羟基氧化镍催化臭氧氧化水中草酸
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摘要
本试验采用过硫酸钾作为氧化剂,氢氧化镍为原料,利用液相氧化法制备羟基氧化镍,并通过X射线衍射(XRD)、扫描电子显微镜(SEM)、傅里叶红外变换光谱(FT-IR)以及热重分析(TGA)对制得产品的理化性质进行分析。采用催化臭氧试验,并控制单一变量,考察羟基氧化镍作为催化剂对草酸的臭氧氧化去除效果,探究不同条件下草酸的去除率,研究了催化剂投加量、臭氧浓度、pH对草酸去除效果的影响。结果表明:与单独臭氧氧化相比,催化臭氧法可以大大提高草酸去除率,反应遵循羟基自由基机理,当催化剂投加量为100 mg/L、臭氧浓度为12.2 mg/L、pH值为3.4时,60 min内草酸去除率最高可以达到92%。
Nickel oxyhydroxide is prepared by liquid phase oxidation by use of K_2 S_2 O_8 and NiOOH as the oxidant and raw material respectively. The characterization of the product is determined by XRD, SEM, Fourier transform infrared spectroscopy and thermogravimetric analysis,and the catalytic performance is investigated in ozonation of oxalic acid. The effects of catalyst dosage,ozone concentration and pH value on the removal of oxalic acid are studied. The results show that nickel oxyhydroxide catalyst enables an interesting improvement of ozonation efficiency during the degradation of oxalic acid compared with ozone alone, and the catalytic ozonation system follows a hydroxyl radical mechanism. The maximum degradation of oxalic acid can reach 92% in 60 min when 100 mg/L catalytic is added with the ozone concentration of 9. 0 mg/L and pH value of 3. 4.
Nickel oxyhydroxide is prepared by liquid phase oxidation by use of K_2 S_2 O_8 and NiOOH as the oxidant and raw material respectively. The characterization of the product is determined by XRD, SEM, Fourier transform infrared spectroscopy and thermogravimetric analysis,and the catalytic performance is investigated in ozonation of oxalic acid. The effects of catalyst dosage,ozone concentration and pH value on the removal of oxalic acid are studied. The results show that nickel oxyhydroxide catalyst enables an interesting improvement of ozonation efficiency during the degradation of oxalic acid compared with ozone alone, and the catalytic ozonation system follows a hydroxyl radical mechanism. The maximum degradation of oxalic acid can reach 92% in 60 min when 100 mg/L catalytic is added with the ozone concentration of 9. 0 mg/L and pH value of 3. 4.
引文
[1]吴光国,谢勇冰,邢林林,等.改性活性炭强化催化臭氧氧化降解草酸[J].过程工程学报,2012,12(4):684-689.
[2]臧兴杰,张华,石锐,等.Mn(Ⅱ)/O_3降解草酸作用机制的定量化解析[J].化工学报,2009,60(2):428-434.
[3]杨玉飞,黄远星,姚吉,等.载锰氮化碳催化臭氧法降解水中草酸研究[J].水资源与水工程学报,2017,28(1):45-49.
[4]常照荣,上官恩波,吴锋,等.羟基氧化镍的制备及应用[J].材料导报,2007,21(6):39-42.
[5]Bader H,HoignéJ.Determination of ozone in water by the indigo method[J].Water Research,1981,15(4):449-456.
[6]王北平.经基氧化镍的液相法制备工艺及电化学性能的研究[D].昆明:昆明理工大学,2007.
[7]韩恩山,康红欣,魏子海,等.混合晶相氢氧化镍的合成和性能研究[J].电源技术,2007,31(5):396-399.
[8]刘澧浦,周震涛.纳米γ米NiOOH的制备、结构与性能[J].电源技术,2007,31(3):228-232.
[9]王新,陈忠,廖代伟.镁掺杂羟基氧化镍的制备、结构和电化学性能[J].电源技术,2009,33(1):33-36.
[10]Ren Y,Dong Q,Feng J,et al.Magnetic porous ferrospinel NiFe_2O_4:A novel ozonation catalysl with strong catalytic property for degradation of Di-N-Butyl Phthalate and convenient separation from water[J].Journal of Colloid and Interface Science,2013,382(1):90-96.
[11]Kasprzyk-Hordern B,Ziótek M,Nawrocki J.Catalytic ozonation and methods of enhancing molecular ozone reactions in water treatment[J].Applied Catalysis B Environmental,2003,46(4):639-669.
[12]Elizarova G L,Zhidomirov G M,Parmon V N.Hydroxides of transition metals as artificial catalysts for oxidation of water to dioxygen[J].Catalysis Today,2001,31(33):71-88.
[13]周宁娟,薛罡,卜聃,等.经基化锌催化臭氧氧化去除水中痕量磺胺嘧啶[J].中国环境科学,2011,31(2):233-238.
[14]夏熙,龚玉良.纳米β米NiOOH的固相合成及其性能[J].电池,2002,32(1):6-9.
[15]陈忠林,徐贞贞,贲岳,等.ZnOOH/O_3催化臭氧化体系去除水中痕量对氯硝基苯[J].环境科学,2007,28(11):2550-2556.
[16]Li X,Zhang Q,Tang L,et al.Catalytic ozonation of P-chlorobenzoic acid by activated carbon and nickel supported activated carbon prepared from petroleum coke[J].Journal of Hazardous Materials,2009,163(1):115-120.
[17]张静,杨忆新,马军,等.CoO_x-TiO_2催化臭氧氧化草酸的研究[J].中国环境科学,2014,34(6):1457-1462.
[18]Chen C,Yu J,Yoza B A,et al.A novel"wastes-treat-wastes"technology:Role and potential of spent fluid catalytic cracking catalyst assisted ozonation of petrochemical wastewater[J].Journal of Environmental Management,2015,152(1):58-65.
[2]臧兴杰,张华,石锐,等.Mn(Ⅱ)/O_3降解草酸作用机制的定量化解析[J].化工学报,2009,60(2):428-434.
[3]杨玉飞,黄远星,姚吉,等.载锰氮化碳催化臭氧法降解水中草酸研究[J].水资源与水工程学报,2017,28(1):45-49.
[4]常照荣,上官恩波,吴锋,等.羟基氧化镍的制备及应用[J].材料导报,2007,21(6):39-42.
[5]Bader H,HoignéJ.Determination of ozone in water by the indigo method[J].Water Research,1981,15(4):449-456.
[6]王北平.经基氧化镍的液相法制备工艺及电化学性能的研究[D].昆明:昆明理工大学,2007.
[7]韩恩山,康红欣,魏子海,等.混合晶相氢氧化镍的合成和性能研究[J].电源技术,2007,31(5):396-399.
[8]刘澧浦,周震涛.纳米γ米NiOOH的制备、结构与性能[J].电源技术,2007,31(3):228-232.
[9]王新,陈忠,廖代伟.镁掺杂羟基氧化镍的制备、结构和电化学性能[J].电源技术,2009,33(1):33-36.
[10]Ren Y,Dong Q,Feng J,et al.Magnetic porous ferrospinel NiFe_2O_4:A novel ozonation catalysl with strong catalytic property for degradation of Di-N-Butyl Phthalate and convenient separation from water[J].Journal of Colloid and Interface Science,2013,382(1):90-96.
[11]Kasprzyk-Hordern B,Ziótek M,Nawrocki J.Catalytic ozonation and methods of enhancing molecular ozone reactions in water treatment[J].Applied Catalysis B Environmental,2003,46(4):639-669.
[12]Elizarova G L,Zhidomirov G M,Parmon V N.Hydroxides of transition metals as artificial catalysts for oxidation of water to dioxygen[J].Catalysis Today,2001,31(33):71-88.
[13]周宁娟,薛罡,卜聃,等.经基化锌催化臭氧氧化去除水中痕量磺胺嘧啶[J].中国环境科学,2011,31(2):233-238.
[14]夏熙,龚玉良.纳米β米NiOOH的固相合成及其性能[J].电池,2002,32(1):6-9.
[15]陈忠林,徐贞贞,贲岳,等.ZnOOH/O_3催化臭氧化体系去除水中痕量对氯硝基苯[J].环境科学,2007,28(11):2550-2556.
[16]Li X,Zhang Q,Tang L,et al.Catalytic ozonation of P-chlorobenzoic acid by activated carbon and nickel supported activated carbon prepared from petroleum coke[J].Journal of Hazardous Materials,2009,163(1):115-120.
[17]张静,杨忆新,马军,等.CoO_x-TiO_2催化臭氧氧化草酸的研究[J].中国环境科学,2014,34(6):1457-1462.
[18]Chen C,Yu J,Yoza B A,et al.A novel"wastes-treat-wastes"technology:Role and potential of spent fluid catalytic cracking catalyst assisted ozonation of petrochemical wastewater[J].Journal of Environmental Management,2015,152(1):58-65.