/g-C3N4nanosheets as 2D heterojunction photocatalysts with enhanced visible light activity[J]. Applied Surface Science, 2016, 364:694-702.
[10] CAO Y, GAO Q, LI Q, et al. Synthesis of 3D porous MoS2/g-C3N4heterojunction as a high efficiency photocatalyst for boost?ing H2evolution activity[J]. RSC Advances, 2017, 7(65):40727-40733.
[11] MBOULA V M, HéQUET V, GRU Y, et al. Assessment of the efficiency of photocatalysis on tetracycline biodegradation[J].Journal of Hazardous Material, 2012, 209-210(4):355-364.
[12] HU J, CHENG W, HUANG S, et al. First-principles modeling of nonlinear optical properties of C3N4polymorphs[J]. Applied Physics Letters, 2006, 89(26):841-853.
[13] CHEN Y, LIN B, WANG H, et al. Surface modification of g-C3N4by hydrazine:Simple way for noble-metal free hydrogen evo?lution catalysts[J]. Chemical Engineering Journal, 2016, 286:339-346.
[14] PATNAIK S, MARTHA S, PARIDA K M. An overview of the structural, textural and morphological modulations of g-C3N4to?wards photocatalytic hydrogen production[J]. RSC Advances, 2016, 6(52):46929-46951.
[15] LU D, WANG H, ZHAO X, et al. Highly efficient visible-light-induced photoactivity of Z-scheme g-C3N4/Ag/MoS2ternary photocatalysts for organic pollutant degradation and production of hydrogen[J]. ACS Sustainable Chemistry&Engineering,2017, 5(2):1436-1445.
[16] LI H, YIN Z, HE Q, et al. Fabrication of single-and multilayer MoS2film-based field-effect transistors for sensing NO at room temperature[J]. Small, 2012, 8(1):63-67.
[17] HWANG H, KIM H, CHO J. MoS2nanoplates consisting of disordered graphene-like layers for high rate lithium battery an?ode materials[J]. Nano Letters, 2013, 11(11):4826-4830.
[18] HOU Y D, LAURSEN A B, ZHANG J S, et al. Layered nanojunctions for hydrogen-evolution catalysis[J]. Angewandte Che?mie International Edition, 2013, 52(13):3621-3625.
[19] ANSARI S A, CHO M H. Simple and large scale construction of MoS2-g-C3N4heterostructures using mechanochemistry for high performance electrochemical supercapacitor and visible light photocatalytic applications[J]. Scientific Reports, 2017, 7:43055-43065.
[20] LI N, ZHOU J, SHENG Z, et al. Molten salt-mediated formation of g-C3N4-MoS2, for visible-light-driven photocatalytic hydro?gen evolution[J]. Applied Surface Science, 2017, 430:218-224.
[21] TIAN Y, GE L, WANG K, et al. Synthesis of novel MoS2/g-C3N4, heterojunction photocatalysts with enhanced hydrogen evolu?tion activity[J]. Materials Characterization, 2014, 87(17):70-73.
[22] LI Q, ZHANG N, YANG Y, et al. High efficiency photocatalysis for pollutant degradation with MoS2/C3N4heterostructures[J].Langmuir, 2014, 30(29):8965-8972.
[23] AHMADI M, RAMEZANI M H, JAAFARZADEH N, et al. Enhanced photocatalytic degradation of tetracycline and real phar?maceutical wastewater using MWCNT/TiO2nano-composite[J]. Journal of Environmental Management, 2017, 186:55-63.
[24] WANG P, YAP P S, LIM T T. C-N-S tridoped TiO2for photocatalytic degradation of tetracycline under visible-light irradia?tion[J]. Applied Catalysis A:General, 2011, 399(1):252-261.
[25] WANG Y, ZHANG H, CHEN L. Ultrasound enhanced catalytic ozonation of tetracycline in a rectangular air-lift reactor[J].Catalysis Today, 2011, 175(1):283-292.
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