Graphdiyene enables ultrafine Cu nanoparticles to selectively reduce CO2 to C2+ products
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 CO 2 to multicarbon (C 2+ ) products, owing...
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| Published in | Nano research Vol. 15; no. 1; pp. 195 - 201 |
|---|---|
| Main Authors | , , , , |
| Format | Journal Article |
| Language | English |
| Published |
Beijing
Tsinghua University Press
01.01.2022
|
| Subjects | |
| Online Access | Get full text |
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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 CO
2
to multicarbon (C
2+
) 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 CO
2
-to-C
2+
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 C
2+
products up to 74%, significantly higher than those of support-free Cu NPs (C
2+
FE, ~ 2%), carbon nanotube-supported Cu NPs (CNT-Cu, C
2+
FE, ~ 18%), graphene oxide-supported Cu NPs (GO-Cu, C
2+
FE, ~ 8%), and other reported ultrafine Cu NPs. Our results demonstrate the critical influence of graphdiyne on the selectivity of Cu-catalyzed CO
2
electroreduction, and showcase the prospect for ultrafine Cu NPs catalysts to convert CO
2
into value-added C
2+
products. |
|---|---|
| AbstractList | 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. 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 CO 2 to multicarbon (C 2+ ) 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 CO 2 -to-C 2+ 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 C 2+ products up to 74%, significantly higher than those of support-free Cu NPs (C 2+ FE, ~ 2%), carbon nanotube-supported Cu NPs (CNT-Cu, C 2+ FE, ~ 18%), graphene oxide-supported Cu NPs (GO-Cu, C 2+ FE, ~ 8%), and other reported ultrafine Cu NPs. Our results demonstrate the critical influence of graphdiyne on the selectivity of Cu-catalyzed CO 2 electroreduction, and showcase the prospect for ultrafine Cu NPs catalysts to convert CO 2 into value-added C 2+ products. |
| Author | Lu, Xiu-Li Zhang, Chao Zhang, Wen Chang, Yong-Bin Lu, Tong-Bu |
| Author_xml | – sequence: 1 givenname: Yong-Bin surname: Chang fullname: Chang, Yong-Bin organization: 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 – sequence: 2 givenname: Chao surname: Zhang fullname: Zhang, Chao organization: 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 – sequence: 3 givenname: Xiu-Li surname: Lu fullname: Lu, Xiu-Li organization: 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 – sequence: 4 givenname: Wen surname: Zhang fullname: Zhang, Wen email: zhangwen@email.tjut.edu.cn organization: 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 – sequence: 5 givenname: Tong-Bu surname: Lu fullname: Lu, Tong-Bu email: lutongbu@tjut.edu.cn organization: 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 |
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| Keywords | multicarbon products graphdiyne nanofibers CO reduction electrocatalysis ultrafine copper nanoparticles |
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| Snippet | Reducing the size of heterogeneous nanocatalysts is generally conducive to improving their atomic utilization and activities in various catalytic reactions.... |
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| StartPage | 195 |
| SubjectTerms | Alkynes Atomic/Molecular Structure and Spectra Binding Biomedicine Biotechnology Carbon dioxide Carbon nanotubes Catalysts Chemistry and Materials Science Condensed Matter Physics Electrocatalysts Graphene Intermediates Materials Science Nanoparticles Nanotechnology Research Article Selectivity Ultrafines |
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| Title | Graphdiyene enables ultrafine Cu nanoparticles to selectively reduce CO2 to C2+ products |
| URI | https://link.springer.com/article/10.1007/s12274-021-3456-2 https://www.proquest.com/docview/2594890604 |
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