石墨相氮化碳活化过二硫酸盐降解亚甲基蓝的研究
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摘要
以石墨相氮化碳(g-C_3N_4)为催化剂,在模拟日光条件下活化过二硫酸盐(PDS)降解阳离子染料亚甲基蓝(MB)。结果表明:g-C_3N_4活化PDS能有效降解MB,且当n(PDS)∶n(MB)=20∶1、g-C_3N_4投加质量浓度为1.0 g/L、120 min时,MB降解率最高可达93.2%;初始pH及温度对MB的降解影响不大;自由基猝灭实验表明硫酸根自由基、羟基自由基、超氧自由基和光生电子空穴均为反应的活性物种,且反应主要发生在g-C_3N_4表面。
Using graphitic carbon nitride(g-C_3N_4)as catalyst,under simulated sunlight condition,perdisulfate(PDS)has been activated,and cationic methylene blue(MB)degraded.The results show that g-C_3N_4activated PDS can effectively degrade MB.When n(PDS)∶n(MB)=20∶1,g-C_3N_4dosage mass concentration 1.0 g/L,and reaction time 120 min,the highest MB degradation rate can reach 93.2%.The influences of pH and temperature on MB degradation are small.Free radical quenching experiments show that sulfate radicals,hydroxyl radicals,superoxygen radicals,and photoelectron holes are all active species of the reaction,and the reaction mainly occurs on the surface of g-C_3N_4.
Using graphitic carbon nitride(g-C_3N_4)as catalyst,under simulated sunlight condition,perdisulfate(PDS)has been activated,and cationic methylene blue(MB)degraded.The results show that g-C_3N_4activated PDS can effectively degrade MB.When n(PDS)∶n(MB)=20∶1,g-C_3N_4dosage mass concentration 1.0 g/L,and reaction time 120 min,the highest MB degradation rate can reach 93.2%.The influences of pH and temperature on MB degradation are small.Free radical quenching experiments show that sulfate radicals,hydroxyl radicals,superoxygen radicals,and photoelectron holes are all active species of the reaction,and the reaction mainly occurs on the surface of g-C_3N_4.
引文
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[24]刘海涛,闫宝林,梁小玉,等.溶剂热法合成具有优异光催化降解染料性能的BiOCl纳米片[J].广东化工,2017,44(18):18-20.
[2]Cardoso J C,Bessegato G G,Boldrin Zanoni M V.Efficiency comparison of ozonation,photolysis,photocatalysis and photoelectrocatalysis methods in real textile wastewater decolorization[J].Water Research,2016,98:39-46.
[3]李庄.高浓度染料废水(含偶氮染料废水)处理技术的研究[D].长沙:湖南大学,2001.
[4]Gao Yaowen,Li Simiao,Li Yixi,et al.Accelerated photocatalytic degradation of organic pollutant over metal-organic framework MIL-53(Fe)under visible LED light mediated by persulfate[J].Applied Catalysis B Environmental,2017,202:165-174.
[5]李丽,刘占孟,聂发挥.过硫酸盐活化高级氧化技术在污水处理中的应用[J].华东交通大学学报,2014,31(6):114-118.
[6]Yang Shiying,Yang Xin,Shao Xueting,et al.Activated carbon catalyzed persulfate oxidation of Azo dye acid orange 7 at ambient temperature[J].Journal of Hazardous Materials,2011,186(1):659-666.
[7]Zhang Jun,Shao Xueting,Shi Chao,et al.Decolorization of Acid Orange 7 with peroxymonosulfate oxidation catalyzed by granular activated carbon[J].Chemical Engineering Journal,2013,232(10):259-265.
[8]Yang Shiying,Xiao Tuo,Zhang Jun,et al.Activated carbon fiber as heterogeneous catalyst of peroxymono sulfate activation for efficient degradation of Acid Orange 7 in aqueous solution[J].Separation and Purification Technology,2015,143:19-26.
[9]谢运超.改性氮化碳材料的制备及其光催化性能的研究[D].上海:上海理工大学,2014.
[10]Zheng Yun,Lin Lihua,Wang Bo,et al.Graphitic carbon nitride polymers toward sustainable photoredox catalysis[J].Angewandte Chemie,2016,46(50):12868-12884.
[11]Liang F F,Zhu Y F.Enhancement of mineralization ability for phenol via synergetic effect of photoelectrocatalysis of g-C3N4film[J].Applied Catalysis B Environmental,2016,180:324-329.
[12]Kong Chao,Li Zhen,Lu Gongxuan.Visible photocatalytic water splitting and photocatalytic two-electron oxygen formation over Cuand Fe-doped g-C3N4[J].Journal of Physical Chemistry C,2016,120(1):56-63.
[13]Yan Z P,Sun Z J,Liu X,et al.admium sulfide/graphitic carbon nitride heterostructure nanowire loading with a nickel hydroxide cocatalyst for highly efficient photocatalytic hydrogen production in water under visible light[J].Nanoscale,2016,8(8):4748-4756.
[14]邵啸,尹晓红,杨晓晓,等.类石墨相氮化碳的制备及光催化还原CO2性能研究[J].精细化工,2017,34(1):74-79.
[15]Dong Fan,Wu Liwen,Sun Yanjuan,et al.Efficient synthesis of polymeric g-C3N4layered materials as novel efficient visible light driven photocatalysts[J].Journal of Materials Chemistry,2011,21(39):15171-15174.
[16]李彦芳.镍铁水滑石/石墨烯复合材料的制备及催化性能研究[D].大连:大连理工大学,2016.
[17]赵妍.铁锰材料活化过硫酸盐去除水中难降解有机污染物的机制与效能[D].长春:吉林大学,2017.
[18]张祺.超声强化电活化过硫酸盐去除水中抗生素的研究[D].武汉:华中科技大学,2016.
[19]杨富花,张静,张古承,等.钴锌双金属氧化物催化单过硫酸盐降解酸性橙7的效果研究[J].环境污染与防治,2017,39(9):976-980.
[20]邓景衡,文湘华,李佳喜.碳纳米管负载纳米四氧化三铁多相类芬顿降解亚甲基蓝[J].环境科学学报,2014,34(6):1436-1442.
[21]张钦库,姚秉华,鲁盼,等.In2TiO5纳米带的静电纺丝法制备及光催化性能[J].环境科学学报,2015,35(12):3832-3837.
[22]高永,孔峰,程洁红,等.TiO2光催化-微滤膜分离深度净化亚甲基蓝印染废水[J].环境工程学报,2012,6(10):3585-3590.
[23]闫春燕,路迢,刘斐,等.钒酸铋/氧化石墨烯复合催化剂的制备及性能[J].广州化工,2017,45(19):33-36.
[24]刘海涛,闫宝林,梁小玉,等.溶剂热法合成具有优异光催化降解染料性能的BiOCl纳米片[J].广东化工,2017,44(18):18-20.