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Graphdiyene enables ultrafine Cu nanoparticles to selectively reduce CO2 to C2+ products

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Abstract

Reducing the size of heterogeneous nanocatalysts is generally conducive to improving their atomic utilization and activities in various catalytic reactions. However, this strategy has proven less effective for Cu-based electrocatalysts for the reduction of CO2 to multicarbon (C2+) products, owing to the overly strong binding of intermediates on small-sized (< 15 nm) Cu nanoparticles (NPs). Herein, by incorporating pyrenyl-graphdiyne (Pyr-GDY), we successfully endowed ultrafine (∼ 2 nm) Cu NPs with a significantly elevated selectivity for CO2-to-C2+ conversion. The Pyr-GDY can not only help to relax the overly strong binding between adsorbed H* and CO* intermediates on Cu NPs by tailoring the d-band center of the catalyst, but also stabilize the ultrafine Cu NPs through the high affinity between alkyne moieties and Cu NPs. The resulting Pyr-GDY-Cu composite catalyst gave a Faradic efficiency (FE) for C2+ products up to 74%, significantly higher than those of support-free Cu NPs (C2+ FE, ~ 2%), carbon nanotube-supported Cu NPs (CNT-Cu, C2+ FE, ~ 18%), graphene oxide-supported Cu NPs (GO-Cu, C2+ FE, ~ 8%), and other reported ultrafine Cu NPs. Our results demonstrate the critical influence of graphdiyne on the selectivity of Cu-catalyzed CO2 electroreduction, and showcase the prospect for ultrafine Cu NPs catalysts to convert CO2 into value-added C2+ products.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 21702146, 21805207, 21790052, and 21931007), the National Key Technology R&D Program of China (No. 2017YFA0700104), 111 Project of China (No. D17003), and the Natural Science Foundation of Tianjin (No. 19JCQNJC05500).

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  1. Ministry of Education International Joint Laboratory of Materials Microstructure, Institute for New Energy Materials and Low Carbon Technologies, School of Material Science & Engineering, Tianjin University of Technology, Tianjin, 300384, China

    Yong-Bin Chang, Chao Zhang, Xiu-Li Lu, Wen Zhang & Tong-Bu Lu

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  1. Yong-Bin Chang
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Chang, YB., Zhang, C., Lu, XL. et al. Graphdiyene enables ultrafine Cu nanoparticles to selectively reduce CO2 to C2+ products. Nano Res. 15, 195–201 (2022). https://doi.org/10.1007/s12274-021-3456-2

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