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物理化学学报  2006, Vol. 22 Issue (04): 403-408    DOI: 10.1016/S1872-1508(06)60012-0
研究论文     
全钒液流电池高浓度下V(IV)/V(V)的电极过程研究
文越华;张华民;钱鹏;赵平;周汉涛;衣宝廉
中国科学院大连化学物理研究所, 燃料电池工程中心, 辽宁 大连 116023; 北京防化研究院军用电源发展与研究中心, 北京 100083
Investigations on the Electrode Process of Concentrated V(IV)/V(V) Species in a Vanadium Redox Flow Battery
WEN Yue-Hua;ZHANG Hua-Min;QIAN Peng;ZHAO Ping;ZHOU Han-Tao;YI Bao-Lian
Full Cell R&D Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, P. R. China; Chemical Defence Institute, Beijing 100083, P. R. China
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摘要： 采用循环伏安、低速线性扫描和阻抗技术, 以石墨为电极, 研究了V(IV)/V(V)在较高浓度下的电极过程. 结果表明, 采用2.0 mol•L-1 的V(IV)溶液时, H2SO4浓度低于2 mol•L-1, V(IV)/V(V)反应极化大, 可逆性差, 表现为电化学和扩散混合控制; H2SO4浓度增至2 mol•L-1以上, V(IV)/V(V)反应的可逆性提高, 转为扩散控制, 且增加H2SO4浓度有利于阻抗的降低; 但H2SO4浓度超过3 mol•L-1, 溶液的粘度和传质阻力大, 阻抗反而增大. 在3 mol•L-1的H2SO4中, 随着V(IV)浓度的增加, 体系的可逆性和动力学改善, 阻抗减小; 但V(IV)浓度超过2.0 mol•L-1, 较高的溶液粘度导致溶液的传质阻力迅速增加, V(IV)/ V(V)的电化学性能衰减, 阻抗增大. 因此, 综合考虑电极反应动力学和电池的能量密度两因素, V(IV)溶液的最佳浓度为1.5～2.0 mol•L-1, H2SO4浓度为3 mol•L-1.
关键词： 全钒液流电池;  V(IV)/V(V);  高浓度;  电极过程    
Abstract: The electrode process of concentrated V(IV)/V(V) species has been studied at a graphite electrode using cyclic voltammetry, linear polarization, and impedance techniques. The results have revealed that in H2SO4 solution below 2 mol•L-1 containing 2.0 mol•L-1 V(IV), the electrode process of V(IV)/V(V) is controlled by the electrochemical polarization and diffusion with poor reversibility. When the concentration of H2SO4 is above 2 mol•L-1, the electrode process of V(IV)/V(V) turns into the diffusion control with improvement of the reversibility. An increase in concentration of H2SO4 solution facilitates a decrease in impedance, whereas too high concentration of H2SO4 solution(>3 mol•L-1) results in a remarkable increase in the viscosity of solution leading to a large mass transportation polarization, and thus the impedance starts to increase a bit. In 3 mol•L-1 H2SO4 solution, the reversibility and kinetics of V(IV)/V(V) are improved gradually as well as the characteristics of impedance with increasing concentration of V(IV) solution. But, when the concentration of V(IV) solution exceeds 2.0 mol•L-1, the viscosity of the solution is so high that the mass transportation polarization increases considerably, resulting in the deterioration of electrochemical performance of V(IV)/V(V) species and an increase in impedance. Therefore, considering from standpoint of increasing the energy density and electrode kinetics comprehensively, the optimal concentration of H2SO4 is 3 mol•L-1 containing 1.5~2.0 mol•L-1 of V(IV).
Key words: Vanadium redox flow battery    V(IV)/V(V)    High concentration    Electrode process
收稿日期: 2005-09-08 出版日期: 2006-04-10
通讯作者: 张华民     E-mail: zhanghm@dicp.ac.cn
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文越华
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引用本文:

文越华;张华民;钱鹏;赵平;周汉涛;衣宝廉. 全钒液流电池高浓度下V(IV)/V(V)的电极过程研究[J]. 物理化学学报, 2006, 22(04): 403-408, 10.1016/S1872-1508(06)60012-0

WEN Yue-Hua;ZHANG Hua-Min;QIAN Peng;ZHAO Ping;ZHOU Han-Tao;YI Bao-Lian. Investigations on the Electrode Process of Concentrated V(IV)/V(V) Species in a Vanadium Redox Flow Battery. Acta Phys. -Chim. Sin., 2006, 22(04): 403-408, 10.1016/S1872-1508(06)60012-0.

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http://www.whxb.pku.edu.cn/CN/10.1016/S1872-1508(06)60012-0    或    http://www.whxb.pku.edu.cn/CN/Y2006/V22/I04/403

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