“Buckets effect” in the kinetics of electrocatalytic reactions

IF 14 1区 化学 Q1 CHEMISTRY, APPLIED 能源化学 Pub Date : 2023-10-20 DOI:10.1016/j.jechem.2023.09.051
Haowen Cui, Yan-Xia Chen
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引用次数: 1

Abstract

In this study, we systematically investigated the effect of proton concentration on the kinetics of the oxygen reduction reaction (ORR) on Pt(111) in acidic solutions. Experimental results demonstrate a rectangular hyperbolic relationship, i.e., the ORR current excluding the effect of other variables increases with proton concentration and then tends to a constant value. We consider that this is caused by the limitation of ORR kinetics by the trace oxygen concentration in the solution, which determines the upper limit of ORR kinetics. A model of effective concentration is further proposed for rectangular hyperbolic relationships: when the reactant concentration is high enough to reach a critical saturation concentration, the effective reactant concentration will become a constant value. This could be due to the limited concentration of a certain reactant for reactions involving more than one reactant or the limited number of active sites available on the catalyst. Our study provides new insights into the kinetics of electrocatalytic reactions, and it is important for the proper evaluation of catalyst activity and the study of structure-performance relationships.

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电催化反应动力学中的“桶效应”
在本研究中,我们系统地研究了质子浓度对酸性溶液中Pt(111)氧还原反应动力学的影响。实验结果显示了一个矩形双曲线关系,即排除其他变量影响的ORR电流随着质子浓度的增加而增加,然后趋于恒定值。我们认为这是由于溶液中微量氧浓度限制了ORR动力学,而微量氧浓度决定了ORR动力学的上限。进一步提出了矩形双曲关系的有效浓度模型:当反应物浓度足够高,达到临界饱和浓度时,有效反应物浓度将成为一个常数。这可能是由于涉及一种以上反应物的反应中某种反应物的浓度有限,或者催化剂上可用的活性位点数量有限。我们的研究为电催化反应动力学提供了新的见解,对正确评价催化剂活性和研究结构-性能关系具有重要意义。
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CiteScore
23.60
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0.00%
发文量
2875
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