碱性水钠锰矿氧化Cr(Ⅲ)的影响因素研究
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摘要
采用氧化还原法合成3个不同氧化度的碱性水钠锰矿,并表征其晶体结构、比表面积和表面化学性质,探讨其对Cr(Ⅲ)的氧化及影响因素。研究表明:随着合成反应的n(Mn7+)/n(Mn2+)逐渐减小,合成碱性水钠锰矿的氧化度和比表面积逐渐减小,其PZC逐渐升高。反应时间和反应条件(p H、Cr(Ⅲ)浓度和矿物用量)均影响碱性水钠锰矿对Cr(Ⅲ)的氧化。在低p H值范围内Cr(Ⅲ)氧化率随着p H的增加逐渐增加,但在高p H值范围内氧化率随着p H的升高而减小。此外,Cr(Ⅲ)的氧化率随着Cr(Ⅲ)浓度的升高逐渐降低,但随着氧化度的提高显著增加。
Alkaline birnessite had been synthesized by an oxidation-reduction method,and its crystal structure,specific surface area and surface chemical property were characterized. The influencing factors of Cr( Ⅲ) oxidation by alkaline birnessite was also studied. The results indicated with decrease of Mn7 +/ Mn2 +in synthetic method,the AOS and specific surface area of synthetic birnessite decreased,but the PZC of synthetic birnessite increased. The effect of reaction conditions( p H,concentration of Cr( Ⅲ),birnessite loadings and AOS) was studied. The oxidation rate of Cr( Ⅲ) increased with the increase of p H in the low p H range,but it decreased with the increase of p H in high p H range. In addition,the oxidation rate of Cr( Ⅲ) decreased with the increase of concentration of Cr( Ⅲ),but it increased with the increase of birnessite loadings and AOS respectively.
Alkaline birnessite had been synthesized by an oxidation-reduction method,and its crystal structure,specific surface area and surface chemical property were characterized. The influencing factors of Cr( Ⅲ) oxidation by alkaline birnessite was also studied. The results indicated with decrease of Mn7 +/ Mn2 +in synthetic method,the AOS and specific surface area of synthetic birnessite decreased,but the PZC of synthetic birnessite increased. The effect of reaction conditions( p H,concentration of Cr( Ⅲ),birnessite loadings and AOS) was studied. The oxidation rate of Cr( Ⅲ) increased with the increase of p H in the low p H range,but it decreased with the increase of p H in high p H range. In addition,the oxidation rate of Cr( Ⅲ) decreased with the increase of concentration of Cr( Ⅲ),but it increased with the increase of birnessite loadings and AOS respectively.
引文
[1]Landrot G,Ginder-Vogel M,Livi K,et al.Chromium(Ⅲ)oxidation by three poorly-crystalline manganese(IV)oxides.1.chromium(Ⅲ)-oxidizing capacity[J].Environmental Science&Technology,2012,46(21):11594-11600.
[2]张晓辉,曹奇光,谢国莉,等.不同还原剂处理实验室Cr(Ⅵ)废水研究[J].环境工程,2014,32(6):61-64.
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[8]董长勋,潘根兴,兰叶青.溶液p H和吸附离子对水相中δ-Mn O2氧化Cr(Ⅲ)的影响研究[J].生态环境,2006,15(1):27-31.
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[10]董长勋,戴儒南,熊建军.δ-Mn O2对Cr(Ⅲ)氧化动力学特征[J].环境科学,2010,31(5):1395-1401.
[11]王强,刘双营,黄玉明,等.水钠锰矿对Cr(Ⅲ)离子的吸附解吸及氧化行为[J].土壤学报,2010,47(1):64-70.
[12]赵怀燕,龚爱蓉,殷辉,等.模拟表生环境水钠锰矿亚结构转化及钙锰矿的形成[J].地球科学(中国地质大学学报),2014,39(2):227-239.
[13]Landrot G,Ginder-Vogel M,Livi K,et al.Chromium(Ⅲ)oxidation by three poorly crystalline manganese(IV)oxides.2.solid phase analyses[J].Environmental Science&Technology,2012,46(21):11601-11609.
[14]徐佳丽,张芬,刘凡,等.不同氧化度碱性水钠锰矿氧化As(Ⅲ)和Cr(Ⅲ)的动力学特性[J].岩石矿物学杂志,2013,32(6):975-984.
[15]Landrot G,Ginder-Vogel MSparks D L.Kinetics of Chromium(Ⅲ)oxidation by Manganese(IV)oxides using quick scanning Xray absorption fine structure spectroscopy(Q-XAFS)[J].Environmental Science&Technology,2010,44(1):143-149.
[16]Chen Y,Chen Y,Lin Q,et al.Factors affecting Cr(Ⅲ)oxidation by manganese oxides[J].Pedosphere,1997(2):185-192.
[17]陈英旭,朱祖祥,何增耀.环境中氧化锰对Cr(Ⅲ)氧化机理的研究[J].环境科学学报,1993,13(1):45-50.
[18]谭文峰,刘凡,李学垣,等.几种土壤铁锰结核对Cr(Ⅲ)的氧化特性(Ⅰ):氧化锰矿物类型与吸附态离子的影响[J].环境科学学报,2001,21(5):592-596.
[2]张晓辉,曹奇光,谢国莉,等.不同还原剂处理实验室Cr(Ⅵ)废水研究[J].环境工程,2014,32(6):61-64.
[3]Feng X H,Zhai L M,Tan W F,et al.The controlling effect of p H on oxidation of Cr(Ⅲ)by manganese oxide minerals[J].Journal of Colloid and Interface Science,2006,298(1):258-266.
[4]Wang Y,Feng X,Villalobos M,et al.Sorption behavior of heavy metals on birnessite:Relationship with its Mn average oxidation state and implications for types of sorption sites[J].Chemical Geology,2012,292/293:25-34.
[5]Zhang Q,Cheng X D,Zheng C,et al.Roles of manganese oxides in degradation of phenol under UV-Vis irradiation:Adsorption,oxidation,and photocatalysis[J].Journal of Environmental Sciences-China,2011,23(11):1904-1910.
[6]郭丽莉,许超,李书鹏,等.铬污染土壤的生物化学还原稳定化研究[J].环境工程,2014,32(10):152-156.
[7]Tu S.Transformations of synthetic birnessite as affected by p H and manganese concentration[J].Clays and Clay Minerals,1994,42(3):321-330.
[8]董长勋,潘根兴,兰叶青.溶液p H和吸附离子对水相中δ-Mn O2氧化Cr(Ⅲ)的影响研究[J].生态环境,2006,15(1):27-31.
[9]Dai R A,Liu J,Yu C Y,et al.A comparative study of oxidation of Cr(Ⅲ)in aqueous ions,complex ions and insoluble compounds by manganese-bearing mineral(birnessite)[J].Chemosphere,2009,76(4):536-541.
[10]董长勋,戴儒南,熊建军.δ-Mn O2对Cr(Ⅲ)氧化动力学特征[J].环境科学,2010,31(5):1395-1401.
[11]王强,刘双营,黄玉明,等.水钠锰矿对Cr(Ⅲ)离子的吸附解吸及氧化行为[J].土壤学报,2010,47(1):64-70.
[12]赵怀燕,龚爱蓉,殷辉,等.模拟表生环境水钠锰矿亚结构转化及钙锰矿的形成[J].地球科学(中国地质大学学报),2014,39(2):227-239.
[13]Landrot G,Ginder-Vogel M,Livi K,et al.Chromium(Ⅲ)oxidation by three poorly crystalline manganese(IV)oxides.2.solid phase analyses[J].Environmental Science&Technology,2012,46(21):11601-11609.
[14]徐佳丽,张芬,刘凡,等.不同氧化度碱性水钠锰矿氧化As(Ⅲ)和Cr(Ⅲ)的动力学特性[J].岩石矿物学杂志,2013,32(6):975-984.
[15]Landrot G,Ginder-Vogel MSparks D L.Kinetics of Chromium(Ⅲ)oxidation by Manganese(IV)oxides using quick scanning Xray absorption fine structure spectroscopy(Q-XAFS)[J].Environmental Science&Technology,2010,44(1):143-149.
[16]Chen Y,Chen Y,Lin Q,et al.Factors affecting Cr(Ⅲ)oxidation by manganese oxides[J].Pedosphere,1997(2):185-192.
[17]陈英旭,朱祖祥,何增耀.环境中氧化锰对Cr(Ⅲ)氧化机理的研究[J].环境科学学报,1993,13(1):45-50.
[18]谭文峰,刘凡,李学垣,等.几种土壤铁锰结核对Cr(Ⅲ)的氧化特性(Ⅰ):氧化锰矿物类型与吸附态离子的影响[J].环境科学学报,2001,21(5):592-596.