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Citation: WANG Chong-Tai, HUA Ying-Jie, SUN Zhen-Fan, WEI Ji-Chong, LI Tian-Lue, TONG Ye-Xiang, LIU Xiao-Yang. Electrochemical Properties of the Dawson-Type Heteropolytungstate Anion P2W18O626- and Its O2 Reduction Electrocatalysis[J]. Acta Physico-Chimica Sinica, 2011, 27(02): 473-478. doi: 10.3866/PKU.WHXB20110208
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Dawson型磷钨杂多阴离子P2W18O626-的电化学性质和对O2还原的电催化作用
用循环伏安、交流伏安和交流阻抗法对Dawson型磷钨杂多阴离子P2W18O626-的电化学性质进行了详细研究, 循环伏安结果显示, P2W18O626-在pH 2.52的0.1 mol·L-1 Na2SO4+NaHSO4溶液中有两对可逆的单电子还原-氧化波和两对可逆的双电子还原-氧化波. 单电子波的峰电位和电流与溶液的pH无关, 双电子波的峰电位则随溶液pH的增加而负移, 峰电流降低, 表明双电子电极过程有H+参与, 其数目为2. 交流阻抗谱表明P2W18O626-的电极过程完全受扩散控制, 实验测定其扩散系数(DO)为2.5×10-6 cm2·s-1. 循环伏安结果表明P2W18O626-的第III对波对O2还原为H2O2具有显著的电催化作用, 催化效率约达300%. 将P2W18O626-应用于PW11O39Fe(III)(H2O)4-构成的类电-芬顿过程, 使该过程对硝基苯的降解效率显著提高.
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关键词:
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Dawson型磷钨杂多阴离子
- / 电催化
- / 氧还原
- / 过氧化氢
- / 硝基苯降解
English
Electrochemical Properties of the Dawson-Type Heteropolytungstate Anion P2W18O626- and Its O2 Reduction Electrocatalysis
The electrochemical properties of the Dawson-type heteropolyanion P2W18O626- were studied in detail by cyclic voltammetry, alternating current (AC) voltammetry, and AC impedance. Cyclic voltammetry results revealed that P2W18O626- possessed two pairs of reversible one-electron redox waves and two pairs of reversible two-electron redox waves in a solution containing 0.1 mol·L-1 Na2SO4 and NaHSO4 (pH 2.52). The peak potential and the peak current of the single-electron wave were independent of the solution pH while the peak potential of the two-electron wave shifted negatively, and the peak current decreased with an increase in solution pH. This indicated that the two-electron electrode process involved H+ and the involved H+ number was 2. AC impedance spectroscopy showed that the P2W18O626- electrode process was fully controlled by diffusion and the diffusion coefficient (DO) was 2.5×10-6 cm2·s-1. The cyclic voltammograms indicated that significant P2W18O626- electrocatalysis towards O2 reduction to H2O2 occurred as evidenced by the third wave pair and a catalytic efficiency of 300% were obtained. Application of P2W18O626- in the degradation of nitrobenzene in the electro-Fenton-like system containing PW11O39Fe(III)(H2O)4- showed a remarkable improvement in terms of degradation efficiency.
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[1]
(1) Toth, J. E.; Anson, F. C. J. Am. Chem. Soc. 1989, 111, 2444.
(1) Toth, J. E.; Anson, F. C. J. Am. Chem. Soc. 1989, 111, 2444.
-
[2]
(2) Sadakane, M.; Steckhan, E. Chem. Rev. 1998, 98, 219.(2) Sadakane, M.; Steckhan, E. Chem. Rev. 1998, 98, 219.
-
[3]
(3) Coronado, E.; ′mez-Garc?′a C. J. Chem. Rev. 1998, 98, 273.(3) Coronado, E.; ′mez-Garc?′a C. J. Chem. Rev. 1998, 98, 273.
-
[4]
(4) Inoue, M.; Suzuki, T.; Fujita, Y.; Oda, M.; Matsumoto, N.; amase, T. J. Inorgan. Biochem. 2006, 100, 1225.(4) Inoue, M.; Suzuki, T.; Fujita, Y.; Oda, M.; Matsumoto, N.; amase, T. J. Inorgan. Biochem. 2006, 100, 1225.
-
[5]
(5) Xi, X. D.; Dong, S. J. J. Mole. Catal. A: Chem. 1996, 114, 257.(5) Xi, X. D.; Dong, S. J. J. Mole. Catal. A: Chem. 1996, 114, 257.
-
[6]
(6) Fay, N.; Dempsey, E.; McCormac, T. J. Electroanal. Chem. 2005, 574, 359.(6) Fay, N.; Dempsey, E.; McCormac, T. J. Electroanal. Chem. 2005, 574, 359.
-
[7]
(7) Lei, P. X.; Chen, C. C.; Yang, J.; Ma,W. H.; Zhao, J. C.; Zang, L. Environ. Sci. Technol. 2005, 39, 8466.(7) Lei, P. X.; Chen, C. C.; Yang, J.; Ma,W. H.; Zhao, J. C.; Zang, L. Environ. Sci. Technol. 2005, 39, 8466.
-
[8]
(8) Mylonas, A.; Hiskia, A.; Papaconstantinou, E. J. Mole. Catal. A: Chem. 1996, 114, 19l.(8) Mylonas, A.; Hiskia, A.; Papaconstantinou, E. J. Mole. Catal. A: Chem. 1996, 114, 19l.
-
[9]
(9) Wang, C. T.; Hua, Y. J.; Li, G. R.; Tong, Y. X.; Li,Y. G. Acta him. Sin. 2008, 66, 835.(9) Wang, C. T.; Hua, Y. J.; Li, G. R.; Tong, Y. X.; Li,Y. G. Acta him. Sin. 2008, 66, 835.
-
[10]
[王崇太, 华英杰, 李高仁, 童叶翔, 玉光. 化学学报, 2008, 66, 835.][王崇太, 华英杰, 李高仁, 童叶翔, 玉光. 化学学报, 2008, 66, 835.]
-
[11]
(10) Wang, C. T.; Hua, Y. J.; Li, G. R.; Tong, Y. X.; Li, Y. G. lectrochim. Acta, 2008, 53, 5100.(10) Wang, C. T.; Hua, Y. J.; Li, G. R.; Tong, Y. X.; Li, Y. G. lectrochim. Acta, 2008, 53, 5100.
-
[12]
(11) Hua, Y. J.;Wang, C. T.; Tong, Y. X.; Zhang, D. S.; Zhang, Q.; u, T. A.; Hu, P. Acta Chim. Sin. 2009, 67, 2650.(11) Hua, Y. J.;Wang, C. T.; Tong, Y. X.; Zhang, D. S.; Zhang, Q.; u, T. A.; Hu, P. Acta Chim. Sin. 2009, 67, 2650.
-
[13]
[华英杰, 崇太, 童叶翔, 张大帅, 张奇, 谷铁安, 胡佩, 化学学报, 2009, 67, 2650.][华英杰, 崇太, 童叶翔, 张大帅, 张奇, 谷铁安, 胡佩, 化学学报, 2009, 67, 2650.]
-
[14]
(12) Prenzler, P. D.; Boskovic, C.; Bond, A. M.; Anthony, G.W. Anal. Chem. 1999, 71, 3650.(12) Prenzler, P. D.; Boskovic, C.; Bond, A. M.; Anthony, G.W. Anal. Chem. 1999, 71, 3650.
-
[15]
(13) Shchukin, D. G.; Sviridov, D. V. Electrochem. Commun. 2002, 4, 02.(13) Shchukin, D. G.; Sviridov, D. V. Electrochem. Commun. 2002, 4, 02.
-
[16]
(14) Haraguchi, N.; Okaue, Y.; Isobe, T.; Matsuda, Y. Inorg. Chem. 1994, 33, 1015.(14) Haraguchi, N.; Okaue, Y.; Isobe, T.; Matsuda, Y. Inorg. Chem. 1994, 33, 1015.
-
[17]
(15) Bard, A. J.; Faulkner, L. R. Electrochemical Methods- undamentals and Applications, 1st ed.; Chemical Industry ress: Beijing, 1986; p253; translated by Gu, L.Y.; Lü, M. X.; ong, S. Z.; Xu, C. C.(15) Bard, A. J.; Faulkner, L. R. Electrochemical Methods- undamentals and Applications, 1st ed.; Chemical Industry ress: Beijing, 1986; p253; translated by Gu, L.Y.; Lü, M. X.; ong, S. Z.; Xu, C. C.
-
[18]
[Bard, A. J.; Faulkner, L. R. 电化学方 -原理及应用. 谷林锳, 吕鸣祥, 宋诗哲,许淳淳, 译; 北京: 学工业出版社, 1986: 253.][Bard, A. J.; Faulkner, L. R. 电化学方 -原理及应用. 谷林锳, 吕鸣祥, 宋诗哲,许淳淳, 译; 北京: 学工业出版社, 1986: 253.]
-
[19]
(16) Wang, C. T.; Hua, Y. J.; Tong, Y. X. Electrochim. Acta 2010, 55, 755.
(16) Wang, C. T.; Hua, Y. J.; Tong, Y. X. Electrochim. Acta 2010, 55, 755.
-
[1]
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