article · ACS Applied Materials & Interfaces
Electrochemical reduction of carbon dioxide into valuable chemicals offers an attractive route to lower carbon emissions. In metal nanocatalysts, shape and exposed crystal facets play critical roles in catalytic performance, yet the optimal facets for zinc oxide catalysts have remained debated. An evaluation of different zinc oxide morphologies, including nanowires, nanosheets, and nanoflowers, demonstrated clear facet-dependent reactivity for converting carbon dioxide into carbon monoxide. Zinc oxide nanosheets exposing the specific (110) facet achieved a carbon monoxide Faradaic efficiency of up to 84 per cent alongside a current density of minus ten milliamperes per square centimetre at minus 1.2 volts. This structure substantially outperformed nanowires displaying the (101) facet and nanoflowers displaying the (103) facet. The porous architecture of the nanosheets enhanced active site exposure, while the (110) facet promoted carbon dioxide adsorption and activation.
Converting carbon dioxide into useful chemicals like carbon monoxide is a vital strategy for addressing industrial emissions. Understanding how specific crystal faces influence reaction efficiency helps scientists design more effective materials. By identifying the superior performance of zinc oxide nanosheets with exposed (110) facets, this work clarifies how tailoring catalyst surfaces can make carbon capture and conversion processes more efficient.
This work remains at an early laboratory stage, focused on catalyst synthesis and electrochemical evaluation. The findings could inform developers of carbon utilisation systems and electrolysers who require selective, cost-effective catalysts to transform industrial carbon dioxide emissions into carbon monoxide feedstock. However, practical commercial deployment will depend on establishing scalable fabrication methods for porous nanosheets and testing their durability under continuous industrial operating conditions.
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Electrochemical reduction of CO<sub>2</sub> to highly valuable products is a promising way to reduce CO<sub>2</sub> emissions. The shape and facets of metal nanocatalysts are the key parameters in determining the catalytic performance. However, the exposed crystal facets of ZnO with different morphologies and which facets achieve a high performance for CO<sub>2</sub> reduction are still controversial. Here, we systematically investigate the effect of the facet-dependent reactivity of reduction of CO<sub>2</sub> to CO on ZnO (nanowire, nanosheet, and flower-like). The ZnO nanosheet with exposed (110) facet exhibited prominent catalytic performance with a Faradaic efficiency of CO up to 84% and a current density of -10 mA cm<sup>-2</sup> at -1.2 V versus RHE, far outperforming the ZnO nanowire (101) and ZnO nanoflower (103). Based on detailed characterizations and kinetic analysis, the ZnO nanosheet (110) with porous architecture increased the exposure of active sites. Further studies revealed that the high CO selectivity originated from the enhancement of CO<sub>2</sub> adsorption and activation on the ZnO (110) facet, which promoted the conversion of CO<sub>2</sub> toward CO. This study provides a new way to tailor the activity and selectivity of metal catalysts by engineering exposed specific facets.
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DOI: 10.1021/acsami.4c01797
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