Oxygen Reduction Reaction in 1-Butyl-1-methyl-pyrrolidinium Bis(trifluoromethanesulfonyl)imide: Addition of Water as a Proton Species

Oxygen Reduction Reaction in 1-Butyl-1-methyl-pyrrolidinium Bis(trifluoromethanesulfonyl)imide: Addition of Water as a Proton Species
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DOI:
10.1149/2.008404jes
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发表时间:
2014
影响因子:
3.9
通讯作者:
Xiao‐Zi Yuan;V. Alzate;Zhong Xie;D. Ivey;W. Qu
Xiao‐Zi Yuan;V. Alzate;Zhong Xie;D. Ivey;W. Qu
中科院分区:
工程技术4区
文献类型:
--
作者:
Xiao‐Zi Yuan;V. Alzate;Zhong Xie;D. Ivey;W. Qu

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在这项工作中,研究了室温离子液体(RTIL)1-丁基-1-甲基吡咯烷鎓双(三氟甲磺酰基)酰亚胺(BMP-TFSI)的物理和电化学行为。在 BMP-TFSI 中添加水,探讨添加水对电导率、电化学窗口 (ECW) 和氧还原反应 (ORR) 的影响。结果表明,当水含量高达 1.0 wt% 时,由于水-离子液体混合物中的“剪切弛豫”,向 BMP-TFSI 添加水会略微增加 BMP-TFSI 的电导率。由于“杂质效应”,BMP-TFSI中水添加量的增加导致混合物的ECW降低。旋转环盘电极 (RRDE) 技术已证实,原始 BMP-TFSI 中的 ORR 过程可归因于单电子转移:O 2+ e−↔ O 2−•。随着水的加入,O 2/O 2−• 氧化还原电对的可逆性大大降低。阳极峰受到抑制可能是由于超氧化物容易与水反应。在添加 BMP-TFSI 的水中,随着电流密度的增加,ORR 峰出现在更正的电位处。 ORR 活性的提高归因于添加 BMP-TFSI 的水中 ORR 的质子效应和电子转移数的增加。
In this work, the physical and electrochemical behavior in a room temperature ionic liquid (RTIL), 1-butyl-1-methyl-pyrrolidinium bis (trifluoromethanesulfonyl) imide (BMP-TFSI) has been investigated. Water was added to BMP-TFSI and the effect of added water on conductivity, electrochemical window (ECW) and oxygen reduction reaction (ORR) was explored. The results show that for water amounts up to 1.0 wt%, water addition to BMP-TFSI slightly increases the conductivity of BMP-TFSI due to" shear relaxation" in the water-ionic liquid mixture. As a result of an" impurity effect", an increase in water addition to BMP-TFSI brings about a reduction in the ECW for the mixture. The rotating ring-disk electrode (RRDE) technique has confirmed that the ORR process in as-received BMP-TFSI can be assigned to one-electron transfer: O 2+ e−↔ O 2−•. The reversibility of the O 2/O 2−• redox couple is greatly reduced with the addition of water. The suppressed anodic peak is likely attributable to the fact that the superoxide readily reacts with water. In water added BMP-TFSI, the ORR peak occurs at a more positive potential with an increased current density. The improved ORR activity is attributed to a proton effect and the increase in electron transfer number of the ORR in water added BMP-TFSI.