<br>Zn-Al LDH 作为 CO2 还原反应电催化剂的见解：原位 ATR-IR 研究,Journal of CO2 Utilization

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Zn-Al LDH 作为 CO2 还原反应电催化剂的见解：原位 ATR-IR 研究
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2024-05-19 , DOI: 10.1016/j.jcou.2024.102804
Margherita Cavallo , Melodj Dosa , Ryosuke Nakazato , Natale Gabriele Porcaro , Matteo Signorile , Matthias Quintelier , Joke Hadermann , Silvia Bordiga , Nataly Carolina Rosero-Navarro , Kiyoharu Tadanaga , Valentina Crocellà , Francesca Bonino

电化学还原二氧化碳 (CO2RR) 预计将在正在探索的限制全球变暖的各种策略中发挥关键作用。在这种情况下，层状双氢氧化物（LDH）正在成为一类有前景的电催化剂，以取代最常用的贵金属。本工作合成了三种不同Zn/Al比的Zn-Al LDH，并通过XRD、STEM-EDX和HR-TEM对其进行了表征。通过定制的三室电池评估了它们对 CO2RR 对 CO 的适用性，结果表明通过降低 Zn/Al 比率可以提高 CO 选择性。首先通过体积吸附测量来表征 CO 与样品的相互作用，结果表明，通过降低 Zn/Al 比，捕获能力会增加。然后通过 ATR-IR 光谱法深入研究了样品与 CO 饱和液体流相互作用的演变。样品在碳酸盐类物质的振动区域（1800-1200cm）表现出不同的演化。为了更好地区分不同的碳酸酯，还使用了环己烷。通过研究 ATR-IR 实验中观察到的不同波段的光谱行为并将这些结果与现有文献进行比较，对碳酸盐的主要红外波段进行了明确的分配。有趣的是，Zn-Al 1:2 LDH是CO2RR最有效的电催化剂，也是唯一表现出较高单齿与总二齿碳酸盐比率的样品，这表明存在较高含量的具有较强碱性的低配位氧阴离子可以影响最终的催化活性。

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Insight on Zn-Al LDH as electrocatalyst for CO2 reduction reaction: An in-situ ATR-IR study

Electrochemical reduction of CO (CO2RR) is expected to play a key role among the various strategies being explored to limit global warming. In this scenario, Layered Double Hydroxides (LDHs) are emerging as a promising class of electrocatalysts to replace the most used noble metals. In this work three Zn-Al LDH with different Zn/Al ratio were synthesized and characterized by means of XRD, STEM-EDX and HR-TEM. Their suitability for CO2RR to CO was assessed by means of a custom-made three-compartment cell, showing an increase in CO selectivity by decreasing the Zn/Al ratio. The CO interaction with the samples was firstly characterized by means of volumetric adsorption measurements, exhibiting an increase in capture capacity by decreasing the Zn/Al ratio. The evolution of the samples in interaction with a CO-saturated liquid flow was then deeply investigated by means of ATR-IR spectroscopy. The samples displayed a different evolution in the vibrational region of the carbonate-like species (1800–1200 cm). To better discriminate the different carbonate cyclohexane was also employed. A definitive assignment of the main IR bands of the carbonate was carried out by studying the spectral behavior of the different bands observed in the ATR-IR experiments and by comparing these results with the existing literature. Interestingly, Zn-Al 1:2 LDH, the most efficient electrocatalyst for CO2RR, is also the sole sample exhibiting a higher monodentate to total bidentate carbonates ratio, suggesting that the existence of a higher content of low coordination oxygen anions with stronger basic character can influence the final catalytic activity.

更新日期：2024-05-19

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