Citation: FEILURE Tuerxun, ZULIPIYA Shadike, NULI Yan-Na, YANG Jun, WANG Jiu-Lin. Pyrazolyl Magnesium Halide/Tetrahydrofuran Solutions for Rechargeable Magnesium Battery Electrolytes[J]. Acta Physico-Chimica Sinica, 2014, 30(9): 1634-1640. doi: 10.3866/PKU.WHXB201407101
吡唑基镁卤化物/四氢呋喃可充镁电池电解液
将不同配比的吡唑与格氏试剂反应制得的吡唑基镁卤化物/四氢呋喃(THF)溶液用作可充镁电池电解液,采用循环伏安和恒电流充放电测试研究了该电解液的镁沉积-溶出性能和氧化分解电位;并通过X射线衍射(XRD)和扫描电镜(SEM)对沉积物的组分和形貌进行了分析. 结果表明,吡唑上的取代基、吡唑与格氏试剂的反应配比对电解液的电化学性能都有影响. 1 mol·L-1 1-甲基吡唑-PhMgCl(1:1摩尔比)/THF反应配制的电解液在不锈钢(SS)集流体的阳极氧化分解电位达到2.4 V(vs Mg/Mg2+),并具有镁沉积-溶出电位低、循环稳定性高、配制方便的特点,有希望应用于实际的可充镁电池体系中.
English
Pyrazolyl Magnesium Halide/Tetrahydrofuran Solutions for Rechargeable Magnesium Battery Electrolytes
Pyrazolyl magnesium halide/tetrahydrofuran (THF) solutions were obtained by the simple reaction of pyrazole compounds with Grignard reagents in THF. Their electrochemical performances as rechargeable magnesium battery electrolytes are reported. The pyrazolyl magnesium halide/THF solutions were characterized in term of anodic stability and reversibility of magnesium deposition-dissolution using cyclic voltammetry and galvanostatic charge-discharge techniques. The composition and morphology of the deposit were analyzed using X-ray diffraction (XRD) and scanning electron microscopy (SEM). It is concluded that the substituents on the pyrazole compound and the molar ratio of the pyrazole to the Grignard both affect the electrochemical performance. An electrolyte consisting of 1 mol·L-1 1-methylpyrazole-PhMgCl (1:1 molar ratio)/THF has an anodic oxidation decomposition potential of 2.4 V (vs Mg/Mg2+) on stainless steel (SS), a low potential for magnesium deposition-dissolution, and a high cycling reversibility, and can be prepared easily, making it a promising candidate for rechargeable battery electrolytes.
-
Key words:
-
Rechargeable magnesium battery
- / Electrolyte
- / Electrochemical performance
-
-
[1]
(1) Zhao, Q. S.; NuLi, Y. N.; Guo, Y. S.; Yang, J.;Wang, J. L. Process. Chem. 2011, 23 (8), 1599. [赵青松, 努丽燕娜, 郭永胜, 杨军, 王久林. 化学进展, 2011, 23 (8), 1599.]
(1) Zhao, Q. S.; NuLi, Y. N.; Guo, Y. S.; Yang, J.;Wang, J. L. Process. Chem. 2011, 23 (8), 1599. [赵青松, 努丽燕娜, 郭永胜, 杨军, 王久林. 化学进展, 2011, 23 (8), 1599.]
-
[2]
(2) Zheng, Y. P.; Nuli, Y. N.; Yang, J.; Chen, Q.;Wang, J. L. Chem. Ind. Eng. Prog. 2011, 30 (5), 1025. [郑育培, 努丽燕娜,杨军, 陈强, 王久林. 化工进展, 2011, 30 (5), 1025.](2) Zheng, Y. P.; Nuli, Y. N.; Yang, J.; Chen, Q.;Wang, J. L. Chem. Ind. Eng. Prog. 2011, 30 (5), 1025. [郑育培, 努丽燕娜,杨军, 陈强, 王久林. 化工进展, 2011, 30 (5), 1025.]
-
[3]
(3) Genders, J. D.; Pletcher, D. J. Electroanal. Chem. Interfa. Electrochem. 1986, 199, 93. doi: 10.1016/0022-0728(86)87044-9(3) Genders, J. D.; Pletcher, D. J. Electroanal. Chem. Interfa. Electrochem. 1986, 199, 93. doi: 10.1016/0022-0728(86)87044-9
-
[4]
(4) Liebenow, C. J. J. Appl. Electrochem. 1997, 27, 221. doi: 10.1023/A:1018464210084(4) Liebenow, C. J. J. Appl. Electrochem. 1997, 27, 221. doi: 10.1023/A:1018464210084
-
[5]
(5) Lu, Z.; Schechter, A.; Moshkovich, M.; Aurbach, D. J. Electroanal. Chem. 1999, 466, 203. doi: 10.1016/S0022-0728(99)00146-1(5) Lu, Z.; Schechter, A.; Moshkovich, M.; Aurbach, D. J. Electroanal. Chem. 1999, 466, 203. doi: 10.1016/S0022-0728(99)00146-1
-
[6]
(6) Aurbach, D.; Moshkovich, M.; Schechter, A.; Turgeman, R. Electrochem. Solid-State Lett. 2000, 3, 31.(6) Aurbach, D.; Moshkovich, M.; Schechter, A.; Turgeman, R. Electrochem. Solid-State Lett. 2000, 3, 31.
-
[7]
(7) Muldoon, J.; Bucur, C. B.; Oliver, A. G.; Sugimoto, T.; Matsui, M.; Kim, H. S.; Allred, G. D.; Zajicek, J.; Kotani, Y. Energy Environ. Sci. 2012, 5, 5941. doi: 10.1039/c2ee03029b(7) Muldoon, J.; Bucur, C. B.; Oliver, A. G.; Sugimoto, T.; Matsui, M.; Kim, H. S.; Allred, G. D.; Zajicek, J.; Kotani, Y. Energy Environ. Sci. 2012, 5, 5941. doi: 10.1039/c2ee03029b
-
[8]
(8) Gre ry, T. D.; Hoffman, R. J.;Winterton, R. C. J. Electrochem. Soc. 1990, 137, 775. doi: 10.1149/1.2086553(8) Gre ry, T. D.; Hoffman, R. J.;Winterton, R. C. J. Electrochem. Soc. 1990, 137, 775. doi: 10.1149/1.2086553
-
[9]
(9) Liebenow, C.; Yang, Z.; Lobitz, P. Electrochem. Commun. 2000, 2, 641. doi: 10.1016/S1388-2481(00)00094-1(9) Liebenow, C.; Yang, Z.; Lobitz, P. Electrochem. Commun. 2000, 2, 641. doi: 10.1016/S1388-2481(00)00094-1
-
[10]
(10) Mizrahi, O.; Amir, N.; Pollak, E.; Chusid, O.; Marks, V.; ttlieb, H.; Larush, L.; Zinigrad, E.; Aurbach, D. J. Electrochem. Soc. 2008, 155, A103.(10) Mizrahi, O.; Amir, N.; Pollak, E.; Chusid, O.; Marks, V.; ttlieb, H.; Larush, L.; Zinigrad, E.; Aurbach, D. J. Electrochem. Soc. 2008, 155, A103.
-
[11]
(11) Aurbach, D.; Lu, Z.; Schechter, A.; fer, Y.; Gizbar, H.; Turgeman, R.; Cohen, Y.; Moshkovich, M.; Levi, E. Nature 2000, 407, 724. doi: 10.1038/35037553(11) Aurbach, D.; Lu, Z.; Schechter, A.; fer, Y.; Gizbar, H.; Turgeman, R.; Cohen, Y.; Moshkovich, M.; Levi, E. Nature 2000, 407, 724. doi: 10.1038/35037553
-
[12]
(12) Aurbach, D.; Schechter, A.; Moshkovich, M.; Cohen, Y. J. Electrochem. Soc. 2001, 148, A1004.(12) Aurbach, D.; Schechter, A.; Moshkovich, M.; Cohen, Y. J. Electrochem. Soc. 2001, 148, A1004.
-
[13]
(13) Aurbach, D.; Gizbar, H.; Schechter, A.; Chusid, O.; ttlieb, H. E.; fer, Y.; ldberg, I. J. Electrochem. Soc. 2002, 149, A115.(13) Aurbach, D.; Gizbar, H.; Schechter, A.; Chusid, O.; ttlieb, H. E.; fer, Y.; ldberg, I. J. Electrochem. Soc. 2002, 149, A115.
-
[14]
(14) Gizbar, H.; Vestfrid, Y.; Chusid, O.; fer, Y.; ttlieb, H. E.; Marks, V.; Aurbach, D. Organometallics 2004, 23, 3826. doi: 10.1021/om049949a(14) Gizbar, H.; Vestfrid, Y.; Chusid, O.; fer, Y.; ttlieb, H. E.; Marks, V.; Aurbach, D. Organometallics 2004, 23, 3826. doi: 10.1021/om049949a
-
[15]
(15) Vestfried, Y.; Chusid, O.; fer, Y.; Aped, P.; Aurbach, D. Organometallics 2007, 26, 3130. doi: 10.1021/om061076s(15) Vestfried, Y.; Chusid, O.; fer, Y.; Aped, P.; Aurbach, D. Organometallics 2007, 26, 3130. doi: 10.1021/om061076s
-
[16]
(16) Pour, N.; fer, Y.; Major, D. T.; Aurbach, D. J. Am. Chem. Soc. 2011, 133, 6270. doi: 10.1021/ja1098512(16) Pour, N.; fer, Y.; Major, D. T.; Aurbach, D. J. Am. Chem. Soc. 2011, 133, 6270. doi: 10.1021/ja1098512
-
[17]
(17) Muldoon, J.; Bucur, C. B.; Oliver, A. G.; Sugimoto, T.; Matsui, M.; Kim, H. S.; Allred, G. D.; Zajicekb, J.; Kotanie, Y. Energy Environ Sci. 2012, 5, 5941. doi: 10.1039/c2ee03029b(17) Muldoon, J.; Bucur, C. B.; Oliver, A. G.; Sugimoto, T.; Matsui, M.; Kim, H. S.; Allred, G. D.; Zajicekb, J.; Kotanie, Y. Energy Environ Sci. 2012, 5, 5941. doi: 10.1039/c2ee03029b
-
[18]
(18) Guo, Y. S.; Zhang, F.; Yang, J.;Wang, F. F.; NuLi, Y. N.; Hirano, S. I. Energy Environ. Sci. 2012, 5, 9100. doi: 10.1039/c2ee22509c(18) Guo, Y. S.; Zhang, F.; Yang, J.;Wang, F. F.; NuLi, Y. N.; Hirano, S. I. Energy Environ. Sci. 2012, 5, 9100. doi: 10.1039/c2ee22509c
-
[19]
(19) Wang, F. F.; Guo, Y. S.; Yang, J.; NuLi, Y. N.; Hirano, S. I. Chem. Commun. 2012, 48, 10763. doi: 10.1039/c2cc35857c(19) Wang, F. F.; Guo, Y. S.; Yang, J.; NuLi, Y. N.; Hirano, S. I. Chem. Commun. 2012, 48, 10763. doi: 10.1039/c2cc35857c
-
[20]
(20) Bian, P.W.; Nuli, Y. N.; Zainapuguli; Yang, J.;Wang, J. L. Acta Phys. -Chim. Sin. 2014, 30 (2), 311. [卞沛文, 努丽燕娜, 再娜甫古丽, 杨军, 王久林. 物理化学学报, 2014, 30 (2), 311.] doi: 10.3866/PKU.WHXB201312201(20) Bian, P.W.; Nuli, Y. N.; Zainapuguli; Yang, J.;Wang, J. L. Acta Phys. -Chim. Sin. 2014, 30 (2), 311. [卞沛文, 努丽燕娜, 再娜甫古丽, 杨军, 王久林. 物理化学学报, 2014, 30 (2), 311.] doi: 10.3866/PKU.WHXB201312201
-
[21]
(21) Zhao, Q. S.; NuLi, Y. N.; Guo, Y. S.; Yang, J.;Wang, J. L. Electrochim. Acta 2011, 56, 6530. doi: 10.1016/j.electacta.2011.04.114(21) Zhao, Q. S.; NuLi, Y. N.; Guo, Y. S.; Yang, J.;Wang, J. L. Electrochim. Acta 2011, 56, 6530. doi: 10.1016/j.electacta.2011.04.114
-
[22]
(22) Feng, Z. Z.; NuLi, Y. N.;Wang, J. L.; Yang, J. J. Electrochem. Soc. 2006, 153, C689.
(22) Feng, Z. Z.; NuLi, Y. N.;Wang, J. L.; Yang, J. J. Electrochem. Soc. 2006, 153, C689.
-
[1]
-
扫一扫看文章
计量
- PDF下载量: 516
- 文章访问数: 863
- HTML全文浏览量: 53

下载: