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一种用于在电催化CO还原过程中抑制竞争性析氢的具有多个高指数晶面的铜催化剂的简便合成方法。

A facile synthesis of Cu catalysts with multiple high-index facets for the suppression of competing H evolution during electrocatalytic CO reduction.

作者信息

Philip Monday, Woldu Abebe Reda, Akbar Muhammad Bilal, Louis Hitler, Cong Huang

机构信息

CAS Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190, China.

出版信息

Nanoscale. 2021 Feb 7;13(5):3042-3048. doi: 10.1039/d0nr07286a. Epub 2021 Jan 29.

Abstract

The electrochemical CO reduction reaction (CORR) over the high-index facets of Cu nanoparticles (NPs) is favourable towards the formation of multi-carbon products, such as hydrocarbons and oxygenates. However, the facile synthesis of Cu NPs with multiple high-index facets remains a great challenge in the research community. Herein, we have prepared numerous Cu catalysts with flat surfaces by electropolishing polycrystalline Cu foils before and after annealing at different temperatures ranging from 200 °C to 1000 °C under an argon atmosphere. The individual electrode crystal orientations were investigated via X-ray diffraction (XRD) and electron backscattering diffraction (EBSD) techniques. As confirmed by the EBSD technique, the formation of high-index facets increases with an increase in the annealing temperature and reaches a high quantity of high-index facets enclosed mainly by (211) and (431) facets with about 94% of those on the electrode annealed at 1000 °C. As a possible application, we have used the different electrodes for CORR at -1.0 V vs. RHE with special emphasis on the formation of H gas and C1 products. Thus, the electrodes prepared at higher temperatures enable the suppression of competing H evolution due to the increased amount of high-index facets. Moreover, the formation rates of C1 products were inhibited as well at the electrodes with increased number of high-index facets. The drops in the formation rates of both H and C1 products indicate that they are consumed in the chemical reaction to commence the formation of multi-carbon products. However, further study is still required with superior attention on CORR towards the C product formation at a range of applied potentials.

摘要

铜纳米颗粒(NPs)高指数晶面上的电化学CO还原反应(CORR)有利于形成多碳产物,如碳氢化合物和含氧化合物。然而,在研究领域中,轻松合成具有多个高指数晶面的铜纳米颗粒仍然是一个巨大的挑战。在此,我们通过在氩气气氛下于200℃至1000℃的不同温度下对多晶铜箔进行退火前后的电解抛光,制备了许多表面平整的铜催化剂。通过X射线衍射(XRD)和电子背散射衍射(EBSD)技术研究了各个电极的晶体取向。正如EBSD技术所证实的,高指数晶面的形成随着退火温度的升高而增加,并且在1000℃退火的电极上,以(211)和(431)晶面为主的高指数晶面数量达到约94%的高水平。作为一种可能的应用,我们使用不同的电极在相对于可逆氢电极(RHE)为 -1.0 V的条件下进行CORR,特别关注H2气体和C1产物的形成。因此,在较高温度下制备的电极由于高指数晶面数量的增加而能够抑制竞争性析氢。此外,在高指数晶面数量增加的电极上,C1产物的形成速率也受到抑制。H2和C1产物形成速率的下降表明它们在化学反应中被消耗以开始形成多碳产物。然而,对于在一系列施加电位下CORR生成C产物仍需要进一步研究并给予更多关注。

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