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Steering surface reconstruction of copper with electrolyte additives for CO₂ electroreduction.

ABSTRACT: Electrocatalytic CO₂ reduction to value-added hydrocarbon products using metallic copper (Cu) catalysts is a potentially sustainable approach to facilitate carbon neutrality. However, Cu metal suffers from unavoidable and uncontrollable surface reconstruction during electrocatalysis, which can have either adverse or beneficial effects on its electrocatalytic performance. In a break from the current catalyst design path, we propose a strategy guiding the reconstruction process in a favorable direction to improve the performance. Typically, the controlled surface reconstruction is facilely realized using an electrolyte additive, ethylenediamine tetramethylenephosphonic acid, to substantially promote CO₂ electroreduction to CH₄ for commercial polycrystalline Cu. As a result, a stable CH₄ Faradaic efficiency of 64% with a partial current density of 192 mA cm^-2, thus enabling an impressive CO₂-to-CH₄ conversion rate of 0.25 µmol cm^-2 s^-1, is achieved in an alkaline flow cell. We believe our study will promote the exploration of electrochemical reconstruction and provide a promising route for the discovery of high-performance electrocatalysts.

SUBMITTER: Han Z

PROVIDER: S-EPMC9174297 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Steering surface reconstruction of copper with electrolyte additives for CO<sub>2</sub> electroreduction.

Han Zishan Z Han Daliang D Chen Zhe Z Gao Jiachen J Jiang Guangyi G Wang Xinyu X Lyu Shuaishuai S Guo Yong Y Geng Chuannan C Yin Lichang L Weng Zhe Z Yang Quan-Hong QH

Nature communications 20220607 1

Electrocatalytic CO<sub>2</sub> reduction to value-added hydrocarbon products using metallic copper (Cu) catalysts is a potentially sustainable approach to facilitate carbon neutrality. However, Cu metal suffers from unavoidable and uncontrollable surface reconstruction during electrocatalysis, which can have either adverse or beneficial effects on its electrocatalytic performance. In a break from the current catalyst design path, we propose a strategy guiding the reconstruction process in a fav ...[more]

PMID: 35672315

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Project description:Understanding how crystallographic orientation influences the electrocatalytic performance of metal catalysts can potentially advance the design of catalysts with improved efficiency. Although single crystal electrodes are typically used for such studies, the one-at-a-time preparation procedure limits the range of secondary crystallographic orientations that can be profiled. This work employs scanning electrochemical cell microscopy (SECCM) together with co-located electron backscatter diffraction (EBSD) as a screening technique to investigate how surface crystallographic orientations on polycrystalline copper (Cu) correlate to activity under CO2 electroreduction conditions. SECCM measures spatially resolved voltammetry on polycrystalline copper covering low overpotentials of CO2 conversion to intermediates, thereby screening the different activity from low-index facets where H2 evolution is dominant to high-index facets where more reaction intermediates are expected. This approach allows the acquisition of 2500 voltammograms on approximately 60 different Cu surface facets identified with EBSD. The results show that the order of activity is (111) < (100) < (110) among the Cu primary orientations. The collection of data over a wide range of secondary orientations leads to the construction of an "electrochemical-crystallographic stereographic triangle" that provides a broad comprehension of the trends among Cu secondary surface facets rarely studied in the literature, [particularly (941) and (741)], and clearly shows that the electroreduction activity scales with the step and kink density of these surfaces. This work also reveals that the electrochemical stripping of the passive layer that is naturally formed on Cu in air is strongly grain-dependent, and the relative ease of stripping on low-index facets follows the order of (100) > (111) > (110). This allows a procedure to be implemented, whereby the oxide is removed (to an electrochemically undetectable level) prior to the kinetic analyses of electroreduction activity. SECCM screening allows for the most active surfaces to be ranked and prompts in-depth follow-up studies.

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Steering surface reconstruction of copper with electrolyte additives for CO₂ electroreduction.

Publications

Steering surface reconstruction of copper with electrolyte additives for CO<sub>2</sub> electroreduction.

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Steering surface reconstruction of copper with electrolyte additives for CO2 electroreduction.

Publications

Steering surface reconstruction of copper with electrolyte additives for CO<sub>2</sub> electroreduction.

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OmicsDI is part of the ELIXIR infrastructure

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Steering surface reconstruction of copper with electrolyte additives for CO₂ electroreduction.