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Quasi-square-shaped cadmium hydroxide nanocatalysts for electrochemical CO₂ reduction with high efficiency.

ABSTRACT: Powered by a renewable electricity source, electrochemical CO₂ reduction reaction is a promising solution to facilitate the carbon balance. However, it is still a challenge to achieve a desired product with commercial current density and high efficiency. Herein we designed quasi-square-shaped cadmium hydroxide nanocatalysts for CO₂ electroreduction to CO. It was discovered that the catalyst is very active and selective for the reaction. The current density could be as high as 200 mA cm^-2 with a nearly 100% selectivity in a commonly used H-type cell using the ionic liquid-based electrolyte. In addition, the faradaic efficiency of CO could reach 90% at a very low overpotential of 100 mV. Density functional theory studies and control experiments reveal that the outstanding performance of the catalyst was attributed to its unique structure. It not only provides low Cd-O coordination, but also exposes high activity (002) facet, which requires lower energy for the formation of CO. Besides, the high concentration of CO can be achieved from the low concentration CO₂ via an adsorption-electrolysis device.

SUBMITTER: Chen C

PROVIDER: S-EPMC8442700 | biostudies-literature | 2021 Sep

REPOSITORIES: biostudies-literature

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Quasi-square-shaped cadmium hydroxide nanocatalysts for electrochemical CO2 reduction with high efficiency.

Chen Chunjun C Yan Xupeng X Wu Ruizhi R Wu Yahui Y Zhu Qinggong Q Hou Minqiang M Zhang Zhaofu Z Fan Honglei H Ma Jun J Huang Yuying Y Ma Jingyuan J Sun Xiaofu X Lin Longfei L Liu Shoujie S Han Buxing B

Chemical science 20210810 35

Powered by a renewable electricity source, electrochemical CO2 reduction reaction is a promising solution to facilitate the carbon balance. However, it is still a challenge to achieve a desired product with commercial current density and high efficiency. Herein we designed quasi-square-shaped cadmium hydroxide nanocatalysts for CO2 electroreduction to CO. It was discovered that the catalyst is very active and selective for the reaction. The current density could be as high ...[more]

PMID: 34659731

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Project description:The electrochemical CO2 reduction reaction (CO2RR) holds enormous potential as a carbon-neutral route to the sustainable production of fuels and platform chemicals. The durability for long-term operation is currently inadequate for commercialization, however, and the underlying deactivation process remains elusive. A fundamental understanding of the degradation mechanism of electrocatalysts, which can dictate the overall device performance, is needed. In this work, we report the structural dynamics and degradation pathway of Cu oxide nanoparticles (CuOx NPs) during the CO2RR by using in situ small-angle X-ray scattering (SAXS) and X-ray absorption spectroscopy (XAS). The in situ SAXS reveals a reduction in the size of NPs when subjected to a potential at which no reaction products are detected. At potentials where the CO2RR starts to occur, CuOx NPs are agglomerated through a particle migration and coalescence process in the early stage of the reaction, followed by Ostwald ripening (OR) as the dominant degradation mechanism for the remainder of the reaction. As the applied potential becomes more negative, the OR process becomes more dominant, and for the most negative applied potential, OR dominates for the entire reaction time. The morphological changes are linked to a gradual decrease in the formation rate for multicarbon products (C2H4 and ethanol). Other reaction parameters, including reaction intermediates and local high pH, induce changes in the agglomeration process and final morphology of the CuOx NPs electrode, supported by post-mortem ex situ microscopic analysis. The in situ XAS analysis suggests that the CuOx NPs reduced into the metallic state before the structural transformation was observed. The introduction of high surface area carbon supports with ionomer coating mitigates the degree of structural transformation and detachment of the CuOx NPs electrode. These findings show the dynamic nature of Cu nanocatalysts during the CO2RR and can serve as a rational guideline toward a stable catalyst system under electrochemical conditions.

Dataset Information

Quasi-square-shaped cadmium hydroxide nanocatalysts for electrochemical CO₂ reduction with high efficiency.

Publications

Quasi-square-shaped cadmium hydroxide nanocatalysts for electrochemical CO<sub>2</sub> reduction with high efficiency.

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