Volume 1, 2023

Revealing the activity and selectivity of ppm level copper in gas diffusion electrodes towards CO and CO2 electroreduction

Abstract

Cu is a unique metal that catalyzes carbon monoxide/carbon dioxide (CO/CO2) to form high-order hydrocarbons and oxygenates through the CO/CO2 reduction reaction (CO/CO2RR) at decent selectivity and productivity. While this has been shown, the limits of the system are still unknown, i.e., the minimum amount of Cu needed for the CO/CO2RR, and the maximum activity that trace amounts of Cu can achieve. Here, we have investigated the activity and selectivity of trace Cu with atomic dispersion over a range of loadings below 2 μg cm−2 and have quantified the mass activity/turnover frequency (TOF) of trace Cu catalysts. A Cu loading of at least 0.042 μg cm−2 initiates the CORR activity with 30% faradaic efficiency (FE) at a partial current density of 102 mA cm−2 forming predominantly CH4. The selectivity moves to C2-based products (CH3COO, C2H4, and CH3CH2OH) with 70% FE as the Cu loading increases to 0.333 μg cm−2, and increasing the Cu loading to 0.812 μg cm−2 results in a 78% FE to C2 with CH3COO accounting for 42% of this. The highest mass activity for CH4 reaches 2435 A mg−1 of Cu, corresponding to a TOF of 267 s−1, while C2 activity reaches 584 A mg−1 of Cu, leading to a TOF of 145 s−1. Both TOFs are several orders of magnitude higher than the reported values. Different from the CORR, the CO2RR demands a higher Cu loading and primarily generates C1 (e.g., CO and CH4). Metal impurities can be extended to others that are active towards the CO2RR, such as Zn for CO2-to-CO conversion. Thus, we suggest that the effect of trace metal impurities must be quantified when developing carbon-based metal-free and coordinated single-atom catalysts for the CO/CO2RR in order to avoid overestimating their activity.

Graphical abstract: Revealing the activity and selectivity of ppm level copper in gas diffusion electrodes towards CO and CO2 electroreduction

Supplementary files

Article information

Article type
Communication
Submitted
15 okt 2022
Accepted
28 noy 2022
First published
28 noy 2022
This article is Open Access
Creative Commons BY-NC license

EES. Catal., 2023,1, 117-124

Revealing the activity and selectivity of ppm level copper in gas diffusion electrodes towards CO and CO2 electroreduction

X. Lyu, J. Li, T. Zhang, Z. Li, I. Hwang, C. Sun, C. J. Jafta, J. Yang, T. J. Toops, D. A. Cullen, A. Serov and J. Wu, EES. Catal., 2023, 1, 117 DOI: 10.1039/D2EY00071G

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