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尺寸可控的锌纳米颗粒在CO电还原过程中的结构和氧化态的原位演变

Operando Evolution of the Structure and Oxidation State of Size-Controlled Zn Nanoparticles during CO Electroreduction.

作者信息

Jeon Hyo Sang, Sinev Ilya, Scholten Fabian, Divins Nuria J, Zegkinoglou Ioannis, Pielsticker Lukas, Cuenya Beatriz Roldan

机构信息

Department of Physics , Ruhr-University Bochum , 44780 Bochum , Germany.

Department of Interface Science , Fritz-Haber-Institute of the Max-Planck Society , 14195 Berlin , Germany.

出版信息

J Am Chem Soc. 2018 Aug 1;140(30):9383-9386. doi: 10.1021/jacs.8b05258. Epub 2018 Jul 18.

DOI:10.1021/jacs.8b05258
PMID:30008209
Abstract

We explored the size-dependent activity and selectivity of Zn nanoparticles (NPs) for the electrochemical CO reduction reaction (CORR). Zn NPs ranging from 3 to 5 nm showed high activity and selectivity (∼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 CORR 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 CORR.

摘要

我们探究了锌纳米颗粒(NPs)在电化学CO还原反应(CORR)中尺寸依赖的活性和选择性。粒径在3至5纳米范围内的锌纳米颗粒对CO生成表现出高活性和选择性(约70%),而粒径大于5纳米的颗粒则表现出类似体相的催化性能。此外,观察到粒径小于3纳米的锌纳米颗粒产氢量急剧增加,这与小尺寸纳米颗粒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CORR过程中还揭示了催化剂中残留阳离子锌物种的存在。预计这些物种在所得的选择性趋势中起作用。我们的研究结果可为开发用于CORR的高活性和CO选择性锌基催化剂提供指导。

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