CuWO_4促进TiO_2光催化降解水中阿特拉津
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摘要
以一种简单的方法制备CuWO_4,并研究了CuWO_4促进Ti O_2光催化降解水中阿特拉津的效能及可能机理。结果表明,反应体系加入少量(50 mg/L)CuWO_4显著加快Ti O_2光催化降解水中阿特拉津,反应270 min降解率达92.1%,较单一Ti O_2催化效率提高1.94倍;CuWO_4在降解过程中显示出较强的稳定性,溶液中微量溶解的Cu~(2+)接收电子形成Cu(II)/Cu(I)的价态变化;随CuWO_4煅烧温度(100～800℃)的升高降解率先增大后下降,500℃达到最大,而Cu~(2+)溶出率则显著降低,CuWO_4-Ti O_2催化体系的正效应归功于固态CuWO_4;光生电子及HO~·自由基及光生电子在反应体系中起主要作用。实验结果有助于其他Cu基半导体提升Ti O_2催化活性的研究。
CuWO_4was prepared by a simple method,and Cu WO_4improving photocatalytic degradation for atrazine by Ti O_2as well as the possible mechanism was studied.Results showed that,an addition of a small amount of CuWO_4(50 mg/L)into the reaction system could significantly enhance the efficiency of atrazine degradation,resulting in an increased degradation efficiency of 92.1%after 270 min,which was 1.94 times higher than that of the single TiO_2.CuWO_4showed robust stability and the slight dissolved Cu~(2+)received e-forming behavior of Cu(II)/Cu(I)during the photocatalytic process.As the sintering temperate of Cu WO_4increased(100～800℃),the degradation efficiency of atrazine increased initially and then deceased,the maximum reached at500℃,but the dissolution rate of Cu~(2+)decreased significantly.The origin of high phtotocatalytic effect of TiO_2-CuWO_4was attributed to the introduction of solid Cu WO_4.The photo-induced electron and HO~·radical played an important role in this reaction system.The experimental results were conductive to the research of improving photocatalytic activity of TiO_2with Cu-bearing semiconductors.
CuWO_4was prepared by a simple method,and Cu WO_4improving photocatalytic degradation for atrazine by Ti O_2as well as the possible mechanism was studied.Results showed that,an addition of a small amount of CuWO_4(50 mg/L)into the reaction system could significantly enhance the efficiency of atrazine degradation,resulting in an increased degradation efficiency of 92.1%after 270 min,which was 1.94 times higher than that of the single TiO_2.CuWO_4showed robust stability and the slight dissolved Cu~(2+)received e-forming behavior of Cu(II)/Cu(I)during the photocatalytic process.As the sintering temperate of Cu WO_4increased(100～800℃),the degradation efficiency of atrazine increased initially and then deceased,the maximum reached at500℃,but the dissolution rate of Cu~(2+)decreased significantly.The origin of high phtotocatalytic effect of TiO_2-CuWO_4was attributed to the introduction of solid Cu WO_4.The photo-induced electron and HO~·radical played an important role in this reaction system.The experimental results were conductive to the research of improving photocatalytic activity of TiO_2with Cu-bearing semiconductors.
引文
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[11] WAN L, SHENG J, CHEN H et al. Different recycle behavior of Cu2+and Fe3+ions for phenol photodegradation over TiO2and WO3[J].Journal of Hazardous Materials,2013,262:114-120.
[12] XU S, SUN D. Significant improvement of photocatalytic hydrogen generation rate over Ti O2with deposited Cu O[J].International Journal of Hydrogen Energy,2009,34:6096-6104.
[13] LIMA A E B, COSTA M J S, Santos R S et al. Facile preparation of CuWO4porousfilms and their photoelectrochemical properties[J].Electrochimica Acta,2017,256:139-145.
[14] YOUREY J E, PYPER K J, KURTZ J B, et al. Chemical stability of CuWO4for photoelectrochemical water oxidation[J].Journal of Physical Chemistry:C,2013,117:8708-8718.
[15] CHEN H, LENG W, XU Y. Enhanced visible-light photoactivity of CuWO4through a surface-deposited CuO[J].Journal of Physical Chemistry:C,2014,118:9982-9989.
[16]皮云正,王建龙.N,N-二乙基对苯二胺/辣根过氧化物酶法测定过氧化氢浓度时臭氧干扰的消除[J].分析化学,2005,33(10):1516.
[17] PAN C S, ZHU Y F. New type of BiPO4oxy-acid salt photocatalyst with high photocatalytic activity on degradation of dye[J].Environmental Science&Technology,2010,44:5570-5574.
[18] XIONG X Q, CHEN H H, XU Y M. Improved ptotocatalytic activity of Ti O2on the addition of Cu WO4[J].J Phys Chem C,2015,119:5946-5953.
[2] DALRYMPLE O K, YEH D H, Trotz M A. Removing pharmaceuticals and endocrine-disrupting compounds from wastewater by photocatalysis[J].Journal of Chemical Technology and Biotechnology,2007,82:121-134.
[3]银洲,张建强.二氧化钛光催化降解环境内分泌干扰物技术的研究进展[J].水处理技术,2013,39(1):24-28.
[4]黄兵华,张晓飞,宋磊,等.TiO2光催化水处理技术综述[J].水处理技术,2014,40(12):11-21.
[5] SCHNEIDER J, MATSUOKA M, TAKEUCHI M. Understanding Ti O2Photocatalysis:Mechanisms and Materials[J].Chemical Reviews,2014,114:9919-9986.
[6] CHEN X, MAO S S, Titanium dioxide nanomaterials:synthesis,properties, modifications, and applications[J].Chemical Reviews,2007,107:2891-2959.
[7] LOW J, YU J. Heterojunction Photocatalysts[J].Advanced Materials,2017,29:1601694.
[8] DENG D, NOVOSELOV K S, FU Q et al. Catalysis with twodimensional materials and their heterostructures[J].Nature NanoTechnology,2016,11:218-229.
[9] LAM S W, HERMAWAN M, COLEMAN H W, et al. The role of Copper(II)ions in the photocatalytic oxidation of 1,4-dixoane[J].Journal of Molecular Catalysis A:Chemical,2007,278:152-159.
[10] MOHAMED H H, MENDIVE C B, DILLERT R et al. Kinetic and mechanistic investigations of multielectron transfer reactions induced by stored electrons inTiO2nanoparticles:A stopped flow study[J].The Journal of Physical Chemistry A,2011,115:2139?2147.
[11] WAN L, SHENG J, CHEN H et al. Different recycle behavior of Cu2+and Fe3+ions for phenol photodegradation over TiO2and WO3[J].Journal of Hazardous Materials,2013,262:114-120.
[12] XU S, SUN D. Significant improvement of photocatalytic hydrogen generation rate over Ti O2with deposited Cu O[J].International Journal of Hydrogen Energy,2009,34:6096-6104.
[13] LIMA A E B, COSTA M J S, Santos R S et al. Facile preparation of CuWO4porousfilms and their photoelectrochemical properties[J].Electrochimica Acta,2017,256:139-145.
[14] YOUREY J E, PYPER K J, KURTZ J B, et al. Chemical stability of CuWO4for photoelectrochemical water oxidation[J].Journal of Physical Chemistry:C,2013,117:8708-8718.
[15] CHEN H, LENG W, XU Y. Enhanced visible-light photoactivity of CuWO4through a surface-deposited CuO[J].Journal of Physical Chemistry:C,2014,118:9982-9989.
[16]皮云正,王建龙.N,N-二乙基对苯二胺/辣根过氧化物酶法测定过氧化氢浓度时臭氧干扰的消除[J].分析化学,2005,33(10):1516.
[17] PAN C S, ZHU Y F. New type of BiPO4oxy-acid salt photocatalyst with high photocatalytic activity on degradation of dye[J].Environmental Science&Technology,2010,44:5570-5574.
[18] XIONG X Q, CHEN H H, XU Y M. Improved ptotocatalytic activity of Ti O2on the addition of Cu WO4[J].J Phys Chem C,2015,119:5946-5953.
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