Operando Evolution of the Structure and Oxidation State of Size-Controlled Zn Nanoparticles during CO2 Electroreduction
Operando Evolution of the Structure and Oxidation State of Size-Controlled Zn Nanoparticles during CO2 Electroreduction
复制标题
DOI：
10.1021/jacs.8b05258
复制
发表时间：
2018-08-01
影响因子：
15
通讯作者：
Roldan Cuenya, Beatriz
中科院分区：
文献类型：
--
作者：
Jeon, Hyo Sang;Sinev, Ilya;Roldan Cuenya, Beatriz
我们探索了 Zn 纳米颗粒 (NP) 在电化学 CO2 还原反应 (CO2RR) 中的尺寸依赖性活性和选择性。 3 至 5 nm 范围内的 Zn NP 对 CO 生产表现出较高的活性和选择性（接近 70%），而 5 nm 以上的 Zn NP 则表现出块状催化性能。此外，对于小于 3 nm 的 Zn NP，观察到氢气产量急剧增加，这与小 NP 上低配位位点含量的增加有关。通过原位 X 射线吸收精细结构光谱测量，在 CO2RR 过程中还揭示了催化剂中残留阳离子 Zn 物质的存在。预计这些物种将在获得的选择性趋势中发挥作用。我们的研究结果可以为开发用于 CO2RR 的高活性和 CO 选择性锌基催化剂提供指导。
We explored the size-dependent activity and selectivity of Zn nanoparticles (NPs) for the electrochemical CO2 reduction reaction (CO2RR). Zn NPs ranging from 3 to 5 nm showed high activity and selectivity (similar to 70%) for CO production, whereas those above 5 nm exhibited bulk-like catalytic properties. In addition, a drastic increase in hydrogen production was observed for the Zn NPs below 3 nm, which is associated with the enhanced content of low-coordinated sites on small NPs. The presence of residual cationic Zn species in the catalysts was also revealed during CO2RR via operando X-ray absorption fine-structure spectroscopy measurements. Such species are expected to play a role in the selectivity trends obtained. Our findings can serve as guidance for the development of highly active and CO-selective Zn-based catalysts for CO2RR.