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Solar reduction of carbon dioxide on copper-tin electrocatalysts with energy conversion efficiency near 20.

ABSTRACT: Copper catalysts modified with tin have been demonstrated to be selective for the electroreduction of carbon dioxide to carbon monoxide. However, such catalysts require the precise control of tin loading amount. Here, we develop a copper/tin-oxide catalyst with dominant tin oxide surface being formed via a spontaneous exchange reaction between sputtered tin and copper oxide. Even though the surface of this catalyst is tin-rich, it achieves an excellent performance towards carbon monoxide production in a flow cell. This contrasts with copper/tin-oxide prepared via atomic layer deposition since it yields selectivity towards carbon monoxide only on a copper-rich surface. Mechanism studies reveal that the tin sites on the tin-rich copper/tin-oxide surface achieve a suitable binding with adsorbed carbon monoxide under the presence of copper. Powered by a triple-junction solar cell, the copper/tin-oxide based electrolyzer sets a new benchmark solar-to-chemical energy conversion efficiency of 19.9 percent with a Faradaic efficiency of 98.9 percent towards carbon monoxide under simulated standard air mass 1.5 global illumination.

SUBMITTER: Gao J

PROVIDER: S-EPMC9537560 | biostudies-literature | 2022 Oct

REPOSITORIES: biostudies-literature

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Solar reduction of carbon dioxide on copper-tin electrocatalysts with energy conversion efficiency near 20.

Gao Jing J Li Jun J Liu Yuhang Y Xia Meng M Finfrock Y Zou YZ Zakeeruddin Shaik Mohammed SM Ren Dan D Grätzel Michael M

Nature communications 20221006 1

Copper catalysts modified with tin have been demonstrated to be selective for the electroreduction of carbon dioxide to carbon monoxide. However, such catalysts require the precise control of tin loading amount. Here, we develop a copper/tin-oxide catalyst with dominant tin oxide surface being formed via a spontaneous exchange reaction between sputtered tin and copper oxide. Even though the surface of this catalyst is tin-rich, it achieves an excellent performance towards carbon monoxide product ...[more]

PMID: 36202808

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Project description:Abstract It remains a real challenge to control the selectivity of the electrocatalytic CO2 reduction (eCO2R) reaction to valuable chemicals and fuels. Most of the electrocatalysts are made of non‐renewable metal resources, which hampers their large‐scale implementation. Here, we report the preparation of bimetallic copper‐lead (CuPb) electrocatalysts from industrial metallurgical waste. The metal ions were extracted from the metallurgical waste through simple chemical treatment with ammonium chloride, and CuxPby electrocatalysts with tunable compositions were fabricated through electrodeposition at varying cathodic potentials. X‐ray spectroscopy techniques showed that the pristine electrocatalysts consist of Cu0, Cu1+ and Pb2+ domains, and no evidence for alloy formation was found. We found a volcano‐shape relationship between eCO2R selectivity toward two electron products, such as CO, and the elemental ratio of Cu and Pb. A maximum Faradaic efficiency towards CO was found for Cu9.00Pb1.00, which was four times higher than that of pure Cu, under the same electrocatalytic conditions. In situ Raman spectroscopy revealed that the optimal amount of Pb effectively improved the reducibility of the pristine Cu1+ and Pb2+ domains to metallic Cu and Pb, which boosted the selectivity towards CO by synergistic effects. This work provides a framework of thinking to design and tune the selectivity of bimetallic electrocatalysts for CO2 reduction through valorization of metallurgical waste. Bimetallic Cu‐Pb electrocatalysts were prepared from industrial metallurgical residues and used to electrochemically convert CO2 into valuable chemicals. The metlas were extracted through chemical treatment with ammonium chloride, and Cu−Pb electrocatalysts with varying ratios were prepared through electrodeposition. Compared with pure Cu, the bimetallic catalyst displayed a promotional effect on the conversion of carbon dioxide to carbon monoxide. In situ and ex situ characterization revealed that the interplay between in situ reduced Cu and Pb sites results in boosted CO production through synergistic effects.

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Solar reduction of carbon dioxide on copper-tin electrocatalysts with energy conversion efficiency near 20.

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Solar reduction of carbon dioxide on copper-tin electrocatalysts with energy conversion efficiency near 20.

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