The Lattice Mismatch-Driven Photochemical Self-Assembly of Supported Heterostructures for Stable and Enhanced Electrocatalytic Carbon Dioxide Reduction Reaction
Metallic heterostructural nanocrystals (HNCs) hold immense potential in electrocatalytic carbon dioxide reduction reaction (CO<sub>2</sub>RR) owing to their abundant active sites and high intrinsic activity. However, a significant challenge still remains in achieving controlled nucleatio...
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| Main Authors: | , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
MDPI AG
2024-11-01
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| Series: | Molecules |
| Subjects: | |
| Online Access: | https://www.mdpi.com/1420-3049/29/23/5560 |
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| Summary: | Metallic heterostructural nanocrystals (HNCs) hold immense potential in electrocatalytic carbon dioxide reduction reaction (CO<sub>2</sub>RR) owing to their abundant active sites and high intrinsic activity. However, a significant challenge still remains in achieving controlled nucleation and growth sites for HNCs on supports and comprehending the influence of the structure–activity relationship on electrocatalytic CO<sub>2</sub>RR performance. This work presents a photochemical self-assembly technique without the necessity for reducing agents or facet-specific capping agents. By controlling lattice mismatch and manipulating transfer paths of photo-generated carriers, we can precisely direct the growth sites and nucleation of nanocrystals, enabling the self-assembly of supported core–shell and Janus nanostructures. Compared to Pd(T)@Au core–shell HNCs with the same loading, Pd cube–Au Janus HNCs exhibit significantly enhanced selectivity and stability toward carbon monoxide (CO) production in CO<sub>2</sub>RR at less negative potentials. The Pd cube–Au Janus HNC electrocatalyst achieved a Faradaic efficiency (FE) of 92.6 ± 3.5% for CO electroreduction, accompanied by a current density of 72.3 mA·cm<sup>−2</sup> at −0.58 V. This work provides an effective strategy for designing advanced supported tandem electrocatalysts to boost the selectivity and durability test of CO<sub>2</sub>RR. |
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| ISSN: | 1420-3049 |